Chapter 8 Nuclear Fission energy for war and peace Soon after the neutron induced radioactivity was discovered, several groups of researchers bombarded uranium by neutrons and analyzed the radioactive products formed thereof. However, results were not what they expected, and they misinterpreted of their results due to their expectations. The German group eventually interpreted their results in terms of fission, and fission was discovered in the midst of World War II. Nuclear fission is a process, by which a heavy nuclide splits into two or more pieces. From masses of nuclides, scientists knew that such a process would release a lot of energy. Thus, research on nuclear fission became the top secret in Germany, England, France, the former U.S.S.R., and the United States. It was obvious that a weapon employing the nuclear fission would be so powerful that whoever had developed it would win. Such a weapon would destroy the enemy in such a way that even the winner will be scared. Soon after the discovery of nuclear fission, the technology was employed to make bombs. The desire to win the war sped up the development of atomic bombs. Two such bombs were used in the war. The destruction was so massive and horrified that no additional nuclear bomb has been deployed in wars. .... For in the development of this organization (the United Nations) rests the only true alternative to war, and war appears no longer as a rational alternative. Unconditional war can no longer lead to unconditional victory. It can no longer serve to settle disputes. It can no longer be of concern to great powers alone. For a nuclear disaster, spread by winds and waters and fear, could well engulf the great and the small, the rich and the poor, the committed and the uncommitted alike. Mankind must put an end to war or war will put an end to mankind. Political will and public pressure have diverted human effort to develop peaceful applications of nuclear energy. As a result, nuclear power reactors have supplied energy for our need for decades and they continue to do so. Yet, reactor accidents have changed the public opinion and about nuclear energy. The future of nuclear reactors became uncertain. However, energy demand is always on the increase, and at some point, the public opinion may shift again. 225 John F. Kennedy September 25, 1961, Address to the United Nations. Nuclear Fission Reactions Soon after their discovery, neutrons were used to bombard all kinds of material to induce radioactivity. Neutron bombardment of uranium produced complicated radioactivity. Because researchers were looking for heavier nuclides, they took a long time to discover that neutron bombardment actually split uranium into two light nuclides, and such a process is called nuclear fission. The Discovery of Fission Reactions No doubt, you have heard of the term nuclear fission because of the infamous atomic bombs and power producing nuclear reactors. Because a new concept is required to recognize fission, the story leading to the discovery of fission is particularly interesting. Why did researchers bombarding uranium with neutrons? What were researchers looking for? What did the radioactivity indicate? How was nuclear fission discovered? Why did neutron bombardment produce many products, and what are the products? Which isotope undergoes fission? Are neutron released in the fission process? Neutrons ? ? Uranium ? -radioactivity After their discovery, neutrons were used to bombard all elements including uranium. At that time, three prominent research groups separately led by Enrico Fermi (1901-1954) in Rome, F. Joliot (1900-1958) and I. Curie in Paris, and Otto Hahn (1879-1968), Lise Meitner, and Fritz Strassmann in Berlin diligently bombarded uranium with neutrons, hoping to produce transuranium elements (elements heavier than uranium). After bombardment by neutrons, uranium samples became radioactive. Beta particle emission was particularly noticeable. The three groups competed with one another to identify the products in these experiments. Since they worked in three different countries, the competition was an international race for the first to identify the nuclide(s) produced. They expected neutron capture reactions followed by emission to produce elements 93 (E93) and 94 (E94), which were unknown at that time. They expected these reactions: U (n, ) 239U92 (, ) 239E93 (, ) 239E94. 238 Otto Hahn (1879-1968) and Fritz Strassmann (1902-1980) were credited with the discovery of nuclear fission received the Nobel Prize for Chemistry in 1944, due to the fact that Hahn and Strassmann published the results without Meitner's name. The Enrico Fermi Award in 1966 went to Hahn, Strassmann, and and Lise Meitner (1878-1968). 226 They published papers offering various interpretations and attacked each other for misinterpretations. The arguments went on for some time while the war intensified in Europe. The French group precipitated a emitter with half-life 3.5 d together with lanthanum, and they interpreted it as an isotope of actinium (Z = 89), which drew criticism from Hahn who argued that and proton emissions were not possible. Hahn, a chemist, Strassmann, an analytical chemist, and Meitner, a physicist, worked together to make transuranium elements. Meitner was very excited when she detected a great increase in radioactivity after uranium was irradiated with neutrons. Strassmann, applied analytical chemistry skills to precipitate the radioactive products. He understood that hydrogen sulfide (H2S) would not precipitate uranium radioactive decay daughters, but after neutron irradiation, he precipitated most of the radioactive products using H2S. The half-life measurements indicated to them that not one but many elements were produced (Shea, 1983). How could one reaction give rise to so many different products? The three groups struggled over this question for many years, and eventually Hahn's group, including Meitner on exile, came to the conclusion that the neutron bombardment caused 235U to split into small fragments whose mass numbers are slightly more or less than half the mass number of uranium. Products, which they earlier thought to be the radioactive as isotopes eka-rhenium, eka-osmium, eka-iridium and eka-platinum, co-precipitated with rhenium, osmium, irridium etc, were later identified as fission products not transuranium elements. The nucleons in a nucleus form a liquid drop, and the fission process is very much like splitting a drop into two, often unevenly. The Official History of the Manhattan Project (US, The Liquid Drop Model and Fission 1977) gives the following story. The discovery of neutron induced fission was first brought to Copenhagen by Dr. Meitner, who, as a nonAryan, was exiled from Germany in 1938. She used barium ions, Ba2+, as a carrier and precipitated the radioactive products from the neutron bombardment. None of the chemical methods could separate the radioactive ingredient from the barium ion, and she concluded that the isotope 238U must have split into two fragments. The atomic weight of barium, 137, is a little more than half of 238. When she arrived at Copenhagen, she communicated her thought to Dr. Frisch, who communicated the information to his friend N. Bohr, who was in the United States at the time. Bohr conveyed Meitner’s insight to Fermi who immediately changed his strategy of research. In March, 1940, Fermi's group (working in Columbia University) found that only the less abundant (0.7%) isotope 235U underwent fission. 227 When Fermi (1901-1954), Szilard (1898-1964), and F. Joliot (1900-1958) learned of the fission of uranium, they were anxious to find out which isotope underwent fission and if neutrons were released in the fission process. If neutrons are released, they had envisioned a chain fission reaction because the newly released neutrons induce more fission reactions. Almost at the same time and independently, researchers in various groups discovered that only 235U underwent fission and neutrons were indeed released. The release of neutron made the fission reactions candidates for a very powerful weapon known as the atomic bomb, which was eventually built and used. During the lecture, a movie on the life of Lise Meitner called "The Missing Link" will be shown. The title was derived from her isolation of the isotope protactinium, 231Pa91, an element unknown until that time. Elements thorium, Th90, and uranium U92 were well known, but the element between them will missing. The movie is a very good video essay that addresses several issues including politics and power. Skill Building Questions 1. What is the lesson learned from the story leading to the discovery of neutron induced fission? (New concepts are required to recognize new phenomena. Concepts are important tools in research. New phenomena create new concepts, and new concepts give new interpretation to old phenomena. Many concepts became theory, and we take some of them for granted.) 2. Why are reactions induced by neutron bombardment of uranium so difficult to explain? How can uranium fission products be identified and confirmed? (The neutron bombardment caused 235U to split into small fragments whose mass numbers are slightly more or less than half the mass number of uranium. Thus, many products were produced. We will discuss this further in the next few sections.) The Fission Nuclear Energy The discoveries that one of the uranium isotopes 235U underwent nuclear fission reactions, and that neutrons were released opened a new frontier for research and development. The discoveries were so important that they were treated as top secret because of the its potential applications in war. Furthermore, these discoveries were made at a time when the entire world was at war, and the war sped up the research and development. How much energy is released per fission reaction? How can the amount be estimated or calculated? What are the applications of fission energy in war and peace? A strategist asks many questions about a new discovery, and a philosopher plans for the future. The questions and plans are seeds for further research and development. We concentrate on the fission process and the energy aspect in this section. A spontaneous reaction releases energy. Neutron induced nuclear fission reactions are spontaneous reactions and they release energy. This quantity is important, because it affects fission research and 228 development. Both theoretical considerations and practical measurements have been carried out to give estimates of the amount of energy released in fission reactions. Some examples showing how estimates can be made are given here. You have learned that when nucleons bind together to form a nuclide, energy is released. The energy so released is called binding energy. The average binding energy is the largest for nuclides with mass number around 56. Thus, splitting up a heavy nuclide such as uranium to give nuclides with mass number about 117 releases energy. A rough estimate is to consider an even split of 235U to give two nuclides of mass numbers 117 and 118. A search of stable nuclides with mass numbers 117 and 118 are 117Sn50, and 118Sn50, their masses being 116.902956 and 117.901609 amu respectively. The mass of 235U92 is 235.043924 amu. The difference in mass 235.043924 - (116.902956 + 117.901609) = 0.2394 amu (931.5 MeV/1 amu) = 223 MeV. E = m c2 In reality, a fission reaction usually gives two unequal fragments, plus 2 to 3 neutrons. These neutron-rich fragments are beta () emitters. As a more realistic example to calculate the energy of a fission reaction, let the two fragments be isotopes of rubidium and cesium plus three neutrons. The reaction can be represented by U+n 235 142 Cs55 + 90Rb35 + 4n + Q. where Q is the mass equivalence of energy released. The neutron-rich cesium and rubidium isotopes are not stable, and they undergo radioactive decays: Cs 142Ba + (~1 m) 90 Ba 142La + (11 m) 90 La 142Ce + (58 m) 90 142 142 142 Rb 90Sr + (half-life, 15.4 m) Sr 90Y + (27.7 y) Y Zr (stable) + (64 h) 90 Ce 142Pr + (51015 y) 142 Pr 142Nd (stable) + (19 h) 142 The total energy can be calculated from the measured masses of 235U, 90Zr, 142Nd, and neutron but some of the energy will not be released during the operation of the reactor due to the very long half-lives (in this case of 90Sr, 142Ce). However, a calculation to estimate the energy may proceed in the following way: Reaction Mass /amu U92 90Rb37 + 142Cs55 + 3n + Q. 235.04924 = 89.904703 + 141.907719 + 3 x 1.008665 + Q 235 The radioactive nuclide 90Sr is present in the fallout of nuclear explosions. It threatens animal and human health, because its properties are similar to calcium. Ingested strontium ions reside in the bone structure. 229 Q = (235.043924 - 89.904703 - 141.907719 - 3 x 1.008665)(931.4812 MeV/1 amu) = 191.4 MeV per fission The energy of 191.4 MeV is equivalent to 0.0000307 J or 307 erg, which is released per fission of 235U nucleus. Fission of one kilogram (1000 g) of uranium-235 will release 7.861019 J 1000g U 1mol U 6.023 10 23 U nuclei 191.4MeV 1.602 10 13 J 235g U 1mol U 1U nucleus 1MeV = 7.861013 J This amount of energy is equivalent to 2.2×1010 kilowatt-hour, 22000 megawatt-hour, or 22 giga-watt-hour. This amount of energy keeps a 100-watt light bulb lit for Energy (MeV) distribution in fission reactions 25,000 years. Kinetic energy of fission fragments 167 MeV In the fission process, the 8 Prompt (< 10–6 s) gamma () ray energy fragments and neutrons Kinetic energy of fission neutrons 8 move away at high speed carrying with them large 7 Gamma () ray energy from fission products amounts of kinetic energy. The neutrons released during 7 Beta () decay energy of fission products the fission process are called Energy as antineutrinos (ve) 7 fast neutrons because of their high speed. Neutrons and fission fragments fly apart instantaneously in a fission process. No delayed liberation of neutrons was ever observed. Gamma rays (photons) equivalent to 8 MeV of energy are released within a microsecond of fission. As mentioned earlier, the two fragments are beta emitters. Recall that beta decays are accompanied by antineutrino emissions, and the two types of particles carry away approximately equal amounts of energy. Beta decays often leave the nuclei at excited states, and gamma emission follows. Estimated average values of various energies are given in a table here. Skill Building Questions 1. Give an example to show how the amount of energy released in a nuclear fission can be estimated. 2. Assume 235U splits into two fragments with masses 100 and 132 and three neutrons. Find the masses of stable nuclides with these masses. What is the fission energy in this cases? 3. How is the fission energy distributed among the various forms? 4. Calculate the speed of a neutron which has kinetic energies of 1 and 2 MeV respectively. 230 The Cyclotron and Fission Research The machine built by Cockroft and Walton accelerated protons, which smashed 7Li nuclei. Any machine that speeds up the velocity of particles are called particle accelerators. Particles from accelerators induced many nuclear reactions, and the value of accelerators in the study of nuclear reactions was soon realized. How can particles be accelerated? How to build particle accelerators? What are the purposes of particle accelerators? How can particle accelerators be used to study fission reactions? A Sketch of the Cyclotron Ions, originated from the center of the cyclotron, accelerated by alternate voltages between the Dee’s follow a spiral path acquiring high energy and exit from a window. Various types of particle accelerators have been built, using electric potentials or electromagnetic forces. Linear particle accelerators made particles moving faster along a straight line; whereas cyclotrons accelerated them as they travel along circular path. The cyclotrons built by Ernest O. Lawrence in Berkeley, California belong to the latter type, and they have given useful results. High voltage Experiment station A Dee A cyclotron has two hollow D-shaped (Dee) sections assembled together with a small space in between. A magnetic field deflects the particles into spiral motion. By applying alternated voltages between the Dees, the cyclotron accelerates charged particles to desirable energies. By changing the strength of the magnetic field, particles of various energies are made available. The first such cyclotron has a diameter of only 13 cm, and it accelerated protons to a maximum energy of 13 keV. Cyclotrons built later with larger diameter accelerated particles to energies between 10 and 100 MeV. Accelerated particles are used to induce nuclear reactions as discussed in the last Chapter. Reactions between accelerated charged particles from cyclotrons and light nuclides produced neutrons of variable energy. The following are some of the reactions: 7 Li (p, n) 7Be T (p, n) 3He 1 H (t, n) 3He 2 D (d, n) 3He 2 D (t, n) 4He 3 T (d, n) 4He. 3 Ernest O. Lawrence (1901-1958) received the Nobel Prize for physics in 1939 for the invention of cyclotron, the first particle accelerator to accelerate particles to high energy. 231 Reactions between tritium (3T or t) and deuterium (2D or d) are particularly important, because these are fusion reactions. Furthermore, they release neutrons of various energies. Cyclotron induced nuclear reactions provide neutrons of controlled energy for the study of fission. For example, some reactions of protons with medium-weight nuclides are listed below together with their threshold energy and neutron energy range. Reaction Threshold* Energy range (keV) energy (MeV) of narrow-energy neutron 51 V (p, n) 51Cr 2.909 5.6-52 45 45 Sc (p, n) Ti 1.564 2.36-786 57 57 Fe (p, n) Co 1.648 2-1425 __________________________________ * The threshold energy is the minimum energy of proton required for the reaction. Energy from the neutron source 27Al (, 1n) 30P mentioned earlier can not be varied. Neutron sources from the cyclotron have an advantage over neutron sources induced by natural radiation, because neutron energy can be varied. This enables the study of energy dependence of neutron induced fission reactions. The variation of cross sections for neutron-induced fission as a function of neutron energy is a vital piece of information for nuclear reactor design. The study showed that fast neutrons (energy ranges from 10 MeV to 10 KeV) are not effective to induce fission, but slow neutrons (0.03 to 0.001 eV) are very effective. Slow neutrons are also called thermal neutrons, because their energy corresponds to room temperatures. Skill Building Questions 1. What are particle accelerators? What are cyclotrons? How do they accelerate charged particles? 2. What are the applications of particle accelerators? 3. What are the advantages of neutron sources from nuclear reactions induced by particle accelerators? (They provide neutron sources of variable but definite energy for experiments.) 232 The Synthesis of Plutonium The intention to synthesize transuranium elements by neutron bombardment of uranium split 235U nuclei. Can transuranium elements be made by neutron capture reactions of uranium? If so, why are tranuranium elements not detected? How can plutonium be dynthesized? What are the properties of plutonium? Why is plutonium a strategic material? Pluto Neptune Uranus Experiments to produce elements 93 and 94 by the (n, ) reaction are sound, but so much fission products were produced that they impaired the detection of transuranium elements. The cyclotron, however, provided high intensity neutrons of definite energy, and it gave a chance for success. The cyclotron provided neutrons for E. M. McMillan (1907-) and P. H. Abelson (1913-), to bombard uranium. In the summer of 1940, they confirmed one product as element 93, and named it neptunium, Np, after the planet Neptune. They inferred that Np would decay by emitting a particle converting itself into element 94, named plutonium after the planet Pluto. These reactions are summarized bellow: 238 U + n 239U + 239 U (half life 23.5 m) 239Np + 239 Np (half life 2.35 d) 239Pu + or in short notations: 238 U (n, ) 239U ( , ) 239Np ( , ) 239Pu or 238 U (n, 2) 239Pu Actually, the neutrons with high kinetic energies are used to produce transuranium elements. The fission theory by Bohr and Wheeler suggested that 239Pu would undergo fission. Thus, the cyclotron in Berkeley was put to work to produce enough plutonium for experiments. By mid1941, the fission characteristic of plutonium was well established. Plutonium was first detected (1940) by Glenn T. Seaborg, Joseph W. Kennedy, and Arthur C. Wahl, from the reaction 238U (d, b) 240Np using deuterium from the 60-inch cyclotron at Berkeley, California. The most important isotope is 239Pu, because it has a long half-life (24,400 Edwin M. McMillan (1907-1991) shared the 1951 Nobel Prize with G. T. Seaborg (1912-1999). He discovered neptunium from the decay reaction 239U (, ) 239Np. In 1940, he and Philip H. Abelson (1913-) isolated Np and discovered the reaction 239Np (, b) 239Pu, and they were credited for the discovery and synthesis of plutonium. 233 y) and it is a fission fuel. This isotope can easily be produced using a breeder reactor, which shall be described later in this Chapter. Plutonium has a very high electrical resistivity and a density of 19.84 g cm-3. It is chemically reactive, dissolving in acids and forming various ions of characteristic colour in water: Pu3+, blue-lavender; Pu4+, yellow-brown; and PuO+2, pink. Many compounds of plutonium have been prepared, often starting from the dioxide, PuO2), the first compound of any synthetic element to be separated in pure form and in weighable amounts (1942). Isotope 244Pu gives a melting point of 912 K, boiling point 3,508 K. The concept of critical mass will be introduced later, and you may be interested in knowing that the critical mass of 239Pu is only 300 grams. Skill Building Questions 1. Describe the neutron capture reaction of uranium leading to the formation of neptunium and plutonium. 2. What is the significance of the synthesis of neptunium and plutonium? 3. Why is 239Pu the most important isotope of plutonium? Uniting Political and Nuclear Powers Neutron induced fission reactions release energy and neutrons. The amount of energy in fission reactions is alarmingly large and the liberation of neutrons in the fission process gives the possibility of an explosive chain reaction, which releases a tremendous amount of energy. At that time, the scientists already foresaw the danger of nuclear power, especially if the technology falls in the wrong hand. Since securing the presidency of Germany in 1933, Hitler became a dictator, and many top scientists in Austria, Hungary, Italy and Germany felt uncomfortable. Scientists with ethnic backgrounds other than German felt threatened. Many European scientists had escaped the Hitler regime and come to the United States. At the time fission was discovered, Hitler invaded Poland, Hungary, Slovak and other European countries. Many scientists were concerned that Hitler would make use of fission to build bombs. Such a move is a threat to the entire world. Why scientists feared the danger of nuclear power? What was the political situation when fission was discovered? Why were so many scientists felt threatened? Who took the initiative to bring the issue to the most powerful political leader and why? What did they do individually and collectively and why? What would you do if you were afraid of the nuclear power falling into the wrong hand? What is an effective strategy to prevent a disaster from happening? 234 Among the concerned people were three Hungarian refugee scientists Leo Szilard, Eugene Wigner, and Edward Teller, who thought the time has come to unite political force with nuclear power. They thought Hitler had the potential and possibility of developing atomic bombs. This matter should be brought to the immediate attention of the President of the United States, Roosevelt. To achieve this, they needed someone with a reputation. They convinced Albert Einstein that such an action was a necessity. Szilar, Wigner and Teller composed a letter for Einstein, and Einstein signed the letter* as the sender. They took the matter so serious that they convinced the economist Alexander Sachs to personally deliver the letter to the White House. (Use Einstein and letter and Roosevelt as keys to search the Internet will get many sites containing this letter) Refugee scientists from Hungary, Germany and Italy (L. Fermi, 1955) have worked under a totalitarian political system, in which totalitarian leaders controlled everything including universities and researchers. The governments knew whatever went on in university laboratories. They were fearful of Germany being the first to develop the atomic bomb. Thus, they took the initiative to bring the issue to the president of the United States. Most American scientists at that time were usually unfamiliar with this type of political control, and they felt less threatened. The likelihood that Germany might develop an atomic bomb caused President Roosevelt to act and he decided immediately to create an Advisory Committee on Uranium that would give financial assistance to universities engaged in uranium research. The sum of $300,000 (remember these are 1940’s dollars) was immediately allocated to Columbia, Princeton, MIT, Chicago, California, Virginia etc. Research on uranium and fission is complicated, and information on many aspects of uranium and of fission is required. Each group worked on one or more aspects of fission, and nuclear research was intensely carried out by many young and old scientists. The Chicago group worked on uranium, and the California group worked on plutonium. Soon they realized that enriched 235U or pure 239Pu would be required for the construction of an atomic bomb. For building an atomic bomb, production of enough fissionable material is the most important task. However, other information such as identification of fission products, accurate cross section for neutrons as functions of energies, moderating neutron motion, and percentages of neutrons that induce fission are all required. Review Questions 1. What is power? What do high political positions, reputation, money, science and knowledge have in common? (Each of these represents a form of power. Agree or not agree, elaborate your view.) * Szilard (1898-1964), Wigner (1902-1995) and Teller (1908-) all played important roles in nuclear physics. Read about them. Wigner shared the Physics Nobel Prize for 1963 with two other physisists, and Teller is known as the father of the hydrogen bomb. For a copy of Einstein’s letter, consult http://www.anl.gov/OPA/frontiers96/aetofdr.html 235 2. Comment on the action taken by Szilard, Wigner, and Teller. (Political and economical forces do influence scientific development. The objective of this question is to raise the awareness of the impact of science on politics and vice versa.) 3. Comment on the reaction of President Roosevelt. Thermal Neutrons Fermi's group irradiated uranium samples with neutrons. They surrounded the samples with different materials at various times and found samples surrounded by water, wood, and paraffin more radioactive. Why surrounding the samples with water, wood, and paraffin increased their radioactivity? What happens to neutrons when they collide with atoms and molecules in a medium? Which one is more effective in slowing neutrons, heavy nuclides or light ones? Why? What are the energies of neutrons after they have scattered many times with atoms? How do these energies depend on the temperature of the medium? After Fermi's group has learned of nuclear fission, they attributed the fission radioactivity increase to the moderation (slowing down) of neutrons by hydrogen and light elements in water, wood, and paraffin. They thought that neutrons are slowed quickly by collision with protons, because the two particles have comparable mass. Neutrons can transfer almost all their kinetic energy to proton in a collision. Materials used to slow down fast neutrons are called moderators. On the average, 20 collisions with protons are sufficient for neutrons to reach an equilibrium state that further collisions will no longer change their average kinetic energy. The average kinetic energy of neutrons depends on the temperature of the A Maxwellian Distribution of Kinetic medium, in which they are in thermal equilibrium Energy (Ek) of Molecules in a Material. with. These neutrons are called thermal neutrons. In the following paragraphs, we further describe No. of molecules with kinetic energy Ek how energy of the molecules depends on the temperature. Molecules in a medium are constantly in motion: 298 K 373 K vibration, rotation, and translation. The average kinetic energy of molecules is directly proportional to the temperature in K. At room temperature (293 K) the average kinetic energy of all molecules is Ek 0.025 eV. Of course, some molecules have higher and some have lower kinetic energies than 0.025 eV. In fact, the kinetic energies of the molecules have a Maxwellian distribution. This skewed distribution is depicted here, and it is different from the normal or bell shaped distribution. As the temperature changes, the skewed distribution shifts slightly to give a higher average kinetic energy. 236 The neutrons collide with molecules and atoms in the medium constantly, and their energies have the same distribution as those of the molecules. Neutrons are often classified as fast, thermal, and cold neutrons according to their kinetic energies. Fast neutrons have a kinetic energy exceeding some threshold, typically 0.1 or MeV. Neutrons just released from the fission reactions are fast neutrons. After some collisions with atoms in the medium, they become thermal neutrons and their typical average kinetic energy is 0.025 eV. The average kinetic energy of cold neutrons is less than 0.01 eV. Slightly different boundaries of division may be given in other literature due to differences in view points or definition of room temperatures, but these are typical values. Cold neutrons are either from super cold hydrogen moderated experimental reactors or selected by diffraction from crystals. There are some special applications for this type of neutrons. Skill Developing Questions 1. Explain the following terms: moderator, fast neutrons, thermal neutrons and cold neutrons. 2. Sketch a distribution for kinetic energies of thermal neutrons. 3. Estimate the velocities of a neutron whose kinetic energies are 0.1 MeV, 0.025 eV, and 0.01 eV respectively. Thermal Neutron Cross Sections Cross section () is a measure of the probability of a given reaction, as we have discussed elsewhere. Cross sections are further classified according to types and reactions. Since thermal neutrons are readily available thermal neutron cross sections (c), are important nuclear data. They are usually given for each nuclide to indicate its probability of thermal neutron capture. For possible fission material, the thermal neutron cross section for fission (f) is also given. How do you look for a suitable fission material for nuclear reactor from a nuclear data source? What parameters indicate the suitability of fission material? What materials are suitable for the construction of fission reactors and bombs? What are the thermal neutron cross sections (c) of some key elements that are useful for the construction of atomic bombs and for nuclear reactors? Thermal neutrons are much better than fast neutrons at inducing nuclear fission. Thus, thermal neutron cross sections for all nuclides have been studied, because many materials are required for fission device (bombs and reactors) constructions. Around 1940, the Uranium Research Program measured thermal neutron cross sections for various reactions of almost all nuclides. In the following list, thermal neutron (capture) cross sections () and thermal neutron fission cross sections (f) are given for some key nuclides. 237 Half-lives (t1/2) of the radioactive nuclides are also given, because they are important properties of the nuclides regarding fission device. 1 2 H c /b 0.33 f /b t1/2 /y 12 14 C N 0.0034 1.82 H 0.00052 16 O 0.0002 113 Cd 19,820 233 235 U U 46 98 530 580 5 1.6×10 7×108 238 U 2.7 2.7×10-6 4.5×109 Note the large difference in cross sections between hydrogen, 1H, and deuterium, 2H, given above. The difference warrants the extraction of heavy water (2H2O or D2O) from natural water for fission device applications. Since the cross section for deuterium is small, heavy water, D2O, does not absorb many neutrons, and using it as moderator for reactors gives sufficient neutrons for using natural uranium as a fuel. If pure water is used as a moderator, hydrogen atoms absorb to many neutrons and 235U enriched uranium is required as fuel. Carbon and oxygen have very small thermal neutron cross sections compared to nitrogen. When Fermi built the first nuclear reactor, he used carbon (graphite) as the moderator, and he put the graphite (moderator) in cans to reduce nitrogen in reactor. The extremely large thermal neutron cross section of 113Cd makes cadmium a good neutron absorber or eliminator. The element cadmium contains many isotopes. The abundance (in %) and thermal neutron cross sections (b) are listed below: 106 c / b Abundance /% Cd 1 1.25 108 Cd 1 0.89 110 111 Cd 0.1 12.45 Cd 24 12.80 112 Cd 2.2 24.13 113 Cd 19,820 12.22 114 Cd 0.3 28.37 The abundance of 113Cd is moderate but adequate. Furthermore, the neutron-capture reaction 113 Cd (n, ) 114Cd leads to a stable isotope. These properties made cadmium a very desirable material for the nuclear technology industry. The thermal neutron cross section of fission of 235U is 160,000 times larger that that of 238U. Fission of 238U is negligible. This difference made it necessary to enrich 235U for nuclear energy and atomic bomb material. Research in the 1940s revealed another important fissionable isotope of plutonium 239Pu. Even though other isotopes of plutonium had higher cross sections than 239Pu, their half-lives are very short. The half lives and thermal fission cross sections of plutonium isotopes are given below for your reference: 236 f t1/2 Pu 150 2.9 y 237 Pu 2100 45 d 238 239 Pu Pu 17 742 88 y 24131 y 240 Pu 0.08 6570 y 241 Pu 1010 14 y 242 Pu 0.2 3.8×105y Other factors in nuclear energy considerations were methods and costs of production. All these factors led to the conclusion that only the production of 235U and 239Pu are feasible and practical. Production of 233U was not worth considering. 238 Review Questions 1. What is the significance of thermal neutron cross sections and thermal neutron cross section for fission? 2. Compare the difference in thermal neutron cross section for hydrogen and deuterium. Describe the implication of the difference. 3. What are the thermal neutron cross sections for isotopes of the following elements: boron, zirconium, and cadmium? What are the products of neutron capture reaction for the stable cadmium isotopes? What are the consequences of the capture reaction? 4. What are the abundances of uranium isotopes in natural occurring uranium? From the thermal neutron cross sections and abundance, discuss work required for using uranium as a fuel for nuclear energy generation. (Consult a hand book for the required data) Fission Products Fission products are nuclides produced in fission reactions. As suggested earlier, rubidium and cesium as two of the possible fission products. Finding out fission products is certainly a strategic project the fission research. What are the fragments produced in nuclear fission? What rays are emitted from the fission product, and why? How does radioactivity of fission products vary over time after fission? What is the distribution of the nuclides in terms of mass numbers? What is the impact of fission products on the applications of fission reactions? After capturing neutrons, the compound nuclei 236U are at excited states with excess energy. The 236U nuclei undergo fission; or emission. The half-life for fission is much shorter (10-14 s) than those of and emissions (half-life for decay is 2.3107 y). Fission is the preferred process. Since many nuclides are produced in the fission process, the study of fission products requires the separation, identification, and quantitative determination of various elements and isotopes. Since heavy nuclides contain more percentages of neutrons than light nuclides do, fission products from the fission of heavy nuclides are too rich in neutrons. Thus, fission products emit particles until they are stable. This aspect has been illustrated when we estimated the energy of fission reactions. Since the nuclei usually split into two pieces of different masses, the mass numbers of fission products range between 40 and 170. In terms of elements, they range from potassium, to tungsten, nearly all the elements in the 4th, 5th, and 6th periods, including the lanthanides*. They include alkali metals (K, Rb, Cs), alkaline earth metals (Ca, Sr, Ba), all the transition metals * We shall discuss the fission products lanthanides again in the section Natural Reactors. 239 from scandium to tungsten, metalloids (Ge, Sb, Te, Se, etc) halogens (Br, I) and inert gases (Kr and Xe). Thus, separation of fission products into various elements is a complicated operation. Some (2 to 4) neutrons are released per fission reaction. The atomic numbers of Sketch of Slow-neutron Fission Yields from fission products are difficult to 235 U as a Function of Mass Number. determine, because they rapidly undergo decay. Studies have revealed that most log(Fission yield) fission events are asymmetrical, with | heavy and light fragments, rather than | ... ... symmetric (with two equal fragments). | . . . . Relative amounts (in percentage of total | nuclides produced) of nuclides formed | . . . . are called fission yields. The plot of | . fission yields from 235U against mass | . . number gives two peaks, one between | mass 80 and 110 and the other between | . . 120 and 160. Between the two peaks is a | low yield region, the center of which | . . corresponds to a mass number 113. A | symmetric fission produces two |___.__________________________. 60 90 110 140 170 fragments of mass number 113 if no Mass no. neutron is emitted. The yield distribution depends on the kinetic energy of the neutrons, but all plots have the general feature of two peaks in similar area. The two peaks have slightly different shapes when kinetic energies of the neutrons are different. Atomic bombs and nuclear reactors are two types of fission application. Fission-product data and their behavior are of fundamental importance, because they have a great impact on the environment and society. Fission products are left following bomb explosions and reactor accidents. For example, some typical long-lived fission products such as 90Sr and 129I are used for monitoring nuclear explosions and accidents. These data are also essential for reprocessing used nuclear fuels and nuclear waste management. Management of used or irradiated fuels also depends on radioactivity of fission products. Most fission nuclides have very short half lives. After a decade, few nuclides remain radioactive. A very low yield nuclide 85K has a half life of 10.7 years, and two other nuclides, 90Sr and 137Cs have half lives of 29 and 30 years respectively. There are no fission nuclides whose half-life lies between 30 and 105 years. Fission products with half lives greater than 100 years with yields greater than 10–4 are 126Sn (1105 y), 126Tc (2.1105 y), 91Tc (1.9106 y), 135Cs (3106 y), 107 Pd (6.5106 y), and 129Tc (1.6107 y). Fission products affect the operation of reactors in many ways, one of which is the absorption of neutrons by fission products. The high-yield fission product 135Xe has a c of 2,640,000 b, and a half-life of 9.2 hours. The presence of this product lowers the level of fission, and this 240 effect is often referred to as xenon poisoning. The chain reaction of the atomic pile in Hanford suddenly stopped in July, 1944. John Wheeler, the poisoning expert, was consulted. After checking the control parameters of the reactor before the interruption, he concluded that it was the xenon. A few hours later, the reactor resumed function, and this is consistent with the half-life of 135Xe. Skill Building Questions 1. Assume two neutrons and 133Xe are produced in a fission reaction, what is the other fragment? Work out the decay scheme and show the half lives of the fission products. (Consult a handbook for required data). 2. Both 129I and 131I nuclides are produced in nuclear fission. Suggest a method for their isolation. What are the half-lives of these nuclides? What are the daughter nuclides in the decays of these fission nuclides? The First Fission Nuclear Reactor Research on uranium has been divided into several tasks. With strong financial support from President Roosevelt, some facts are well known to the inner circle of researchers involved with the uranium project. Neutrons are released in nuclear fission of 235U. Thermal neutron cross sections for many elements have been measured. Will uranium undergo a chain fission reaction? Will the chain reactions lead to a runaway explosion? Can a chain fission reaction be controlled? How to control a chain reaction to sustain for a long period of time? Since neutrons are released, uranium undergoes a chain fission reaction, when the neutrons are moderated, and sufficient number of them will cause the next generations of reaction. Firmly believed in this, Fermi’s group assembled uranium into an atomic pile to test the feasibility of a sustained chain fission reaction. They used natural uranium with graphite as moderator, cadmium in the control rod, and boron in the neutron detector. These are the key requirements for nuclear reactors. Because this was the first atomic pile, only the trial and error method was available to them. They experimented with various materials as they assembled the atomic pile. They used water as the moderator at the beginning, and it did not work. They thought water absorbed too many neutrons. They switched to graphite, still not working. They attributed the failure to the impurity in graphite, so they purified graphite, and made it into bricks. Due to high thermal neutron cross section for nitrogen (1.82 b), they put graphite and uranium into cans and removed the air from them. Step by step, they identified and solved many problems. They placed alternate layers of graphite bricks and pieces of natural uranium and constructed an atomic pile in a racquet court at Stagg Field at the University of Chicago. 241 Another major problem for the first nuclear reactor was the size of the atomic pile. Various calculations have given an estimate of the amount of required uranium, but experiments give the ultimate test. Fermi’s group built up the pile, and tested the operation as the size grew. After years of effort, the atomic pile had a sustained chain reaction of a fission nuclear reactor on December 2, 1942 (Fermi, 1955). This was the beginning of the controlled fission reaction. Its success not only provide the pile as a tool for other research, the reactor became a research tool for future reactor design. Its operation provides data for the construction of larger and more sophisticated reactors. It was indeed a great event. The way they built the first reactor was risky and dangerous in today’s standards. For example, control rods were manually handled. When the reactor was powered up for testing, the emergency measures were solutions of boron and cadmium compounds ready to be poured on to the pile by people standing on guard. On the other hand, every step was handled carefully, and the reactor operation did not have any major problems. In 1946 the first controlled nuclear chain reaction in Russia was achieved at the Kurchatov Institute, four years following Fermi's in Chicago. As of 17 August 1995 there were 425 nuclear power reactors in operation worldwide. At that time, the U.S.A. had 107 nuclear reactors in operation, generating the most nuclear power, more than twice that of France, the world second largest. According to the Uranium Institute information, (www.uilondon.org), Belgium, France, Lithuania, and Sweden, had more than 50% power supplied by nuclear reactors in 1996, whereas the U.S.A., Canada and Japan had 22, 16, and 33% respectively. Skill Building Questions 1. What is a chain reaction? In the fission reactions, what is the chain carrier? What is the principle of a fission reactor? How can a chain reaction be controlled from a runaway explosion? 2. What method was used to build and test the first nuclear reactor? (Trial and error is a powerful method for problem solving). 3. Why was water not a suitable moderator for Fermi’s first nuclear reactor? What are desirable properties for a material used as moderator? (light mass, low thermal neutron cross section, low cost of production, and desirable engineering properties) 242 The Atomic Bomb Project The US government was under pressure to complete building the atom bomb because of the threat that Germany’s ability under Hitler to build it first. In 1942 the United States put the "Manhattan Project" into effect to speed up the construction of the atom bomb. In December 1994, one of the most unusual events in postal stamp history occurred. A planned U.S. Atomic Bomb Stamp was canceled less than twenty days after it was disclosed. The stamp was a full color portrait of the atomic bomb's mushroom cloud with the caption "Atomic bombs hasten war's end, Aug 1945". It was one of a set of ten commemorative issues planned for the 50th anniversary of World War II in 1995. Thus, issues related to the atomic bombs are always controversial. A summary of events in the creation of the atomic bomb is given here because there is a lot to learn. However, you are the judge for what is valuable. The Manhattan Project The responsibility of constructing the atomic bomb was first given to the Atomic Committee of the Office of Scientific Research and Development (OSRD). In May 1942, committee members E. Lawrence, A.H. Compton, H. Urey (all three were Nobel laureates), L. Briggs, E. Murphree met with J.B. Conant, the director of OSRD. On September 23, 1942, the Uranium Committee met with Secretary of War Henry L. Stimson, Chief of Staff General George C. Marshall and other top military officers including Major General Leslie R. Groves, who was named (assigned) the Executive Officer to carry out the policy. The building of the atomic bomb was placed under the control of the military, with a head office located in New York City at the Manhattan Engineering District. Thus, it is known as the Manhattan project. What is the Manhattan project? What are the goals of the project? How did it achieve its goals? What are some of the management skills used in the Manhattan Project? How did the project involve Canada and the U.K.? The Manhattan Project was carried out under secrecy. Workers on the project were not allowed to communicate their information to each other unless they were authorized to do so. This process was called compartmentalization, and as a result some top scientists working on the project did not know the ultimate goal was to build atomic bombs. Once the Manhattan project was underway, discussion between Grove and J. Chadwick brought cooperation between Britain and America. Both governments decided to relocate the work to a place near Chicago from Cambridge, England. A joint venture between the Britain and Canada started, and a large research establishment was set up in Montreal under the 243 general direction of the National Research Council (NRC) of Canada. Practically, the whole Cambridge group under Dr. Halban moved to Montreal. In 1944, he was succeeded by J.D. Cockroft. The joint British-Canadian-American enterprise selected Petawawa, Ontario on the Ottawa River for a heavy-water nuclear reactor to produce both 239Pu and 233U, with heavy water and uranium supplied by the United States. An experimental pile was constructed near Chalk River, and a residential village of the workers was named Deep River. The first zeroenergy exponential pile (ZEEP) started operation on September 7, 1945. This was the first nuclear reactor outside U.S.A. General Grove controlled scientists working in the Manhattan project. The military mentality was and still is different from scientists, and there were constant conflict between the management and the scientists. The scientists thought building one, at most two bombs would finish the war, but Grove followed the military principle: "once you have a bomb, its constant supply must be maintained". The history of the Manhattan project is interesting, and every worker has a unique version of his or her own. To preserve the history, many top scientists were interviewed, and the records preserved. Actually, many of the workers were Nobel Prize winners, some of whom were awarded after World War II. This results in the publication of many books, and there is plenty of information available from the Internet maintained by U.S. government libraries. There are some official versions of the history, but personal reflections are more interesting to read. Many aspects are associated with the Manhattan project. These aspects range from chemistry to chemists, from physics to physicists, from engineering to engineers, from civilian to military, from war to peace, from victory to defeat and from history to technology. Whatever your interests are, you can always find something in this great human endeavour which started with a simple objective of building a powerful bomb. However, once started, it has developed into perhaps the most important project of human history. Many sections in this Chapter is part of this project, and you may also find a lot to read on the Internet as well as in the Library. Skill Developing Questions 1. What are the purposes of the Manhattan project? (problem solving). 2. How did the Manhattan Project affect the nuclear technology on Canada? What role did Canada play in the Manhattan Project? 3. What type of person was General L. Groves? He was not a scientist, and the building of the atomic bomb was a scientific challenge. How did Groves manage his difficulty? Who are his advisors? 244 Producing Materials for Atomic Bombs The Manhattan Project was established to apply nuclear fission for the construction of atomic bombs. Extensive research has established that 235U and 239Pu were practical fissionable nuclides. These were the most desirable commodities for the atomic bomb construction. Furthermore, they were required for testing related to the design, and eventually the making of the bomb. 235 239 How can pure 235U and 239Pu be produced? What are the methods for their preparation or production? What was the principle used for each method? U Pu At the start Several methods for the production of fission material were proposed, but at that stage, none was a guaranteed success. For uranium, the tasks were to separate* 235U from natural uranium which consists of 0.7% 235 U and 99.3% of 238U. The production of 239Pu involved synthesis of an entirely new element. Urey's research group had extensive experience with gas diffusion. They knew that gas molecules with different molecular mass could be separated by a diffusion method. They also learned all properties about the compound UF6. Thus, they suggested a separation of 235UF6 from 238UF6 using a gas diffusion method. Lighter molecules pass through membranes containing pin holes faster than heavier molecules. The molecular weight of 235UF6 is 389 compared to 392 for 238UF6. A gas of UF6 made from natural uranium contains both 235UF6 and 238UF6. When this gas passes through membranes and long tubes, the gas that first comes through contains a little more 235UF6. After many stages of concentrations, the gas is more concentrated with 235UF6. This is known as the gas diffusion method. Since the molecular weights differ so little the industrial operation is a long and laborious process. Another method suggested by Urey’s group is called the centrifuge method. The group wanted to create a strong field of gravity by high-speed centrifugation for the separation of the lighter gas. Like the gas diffusion method, the centrifuge method feeds UF6 gas into a series of vacuum tubes 1 to 2 meters long and 15-20 cm diameter, each containing a rotor. When the rotors are spun rapidly, at 50,000 to 70,000 rpm, the heavier molecules 238UF6 increase in concentration towards the cylinder's outer edge. There is a corresponding increase in concentration of 235UF6 molecules near the center. Enhanced concentration is further achieved by inducing an axial circulation within the cylinder. The enriched gas is drawn off and goes forward to further stages while the depleted UF6 goes back to the previous stage. * For uranium enrichment, consult http://www.uic.com.au/nip33.htm and http://www.fas.org/nuke/guide/usa/facility/portsmouth_oh.htm, and http://www.npp.hu/uran/3diff-e.htm 245 To obtain efficient separation of the two isotopes, centrifuges rotate at very high speeds, with the outer wall of the spinning cylinder moving at between 400 and 500 meters per second to give a gravitation field a million times that due to the Earth. Lawrence's group in California has built machines to accelerate particles, and they knew well how to manipulate the behavior of particles. The group suggested an electromagnetic method to first ionize the UF6 molecules, accelerate them by electric field, and then bend them by a magnetic field. Due to the mass difference, 235UF6+ and 238UF6+ would bend along different curvatures in an electromagnetic field. Uranium Isotope Enrichment by the Electromagnetic Method. Another method called thermal diffusion to enrich 235U developed in the Naval Research 238 From a UF6 Laboratory was by Philip Abelson, who explored 235 particle collector UF6 nuclear energy for submarine propulsion. This accelerator collector project was led by Ross Gunn. The method also makes use of UF6. Liquid UF6 is placed in the middle layer of three long vertical concentric pipes. Hot steam at 550 K is sent through the inner tube and warm water at 340 K is sent through the outer layer. The liquid UF6 in the middle layer is sandwiched between two different temperatures, and this causes the lighter 235UF6 to rise to the top and be collected. Because hot steam is required, this method consumes too much energy, and the top portion is only slightly enriched in 235U. The naval research lab was not part of the Manhattan project. But the slightly enriched material sped up the enrichment process using the electromagnetic method. Despite the strained relationship between Ross Gunn and the Atomic Committee, the thermal diffusion technique was also adopted in Oak Ridge for the mass production of 235U. Plutonium can be produced by bombarding 238U with fast neutrons, from particle accelerators and from nuclear reactors using either graphite or heavy water as moderators. After a full day of discussion, the Atomic Committee could not decide whether to eliminate even one technique. They recommended to President Roosevelt to support all methods for the production of fissionable material. Facing a national emergency, Roosevelt authorized an all out effort for the production of 235U and 239Pu. Skill Developing Questions 1. What methods are available for the enrichment of 235U? Describe how each of the method works. 2. How can 239Pu be produced? (Review Nuclear Reactions). 246 Critical Masses Neutrons outside a nucleus decay with a half-life of 12 m. They are also absorbed by other materials than nuclei of 235U or 239Pu. Only fractions of neutrons from fission are captured by 235 U nuclei leading to another fission reaction. In a small quantity of fissionable material, so few neutrons induce fission reactions, and a chain reaction will not be sustained. The minimum quantity for a sustained chain reaction to take place is called the critical mass or critical size. Of course, the critical mass depends on the moderator, chemical and physical states, shape etc. In general, the term refers to the minimum quantity for an explosion. What are the critical smasses of 235U and 239Pu? How can they be determined? How to design and build devices for their investigation? There are many factors to consider in order to estimate the critical masses for 239Pu and 235U: the cross sections of all materials involved, the volume, the half life of neutrons, path of neutrons etc. Thus, estimates must be verified by experiments. These experiments were extremely dangerous, because an accidental assembly of a critical mass would lead to an explosion. The experiment to determine the critical mass was called tickling the dragon's tail. It was done at night in the remote Omega Canyon. By 1944, enough 239Pu was produced. A fearless 32-year old Canadian from Winnipeg called Louis Slotin was one of the workers who performed these experiments. They operated a strange machine called the "Guillotine". Pieces of fission material dropped from the top of the Guillotine. The neutron intensity was monitored as the piece dropped and past an almost critical assembly. As larger pieces were used, the neutron activities increased. Using the Guillotine, the two pieces were in contact for a very short period, and they had hoped the short contact time would limit the chance of a nuclear explosion. The Idea of a Guillotine for Critical Mass Determination Neutron monitoring devices Releasing mechanism 235 239 U or Pu Today the critical mass is known to be 300 g (2/3 lb) and 900 g (2 lb) respectively for pure 239Pu and 235U. The critical mass depends on the shape and purity of the sample. Shortly after the war, L. Slotin, died in an accident due to overdose of neutron radiation, when he, on May 21, 1946, separated an explosive assembly to protect his colleagues in the room with his bare hands. As mentioned at the start, the critical mass depends on the shape and other factors. To further reduce the critical mass for atomic bombs, the Manhattan Project used explosion around chunks of fission material to reduce the volume to increase the efficiency of neutron capture. 247 Atomic bombs are sophisticated devices, their design and construction are secretive. Nuclear weapons include warheads for strategic ballistic missiles, smaller tactical nuclear weapons, artillery projectiles, demolition munitions (land mines), antisubmarine depth bombs, torpedoes, and short-range ballistic and cruise missiles. The U.S. stockpile of nuclear weapons reached its peak in 1967 with more than 32,000 warheads of 30 different types; the Soviet stockpile reached its peak of about 33,000 warheads in 1988. Skill Developing Questions 1. Why is there a minimum mass requirement for a sustained chain reaction? What is the meaning of critical mass? 2. How would you design an experiment for the testing of a critical mass for a nuclear reactor design or bomb design? 3. Why are the critical masses of 235U and 239Pu different? Nuclear Bomb Explosions Under the management of Leslie Grove and the leadership of many top scientists such as Luis Alvarez, Herbert Anderson, Hans Bethe, Niels Bohr (code name Nicholas Baker), Lyman J. Brigs, James Chadwick, Arthur H. Compton, James B. Conant, Enrico Fermi, Richard Feymann, Otto Frisch, James Franck, Clarence Johnson, Ernest Lawrence, Willard Libby, John Marshal, Robert Mulliken, Edgar V. Murphree, Robert J. Openheimer, I. I. Rabi, Glenn T. Seaborg, Emilio Segrè, Leo Szilard, Edward Teller, Robert L. Thornton, Harold C. Urey, Eugene Wigner, Walter H. Zinn* , etc., Large quantities of 239Pu and 235U have been produced. What kind of and how many workers were involved in building the atomic bomb? How was the work divided in the Manhattan Project? When and under what circumstances were the first three atomic bombs exploded? What are the dangerous effects of atomic explosions? The business of building the bomb started with research in the basic sciences of mathematics, chemistry and physics. Scientific results were applied by engineering design, manufacture, and processing through management. Jobs involved research, design, engineering, construction, operation and management. Enormous financial resources (forms of power) have been allocated to the Manhattan project, which recruited a large number of workers. Two major sites of fission material production facilities were the 59,000-acre Oak Ridge and the 450,000-acre Hanford Engineer Work. The total work force in the two areas was 125,000, and many of them had advanced degrees. Openheimer was the director for the design and construction of the atomic bomb in a third site called Project Y (Los Alamos Laboratory) within the Manhattan Project. Enormous amounts of work were done outside these sites. * Walter H. Zinn was a native of the Kitchener-Waterloo area. 248 Almost the whole of United State, Canada, and the U.K. were engaged in making the atomic bombs. A nuclear explosion is an uncontrolled nuclear fission. When a critical mass is assembled, neutrons from the natural fission process initiate a chain reaction. The number of nuclei undergoing fission reactions increases rapidly leading to an explosion. The energy released in fission reactions blow the fission material apart, and at some point, the chain reaction stops. In order to get a high efficiency, the construction of a bomb is more sophisticated. Using chemical explosives around the fission material causes an implosion that compresses the fission material into a high-density assembly. This construction not only reduces the critical mass, it confines the material from flying apart until most of the fission material was used up. The Implosion Arrangement Ignition points Chemical explosive 239 Pu Fission material is surrounded by chemical explosive which is ignited at many points simultaneously. The explosion forces pieces of 239Pu together and even reduces the volume to reduce the critical mass. On July 16, 1945, a plutonium (Fat Man) bomb was tested in the desert area called Jornada del Muerto (Journey of Death), part of the Alamogordo bombing range in southern New Mexico*. Two hemispheres of plutonium, attached to a 30-meter steel tower, was forced to fuse together by implosion so that they formed a critical mass for a rapid chain reaction (Rhodes, 1986). This is known as the Trinity Test, which was estimated to have cost (1945) US$2,000,000,000. Although the resignation and arrest of Mussolini on July 25, 1944, and suicide of Hitler on April 30, 1945, ended the war in Europe, Japan was still engaged in fierce fighting with the U.S. in the Philippines. Besides, Japan had occupied a large part of China, Vietnam, Malay Peninsula, all of Korea, Hong Kong. Thus, work on the atomic bomb did not slow down. Three weeks after the Trinity Test at 8:15 am local time on August 6, 1945, the atomic bomb Little Boy was dropped on Hiroshima by a modified (to carry the A-bomb) B-29 bomber. The 235 U-fueled bomb exploded 660 m above the city to eliminate local fallout. Two pieces of 235U were loaded into a special gun, one at the muzzle, and the other in the barrel. When fired, the two pieces with a combined weight of 60 kg contacted, a critical mass was reached, and explosion followed. The explosive energy was equivalent to 20,000 tons of TNT. The 235U bomb has never been tested before. Note that pieces were brought together to reach the critical size in different fashion, due to the property difference between uranium and plutonium. Three days later on the 9th, a 239Pu-fueled bomb exploded over Nagasaki, destroying half of the entire city. This bomb is the same type as the Fat Man used in the Trinity Test. The heat * For more on The Trinity Site, New Mexico consult http://www.viva.com/sw.trinity.html 249 and light emitted when the bombs exploded were so intense that everything within 1000 m vaporized. The explosion was seen as far as 300 km. Following the light and energy release is the explosion shock wave that destroyed buildings and deafened ears. Secondary fires caused further destruction. Earthquake detection instruments around the world measured the shock wave. The fallout and radioactive fission products caused short-term and long-term health problems for an indefinite period of time. A total of 130,000 died in the two explosions. Many of the injured were left in such an awful condition that they envied the dead. In Germany, the War Office received enthusiastic letters in April 1939 for military Sixteen hours ago an American airplane dropped one application of nuclear fission. Experiments bomb on Hiroshima, Japan, and destroyed its of chain reactions using uranium and usefulness to the enemy. That bomb had more power graphite were planned. Werner Heisenberg than 20,000 tons of T.N.T. .... had erroneous results about the graphite Harry S. Truman 1 experiment, and recommended that heavy water be used as moderator. The German team had enriched uranium to contain 1% 235 U for the project. Several times, Allies’ bombing destroyed the prototypes. The project was still at the experimental stage when Germany was defeated. The German bombs, moderated by heavy water, had such enormous sizes that they would have had to be delivered by huge trucks or ships. The Joliot-Curie team in France and the British weapon project also started work on the possibility of building an atomic bomb, but neither had developed to the stage of actually building the bomb at the end of WW II. Skill Building Questions 1. How do the masses come together to reach critical masses in atomic weapons? 2. How do atomic bombs destroy and what are the differences between atomic bombs and chemical explosives? What are the four stages or means of destruction by nuclear weapons? ( radiation and heat, shock wave, secondary fires, fallout and radioactivity) The Nuclear Arms Race During World War II, the Soviet Union under the leadership of Stalin competed with the U.S. and Britain for military superiority, even though the Soviets fought Hitler together with the Allies. The cooperation between the United States and Britain (Canada was part of Britain at that time) in the Manhattan Project made the competition fierce. The U.S. was, and still is, the leader of the North Atlantic Treaty Organization (NATO), and the competition between the communist block and the capitalist block is known as the cold war. The period lasted more than 40 years until the communist block disintegrated due to economical failure of the communist system, which did not give incentive for hard working. 250 Since the beginning of the Uranium project in the U.S., information and results on uranium research were treated as top secret. Spy wars between the two blocks not only heated up the cold war, but they raised much psychological tension in everyone’s mind living during that time. Why are results of scientific research treated as top secret? What information is secret? Why nations spy on each other? How did the former Soviet Union carry out the atomic and hydrogen bomb projects? The secret of science is for everyone to discover, but research is costly in terms of time and manpower. Thus, nuclear data and principles are considered top secret. Spy activity for atomic data and information is practiced. In the Soviet Union, Igor Vasilyevich Kurchatov (1903-1960), first observed the fission reaction in 1934 and he wrote a book called Splitting the Atomic Nucleus in 1935*. He built cyclotrons for the study of radioactivity. In 1939, Kurchatov and his coworkers published studies of nuclear chain reactions. The Soviet scientists also learned the German discovery of fission reactions. However, their work on uranium was suspended when Germany invaded Russia. The Soviet government needed scientific and technical strength for weapons of more immediate value (Britannica, 1973). After Germany surrendered at Stalingrad on February 2, 1943, Stalin heard of the American effort to build atomic bombs. He ordered the program to be re-established in 1943 under the control of Kurchatov. Soon, other physicists joined the panel. By late 1940, Igor Kurchatov and others in Leningrad started studies on nuclear reactors after having learned of nuclear reactions. One of Kurchatov's students observed the gradual disappearance of articles on fission in US journals, and he wrote an impassioned plea to several outstanding USSR physicists and the State Defense Committee to continue research on the chain fission reaction. The government and Soviet scientists reacted to it, and the Uranium Institute was established in Moscow. The most noted spy within the Manhattan project is Klaus E.J. Fuchs (1911-1988). He was a German born physicist who joined the German Communist Party in 1932 while he was a student at the University of Kiel. He became a British citizen in England. When Otto Frisch told him to come to the U.S. to work on the atomic bomb program, he went to the Soviet Embassy in London. During his time in the U.S. he was regularly contacted by the Soviet intelligence chief Gaik Ovakimian via H. Gold. He supplied the Soviet with a treasure house of information about the atomic bomb, including the design of the 235U and 239Pu bombs. As a result, the Soviets were well informed of the Manhattan project. The secret material was codenamed the "candy", and Gold was the "candy man" (Brown and MacDonald, 1977). * If the year is accurate, Kurchatov discovered fission before the German group did. 251 The "candy" certainly helped the Soviet nuclear program. Four years after the explosion in Hiroshima, the Soviet Union detonated her first atomic bomb on August 29, 1949, much to the astonishment of the U.S. government, and after confirmation by U.S. scientists, president Truman informed the public of the explosion on September 23. Americans were alarmed, and this led to the speedy development of the hydrogen bomb under the leadership of Edward Teller in the US. Two years after the U.S. tested a thermonuclear (hydrogen) bomb, the Solviet's also tested one. The cold war heated up and the arms race became frantic. Both the U.S. and the Soviet Union have developed so many fission- and fusion- bombs that they could have destroyed the world had there been a war. Bethe hypothesized that most of the energy from the stars, including the sun, is derived from fusion reactions, and soon after the World War II, efforts were directed towards the creation of a weapon of tremendous power by utilizing fusion. In 1952-1953, the so-called hydrogen bomb became a reality. Skill Developing Questions 1. Highlight some of the events of the Cold War? (Korea war, Vietnam war, Berlin wall, Cuba crisis etc. You will get thousands of sites searching with the key word “cold war”.) 2. In your opinion, what event marks the end of the cold war? (Have an idea of your own, rather than take others’ words for granted) 3. What are the worst threat during the cold war? How does the end of the cold war affect our lives? 4. Had the cold war not ended, what can and shall we do? 252 Nuclear Reactors Having seen the devastation of atomic bombs, scientists, including those who worked on the Manhattan project, campaigned against further nuclear weapon development. They wanted to turn the giant industries associated with the Manhattan project into peaceful applications, especially as an energy supply. Classified by purpose, there are two types: research and power generation nuclear reactors. Research reactors provide subatomic particles for experiments and for working out the parameters for reactor design, but power reactors are used for converting nuclear energy into electric energy. Either one may be a breeder, which produces more fissionable material than it consumes. All reactors make use of fissionable heavy nuclides 235U or 239Pu. Controlled Nuclear Fission Reactions Unlike uncontrolled nuclear explosions, chain fission reactions are controlled to maintain steady states in nuclear reactor technology. The energy released is diverted away to serve our needs. What are the key components of fission reactors? How can we control chain fission reactions from explosions? How can fission energy be diverted? Designs of fission reactors are complicated with much of the work done by engineers, particularly nuclear engineers. However, the basic principle for nuclear reactor is simple. A reactor has some basic components: a reactor core holding fission material or fuel; moderator, control rods holding neutron absorbers, monitoring devices and indicators of operation, and an energy transfer system. Basic Elements of Fission Reactors Control rods moderator Reactor Core Energy transfer system Monitoring Both natural uranium and 235U enriched devices uranium have been used in power reactors. The melting point of uranium is 1403 K, but uranium metal undergoes a phase transition at 933 K. The structure change in phase transition limits the operating temperature to below 933 K. The melting point of UO2 is 3138 K. Thus, most modern reactors employ uranium oxide pellets as fuel. The pellets are clad in either stainless steel or Zircaloy. Zircaloy is zirconium (Zr) with 1% tin, and very small amounts of other metals. Its usage was due to low thermal neutron absorption (about 1.5 b compared to 2.5 b for iron). Zirconium is a hard, lustrous, silvery metal, very corrosion-resistant due to the formation of an 253 oxide layer coating, but will burn in air. It is unaffected by acids, except hydrogen fluoride (HF), and alkalis. It has several isotopes with masses between 90 and 96, with an average thermal neutron cross section s = 0.184 b. Stainless steel is preferable to Zircaloy for hightemperature, sodium-cooled reactors. Since neutrons from fission reactions are fast or high energy neutrons, they have to be slowed down in order to be captured by fissionable nuclei. Moderators are compounds containing light nuclides such as 1H, 2D, 4He, 12C, 16O, 19F. The common substances suitable for moderators are: graphite, H2O, D2O He (100 Atm and 1273 K) Be (high temperature liquid metal). Na (773 to 873 K used in breeder reactor) BeF2 + ZrF4 ( for GCR) Combinations of moderators and coolants have been used for reactors. Rates of fission reactions are proportional to the numbers of neutrons in the core area, and these numbers are controlled by lengths of control rods in the core area. Control rods are made of materials with high thermal neutron cross sections. These include: Cadmium, Boron, Carbon, Cobalt, Silver, Hafnium, and Gadolinium We have discussed the thermal neutron cross sections of cadmium earlier. Cadmium is the most common material considered for control rods. However, the requirements for fission reactors are different from nuclear bombs. Another effective neutron absorber is gadolinium, which consisted of the following isotopes. Their natural abundances and neutron capture cross sections are given: 152 Gd Abundance /% 0.20 c / b < 125 154 Gd 2.15 90 155 156 Gd 14.73 61,000 Gd 20.47 2 157 Gd 15.68 255,000 158 Gd 24.87 2.4 160 Gd 21.8 0.77 There are two isotopes of Gd that are particular potent for capturing neutron, both have odd number of nucleons. Neutron capture reactions 155Gd (n, ) 156Gd and 157Gd (n, ) 158Gd lead to stable isotopes of the same element. The monitoring system consists of neutron, alpha, beta, and gamma detectors as well as thermometers and liquid flow meters. Neutron intensities and radioactivity of some fission products are monitored constantly, and all readings are displayed in control rooms. Careful measurements before let to a comprehensive system for operation of the reactor. The energy transfer system takes heat released from fission reaction away from the core by pumping a cool fluid (gas or liquid) to the core. Skill Building Questions 254 1. What are the key components of nuclear reactors? What materials are used in each of the components? 2. Why are uranium and plutonium oxides instead of metals used for the core of fission reactors? What are the key requirements of nuclear reactors in terms of chain reactions? 3. What elements are good moderators? 4. What elements are commonly used for the construction of control rods and why? 5. What is the form of energy released in nuclear fission? How can the energy be diverted away? How is the energy delivered to industry and home usage? Types of Nuclear Reactors After the war, the United States set up a Civilian Power Reactor Program (CPRP) to coordinate the study of nuclear reactors for peaceful application of nuclear energy. The Atomic Energy of Canada, Limited was and still is the Canadian body for nuclear technology applications. Electric energy was seen as the basic utility to benefit the society the most. How does one build an effective nuclear reactor for electric power generation? Why are there so many types of nuclear reactors? The first few nuclear reactors were built to study how nuclear reactors function, and perhaps to produce plutonium for atomic bombs. After WW II, CPRP was set up to find out the most economical and safe way to convert fission energy to electric energy. The Program decided to investigate the following eight types of power reactors: Fast Breeder Reactors (FBR) Aqueous Homogeneous Reactors (AHR) Heavy Water Moderated Reactors (HWR) Pressurized Water Reactors (PWR) Boiling Water Reactors (BWR) Organic-Cooled Power Reactors (OCPR) Sodium Graphite Reactors (SGR) Gas-Cooled Reactors (GCR) Although this is not an exhaustive list, it gives a good summary of various ways to construct nuclear reactors. This list is a result of human ingenuity in turning scientific discoveries into applications. Fast breeder reactors are unique in that they are designed to produce fission material 239Pu or 233 U while generating electric energy. Large amounts of 238U capture fast neutrons and produce 239 Pu by the reaction 238U (n, 2) 239Pu. When 232Th is used instead of 238U, 233U is produced by the reaction 232Th (n, ) 233U. Since neutrons at higher energy are required, water is not a suitable moderator. Most FBRs use molten sodium as a coolant because it is economical, and compatible with other structural materials. Sodium boils at 1153 K, and thus there is no need to pressurize it. It is also a good thermal conductor, and the hot liquid from the reactor core 255 can be used for steam generation. FBRs require 20 to 30% fissionable material to produce enough neutrons to reach critical operation. As a result, the cores are smaller (1.5 m diameter by 0.9 m high) than the thermal reactors. Aqueous homogeneous reactors (AHR) are also unique in that they have no cores. Compounds of fission material are dissolved in a solution. The fission fuel and moderator are in one homogeneous phase. Accidental explosions of large tanks of uranium solutions (passing critical sizes) have been known. These tanks are uncontrolled homogeneous reactors. Heavy water moderated reactors (HWR) are moderated by heavy water 2D2O. Typical examples of HWR are the CANadian Deuterium Uranium (CANDU) Reactors. Using heavy water as the moderator, natural uranium instead of 235U enriched uranium is used. Producing heavy water is a simpler process than enriching 235U. Boiling water reactors (BWR) operate at the boiling temperature of the water (373 K) in the reactor core zone. Steam is generated and passed directly to the turbine for electric energy generation. The disadvantage of this system is the radioactive steam in the turbine. The boiling of water at the core made the water an ineffective moderator, resulting in operational problems. Thus pressurized water reactors (PWR) operating under high pressure by multiple pumps are more practical. The Westinghouse PWR operated at a pressure of 2500 psi (pound per square inch), and pumped 93,000 gallon per minute. The coolant temperature ranges from 560 to 600 K (Masche, 1971). This coolant went through a heat exchanger to convert water into steam for driving turbines of generators. The efficiencies of PWRs are about 30%. Because of the success of pressurized water reactors, there has been talk about boiling heavy water reactor (BHWR) or pressurized heavy water reactors (PHWR). In these reactors, natural uranium can be used because of lower thermal neutron absorption of the heavy water. Sodium graphite reactors (SGR) are moderated by graphite (12C) and cooled by molten sodium metal. The design of these reactors is similar to that of fast breeder reactors. Natural uranium is used as fuel when graphite is the moderator. These reactors produce 239Pu. When the core is cooled by other gases, they are called advanced gas-cooled reactors (AGR). The first AGR was built to produce plutonium for atomic bombs. The first AGR for electric power generation was planned in the U.K., to take advantage of the experience already gained in the plutonium production reactor. There are two AGRs in Hinkley Point and in Somerset, U.K. They started power generation in 1976. The CO2 enters the core at 567 K and leaves at 918 K to heat the water coil for steam generation. A few AGRs are in use in the U.K. and France, but both countries have switched to light water reactors using enriched uranium. The AGRs can reach a net efficiency of 40%. Skill Developing Questions 1. Name five types of reactors and give a short description for each type. 256 2. Do fast breeder reactors create energy? Is the principle of energy conservation violated in the FBR technology? 3. What are the advantages and disadvantages of the CANDU reactors? Breeder Reactors For fear of running out of supply in the future, scientists and engineers tried to build fast breeder reactors (FBR) that produce more fuel than they consume while generating power. Why are breeder reactors desirable? What are some of the general characteristics of FBR? What nuclear reactions can be used to breed fission material? Which type of breeder reactor is the most economical? How many breeder reactors have been built? How many breeder reactors are in operation today? According to the type of fuel bred, there are two types of breeder reactors. The 233U cycle (or thorium cycle) makes use of the reactions, 232Th (n, ) 233U. Some related data regarding this cycle are given below: Th (half life, 1.4×1010 y) + n 233Pa + , (c = 7.4 b, f = 5.6×10-5 b) 232 Pa ( , ) 233U 233 (half lives, 27.0 d for 233Pa, and 1.6×105 y for 233U). The thorium cycle breeder reactors require thermal neutrons. Molten metal and cold water are used as the coolants. The 239Pu cycle (or the uranium cycle) makes use of the reaction U + n 238 239 U (c = 2.7 b) U ( , ) 239Np ( , ) 239Pu 239 The uranium cycle breeder reactors require fast neutrons. Liquid metal and steam may be used as coolants for fast breeding. 257 The cores of breeder reactors are small but they contain highly enriched fission fuel. The enrichment reach 40 to 60% compared to 3% for HWRs. The cores are Boron blanketed by layers of 238 232 graphite U or Th to absorb shield the escaping neutrons. Molten sodium or other metal is used to transfer the heat of fission from the core to the heat exchanger for power generation. Basic parts of a FBR is illustrated here. Basic Elements of a Fast Breeder Reactor Fuel loading machine B R E E D E R Core Magnetic pump B L A N K E T Heat exchanger The FBRs have been in operation in the U.S., U.K., France, the former U.S.S.R., Japan, and perhaps in China. In the U.S., Experimental Breeder Reactor No. 1 (EBR-1) began operation in December 1951. The core had an approximate diameter of only 21 cm and a total volume of 6.2 liter. The core power was 960 kw. During one of the critical experiments, the reactor had a melt down in Nov. 1955. The Experimental Breeder Reactor No. 2 (EBR-2) had a power rating of 60 Mw. A bigger Enrico Fermi Atomic Power Plant was designed to give 300 Mw. There had been considerable interest in developing reactors for aviation and ships. Many submarines are powered by nuclear reactors. The United State cooperated with France and England in these ventures, and the former USSR had its own program. Fast breeder reactors burn a large fraction of uranium, and the fuel costs were low. The heat produced in these reactors can be used for power generation and other functions. In Britain, the first FBR was built at Dounreay (Scotland), and it started operation in 1959. This reactor core contained 46.5% 235U enriched uranium metal clad in niobium tubing. These tubes formed a hexagonal array 0.54 m in diameter, and 0.54 m in height. The small reactor core and the blanket produced 60 Mw thermal energy, and required a sophisticated cooling system to handle. The electric power from this reactor was 14 Mw, giving an efficiency of 23%. The total mass of uranium was 220 kg. The breeder blancket contained 20 tons of depleted uranium. The reactor was shut down in 1977. It served well, and it provided data for the construction of bigger FBRs. A larger one built at the same location became operational in 1974. Russia had a prototype called BN 350, which started operation in 1970. A French prototype Phenix started in 1973. Phenix output an electric power of 250 Mw, and the next generation Super Phenix, which generated 1200 Mw electric power, became operational at Creys Malville 258 in 1985. This is a pool type reactor with a core of 3.66 m in diameter by 1 m high and contains 32 t of uranium and plutonium oxide with plutonium concentration of 15% in the center increasing to 18% in the outer elements. The coolant is 3200 t of molten metal. A Washington Representative of The Federation of Electric Power Companies of Japan recently wrote: ”To maximize these benefits on a long-term basis, the commercialization of fast breeder reactor (FBR) technology remains the long-term goal in Japan's future energy program. To attain this goal, the Power Reactor and Nuclear Fuel Development Corporation (PNC) has developed both an experimental and a prototype FBR. The experimental reactor "JOYO" has been operational since 1977. In April 1994, the prototype reactor "MONJU" reached criticality.” Thus, breeder reactors are actively being studied despite the bad publicity of nuclear reactors due to accidents in recent years. Skill Building Questions 1. What fission fuels are produced from breeder reactors, and by what reactions? 2. Describe some design features of a breeder reactor. 3. What is the future of breeder reactors? The CANDU Reactors The governmental body for nuclear technology in Canada is the Atomic Energy of Canada Limited (AECL). It has played a key role in the development of nuclear technology in Canada, including the development of the CANadian Deuterium Uranium (CANDU) Reactors. Why are the CANDU reactors unique? What are the unique features? What are the advantages and disadvantages of CANDU reactors? Most fission processes generate on the average between 2 to 3 neutrons per fission. The neutron yields depend on the temperature of the moderator, and the following are some typical average neutron yields for neutrons of various energies. 235 U + n(0.025 eV thermal) fission + 2.42 n. 235 U + n(fast) fission + 2.58 n. 233 U + n(thermal) fission + 2.49 n. 233 U + n(fast) fission + 2.59 n. 239 Pu + n(thermal) fission + 2.88 n. 239 Pu + n(0.5 MeV fast) fission + 3.0 n. Some of these neutrons are captured by fissionable nuclides leading to another fission to maintain the chain reaction, but most are wasted because they are absorbed by the moderator, 238 U, and the supporting structural material of the reactor. If each generation of neutrons fails to produce at least as many fission reactions in the next generation, the chain reaction stops. Natural uranium contains only 0.7% 235U. The combined absorption of 238U and 1H2O in the moderator made natural uranium impractical as a fission fuel. The much smaller thermal 259 neutron cross section of 2D made heavy water D2O an attractive moderator for using natural uranium as feeding stock for nuclear reactors. The first heavy-water-moderated, light-water-cooled reactor, research reactor NRX was commissioned in 1947. Natural uranium metal sheathed in aluminum was used in the core. Its success led to the commission of NRU ten years later. NRU was a 200-Mw-research reactor, moderated and cooled by heavy water. Later a nuclear power demonstration (NPD) station was built at Rolphton, Ontario, Canada's first venture into power reactors and the first heavywater nuclear power plant in the world. NPD was a 20-Mw prototype, and it provided data for the design and construction of CANDU reactors at Douglas Point Ontario, which was built with the cooperation between AECL and Ontario Hydro. The CANDU reactors are a successful venture in reactor technology. Some features of CANDU reactors are described below. (1) Today, 22 CANDU reactors supply 20% of electric power in Canada. AECL sold the first CANDU reactor to Argentina in 1974. It and one sold to Republic of Korea become operational in 1983. Some have been sold to India and China. (2) The fuel tubes are tied together to form bundles, which are loaded into horizontal tubes of the reactor cores for CANDU reactors. Fuel bundles can be replaced without having to shut down the reactors. The Pickering Unit 7 sets a world record for continuous operation of 894 days without a shutdown. (3) CANDU reactors use natural uranium oxide as fuel, eliminating expensive enrichment process, but they require heavy water as moderator. Extracting heavy water is probably more economical, but new methods for 235U enrichment may off set the cost in the future. (4) Using natural uranium as fuel generates larger volumes of nuclear wastes in CANADU reactors. More space is required to dispose CANDU nuclear wastes compared to reactors using 235U enriched uranium as fuel. However, CANADU reactors also produce 239Pu, but the costs for processing 239Pu is also higher than those from FBRs. Recently, the web site (http://www.aecl.ca/) of AECL gave the following statements in its overview: “Atomic Energy of Canada Limited (AECL) was established in 1952 as a Crown corporation and reports to the Parliament of Canada through the Minister of Natural Resources. AECL's mandate has naturally evolved over the decades from the development of peaceful applications of nuclear energy to a focus on its flagship product, CANDU power reactors, and MAPLE research reactors. AECL develops, markets, and manages the construction of CANDU power reactors, MAPLE research reactors, performs associated R&D, carries out underlying reactor research, supplies CANDU and light water reactor (LWR) support services, and offers radioactive waste management products and services. AECL and its Canadian and international business partners have designed, engineered, supplied components and managed the construction of CANDU units on four continents. The CANDU reactor is ideally suited to providing the electricity requirements in the rapidly-growing economies of the Asia-Pacific region, and in other countries around the world. For more about CANDU reactors, visit the web site of AECL (aecl.ca). There are some photographs about the nuclear core and reactors. 260 Skill Developing Questions 1. What are the unique features of CANDU reactors? 2. What are the advantages and disadvantages of CANDU reactors? 3. Ontario Hydro uses CANDO reactors for power generation. Find out the following: number of reactors in operation, number of reactors in idle, amount of power generated by each reactor, total power consumption in Ontario, percent of power supplied by nuclear reactors, other means of power generation and their share of power generation, and power export or import in Ontario. Nuclear Reactor Accidents From scientific or engineering point of view, an accident is a series of undesirable events that took place due to accumulated causes. A full disclosure of the background information and of the details of the events helps to improve future design and operation. An accident is costly in economic, cultural and social terms. Nuclear accidents attract attention, because of the radioactivity associated with them. How safe or unsafe are nuclear reactors? What major nuclear accidents have happened in the past? What are the major causes of these accidents? For each case, what are the events taking place in sequence? What can be learned from the accidents? How can the accidents be prevented? What are the consequences of accidents? As early as 1952, a heavy-water-moderated light-water-cooled experimental reactor in Chalk River had a partial melt down. Some radioactive materials were released, but in those days, nuclear events were top secret. In 1958, a fuel element in another HWR was not cooled, but radioactivity was contained. Graphite fire occurred in a graphite-moderated gas-cooled reactor in Britain. About 20,000 Ci of radioactive 131I were released. Steam explosion and graphite fire was blamed for the Chernobyl reactor accident near Ukraine in 1986. Sodium-cooled fast breeder reactors at Lagoona Beach (near Detroit) in the U.S. experienced a cooling system blockage resulting in a partial meltdown in 1966. A secondary sodium leak happened to a similar reactor in Japan in 1995. Some accidents have also happened for light water reactors. The Three Mile Island reactor accident that happened in 1979 involved a PWR. A BWR belonging to the U.S. army near Idaho Falls exploded in 1961. Accidents do happen despite great effort made in their prevention. Those mentioned above were some of the reported accidents, but there are other unreported nuclear reactor accidents. To date, there are about 500 nuclear power reactors in the world, and the number is increasing. 261 Events in two well-known reactor accidents illustrate some problems encountered in nuclear power technology. The accidents already have had their social and economical impacts due to extensive reports in the media. These reports concentrate on the damages and effects, rather than how the accidents have happened. Those contain technical details appeared only in scientific and technical journals. Experts are more interested in the events leading to the accidents than the phenomena of accidents, because they want to learn from the events to give better designs, policies and guidelines to prevent or reduce accidents in the future. Three Mile Island Accident: Reactor number 2 on Three Mile Island (TMI-2) was a pressurized water reactor (PWR) designed to generate 3000 Mw heat (Thomas, 1980 and Martin, 1980). The reactor core consisted of 93 metric tons of UO2 made with enriched uranium. The UO2 powder was pressed, sintered into pellets of 9.4 mm in diameter, 45 cm length. The pellets were stacked inside Zircaloy-4 cladding tubes of 10.9 mm diameter by 3.9 m in length. There were 208 fuel rods in each fuel assembly, and 177 fuel assemblies in the core, which contained three enrichment levels of 235U: 1.98%, 2.64%, and 2.96% by weight. Fuel assemblies were protected with cladding covers from coolant corrosion. Block Diagram of a Pressurized Water Reactor Relief valve Reactor & Pressurized containment primary building cooling loop Heat exchange and steam generator Cooling tower & housing Turbine & generator Reactor core Pumps Auxiliary pumps & valves Secondary cooling loop The reactor generated 2772 megawatts of heat, and the primary coolant was pressurized (15.1 megapascals or about 150 atm) water at 565 K, and heated up to 593 K at the outlet. A heat exchanger and steam generator converted water in the secondary cooling loop to steam, which rotated the turbine of the generator. At almost exactly 4:00 am, March 28, 1979, a pump which supply the feed water to the steam generator (secondary cooling loop) failed due to the trip of another pump, which was connected to the same water supply system in series. 262 When the pump failed, operators tried to start the auxiliary pumps of the secondary cooling loop to remove the heat from the primary coolant so that the reactor could be shut down to a standby conditions. The valves of the auxiliary pumps had been closed for an earlier test operation, but the valves were never turned back on. Since no feed water reached the steam generator to remove heat from the primary coolant, the volume of the primary coolant increased due to heating. The increased pressure of the system led to the opening of the relief valves. All these happened within 9 seconds. The relief valves did not close after the pressure fell to normal operating conditions, resulting in loss of coolant. Part of the core was uncovered by water, and energy released from decays of fission products heats up the core causing it to melt. The core damage was the worst of any commercial power reactors till that time. At high temperature, the Zircaloy-4 was oxidized by water, producing a large volume of hydrogen gas that eventually ignited. Extensive damage was made to the core, the containment building, and the auxiliary building. No one was killed or injured, and the leak of radioactive material was limited. However, the damage became the wellknown nuclear TMI-2 reactor accident. The psychological pressure experienced by residents near the reactors during and after the accidents was immeasurable. Long-life Fission Products in the Core after the Accident at Three Mile Island. Isotope Activity /Ci Half-life Amount* 85 9.7104 10.7 y 4.71013 90 7.5105 28.8 y 9.81014 K Sr The decay energy of fission products 129 I 2.210–3 1.6107 y 1.61012 caused a melt down. The release of 131 radioactive fission products was a major I 8.04 d 7.0107 7.01013 concern. From the fission yields, we have 133 Xe 5.25 d some idea of their quantities. Some the 1.5108 9.81013 long-life fission products that remained in 137 Cs 30.2 y 8.4105 1.11015 core are tabulated by Voilleque (1980). The * Amount = Activity x half-life (s)/0.693, activity giving was called core-intensity, but a number related to the number of nuclei, but the details of measurements were not due to uncertainty in the definition of Activity, available. Thus, the total activity could not Ithese value do not reflect the "real" amount. be estimated. However, the activity enables us to calculate the relative amount present. Multiplying the activity by its half life gives a quantity which reflects the quantity of a nuclide. The amounts for the nuclides in the table indicate higher quantities for 90Sr and 137Cs. These are fragments of high yields, in agreement with the fission yield curve. The Chernobyl Accident: The former USSR's nuclear power generation was derived from reactor technology they have used to produce 239Pu. In the early 1970s, a team of scientists and engineers embarked upon an ambitious power generation program. They coined the acronym RBMK for the graphite-moderated, channel-tube-cooled reactors. Two pairs of 1,000 Mw RBMK were commissioned at Leningrad in 1974, and later in Kurst and Chernobyl (1,500 Mw). Reactor 4 in Chernobyl had been in operation for three years prior to the accident, and it had been running at 83% capacity in 1985. 263 Electric power is required to operate various controls for the shut down of a nuclear reactor. Most power reactors have battery reserves in case of power failure. On April 26, 1986, Reactor 4 at Chernobyl was scheduled for a safety test in case of a sudden power failure. Ironically, the safety test led to a catastrophic accident. During a power failure, the pump would stop to send steam to drive the turbine of a generator. The engineers wanted to find out if the power generated by the residual momentum of the generator and turbine would be able to safely shut down the reactor. Since the electrical system was tested, they ignored possible problems with the reactor. They paid little attention to the safety of the reactor. The test team shut down the emergency core cooling system (ECCS) before they started the test. From 1.00 to 13:00 hr on April 26, the reactor power was gradually reduced to 50% as planned and it was held at that level till 23:00 hr, at which time they further reduced the power. When the power from the generator driven by the reactor become too low, the power from the reactor can no longer safely operate the controls. The operators switched the controls to power supplied by the grid (the nation wide network of regulated electric power). They forgot, however, to send a signal to hold the power of the grid. Because the controls used so much energy, the grid power was reduced to a low level resulting in unsafe operating condition. Several undesirable conditions such as requiring excessive pumping for the steam remover, over heating in the core area, and difficulty in reactor control were observed at this stage. When reactor power fell to 30 Mw, they had to manually withdraw some of the control rods to bring it back to 200 megawatt. Between 23:30 to 1:20 hr, a series of operational and control difficulties were encountered due to inadequate cooling. The operators should have shut the reactor down at this time, but they increased power hoping to correct the problems. The reactor power became unstable, rose rapidly at 1:23:40 hr, at which time the shift foreman ordered the shutdown of the reactor, but it was too late. There was insufficient capacity left in the control rods which were in core, and the others at the top of the core could not be inserted fast enough to overcome the power increase caused by other factors. Power surged to 100 times the designed capacity generating excessive steam, fragmented the reactor core, and eventually the catastrophic destruction of the reactor building (Young, 1987). The accident caused extensive damage. About 30% of the reactor core melted at temperatures of 4000 to 5000 K. A quarter of the graphite block blew away from the core. Some 10% of the graphite were burned in a fire; and the 1000-ton roof of the building housing the reactor blew off, damaging all the pipes and electric connections. The chain fission reaction halted only when the reactor disintegrated. After the explosion, emergency crews dropped sand, boron and lead compounds to cover the core material to extinguish the graphite fire and to contain the fission products from releasing. The reactor core disintegrated and the buildings were destroyed. More than 7 million Ci of radioactivity were released into the atmosphere. Thus, the Chernobyl accident affected a much wider area than the TMI-2 accident. Due to the hot core and the graphite fire, nearly all the 264 inert gases in the fission products such as 133Xe, 85Kr, and 85mKr escape into the atmosphere on the first day. Much of the volatile fission products 131I, 132Te, 134Cs, and 137Cs had also escaped. Radioactive iodine (131I) strontium (90Sr, 89Sr), etc., escaped on the first day into the atmosphere came down with the rain in Scandinavia and other northern European countries (Clough, 1987). Despite the containment effort, heat from radioactive decay (~15 Mw) caused the core material to heat up a few days later, releasing more radioactive nuclides on the 7th, 8th and 9th days. At that time, they pumped liquid nitrogen to cool the core material, and the fission products release stopped on day 10. Different compositions of radioactive nuclides were released in nine (9) days, and wind and rain carried them to various parts in Europe. Detailed study of the compositions of radioactive nuclides in the atmosphere atop the damaged reactor, and those that came down with the rain agreed with the idea that the wind was responsible for the further distribution. The health and social implications of reactor accidents will be discussed later after we have considered the interactions of radiation with matter and the safety issues of ionized radiation. Learning From Accidents: Nuclear reactor accidents influence not only the nuclear industry but also everyone's life. Prior to these accidents, nuclear energy was considered one of the safest and most economical, resulting in the construction of many nuclear power plants for industrial applications and for raising living standards. Accidents have brought the issues related to nuclear energy into the political arena. The public now wants to decide the future of nuclear energy, so the hands of experts are no longer free. Information on nuclear technology must be known to and understood by every educated citizen, and nuclear technology experts must also bear social and environmental responsibilities. Over-simplified descriptions have been given above for the reactor accidents. A full disclosure of the details would require many volumes of documents to sort out all the lessons we and the experts need to learn. In short, both design deficiencies and operational faults led to these accidents. In both accidents, energy released by fission products contributed to the accidents. It is easy to say that human errors are involved, but giving the same circumstance of operation and mental state of the operators, another choice might not be possible. From the description, one can get some idea about errors made during the course of the accidents, but there are other reasons. Experts should be and are inspecting every piece of the records and they are studying the damaged reactors for clues to improve future design and operation procedures. There is much to learn from accidents. Future of Fission Reactors:* Fission reactors have been used for research, power generation, and breeding fissionable nuclides. Just after World War II, nuclear energy was considered reliable, clean, economical, and plentiful. Thus, much development had been made for power generators. As a result, all types of power reactors mentioned earlier had been developed and are commercially available. Nearly 300,000 to 380,000 Mw were generated in 1960, and nuclear * For more information of civil nuclear industry, visit the web site of Uranium Institute: www.uilondon.org 265 power plant was in great demand in 1967 and 1968. Japan ordered three light water reactors (LWR), and began operation in 1970. According to the report by Nagashima & Izumi (1968), Japan would have reached 40,000 Mw by 1985, and 150,000 Mw by 2000, with a breeder reactor planned for 1985. Many reactors had been ordered by developing countries, and the energy definitely raises living standards of people in them. In the 1970s, the public became aware of the danger of radiation, and problems with radioactive waste compounded the predicament. Furthermore, the TMI-2 and the Chernobyl Accidents had given a negative image to nuclear power generation, and they had slowed down the development. Companies who invested heavily on nuclear power generation had not anticipated these developments. Indeed, many difficulties are present in decommissioning (orderly dismantling) a nuclear power plant. All factors such as construction, maintenance, fuel, decommission, safety, solving social and environmental problems, and waste management, have to be considered in the calculation of cost for nuclear energy. The future of nuclear power generation very much depends on the costs of coal, gas and fossil fuel. Economic conditions, energy demands and public perception will play important roles about the future of nuclear energy. However, burning fossil fuel increases CO2, a green house gas. Much scientific research is required to balance human demands of energy and their longterm survivor. Skill Building Questions 1. Briefly describe the events resulting in the meltdown of the Three Miles Island reactor No. 2? What changes in operation procedures will you suggest in view of the accidents? 2. Describe the Chernobyl's nuclear reactor accident. 3. Why are we more concerned with the radioactivity of the fission products, but not that of 235U and 238U in nuclear reactor accidents? Natural Fission Reactors In 1972, a French chemist H. Bouziques analyzed the 235U abundance of uranium samples. He found some contained 0.7171% 235U, which was low compared to normal values of 0.71950.7204%. He noticed that these low 235U samples came from Oklo, Gabon in West Africa. Some samples from that area has 0.440% 235U, and this led to further exploration of Oklo. What are the reasons for the low abundance of 235U in the samples? Can it be due to natural fission reactors? Could natural nuclear reactors exist? How did they start and end? What evidences support the natural fission reactor site long ago? 266 One possible explanation of the low abundance is that 235U was depleted due to natural fission long ago. The depletion of 235U may be due to natural fission reactors. When a large quantity of uranium ore is concentrated in one location, a critical size can be reached. When moderated by water, natural fission reactors are possible. However, additional supporting evidences are required. Had there been a natural reactor, the fission products must be present. Much of the fission products are rareearth elements, and the French group studied isotope distributions of rare earth elements in Oklo. In general, isotope distributions of natural elements and elements from fission products are different. For example, the isotope distribution of neodymium (Nd) is given here. Apparently, the isotope distribution of Nd from Oklo resembles that of fission products. Isotope distributions of other elements in Oklo ore showed further evidence for a natural reactor, and they estimated the existence of a natural reactor 1.8 billion years ago, which was dated by various radiometric dating methods (Kuroda, 1982). Isotope distribution of neodymium mass Natural Fission Oklo* 142 143 144 145 156 148 150 27.11 12.17 23.85 8.30 17.22 5.73 5.62 0 28.8 26.5 18.9 14.4 8.26 3.12 0 25.7 29.3 18.4 14.9 8.2 3.5 * Values after correction for decay and other factors. II In fact, in Oklo, several natural fission reactor sites had been identified, one of which had a 110 m area containing 235U depleted uranium ore. The ore contains the rare earth elements: lanthanum, cerium, praseodymium, neodymium, europium, samarium, and gadolinium. Uranium ore from other areas lack these elements. Furthermore, other fission products such as yttrium, zirconium, ruthenium, rhodium, palladium, niobium, and silver were found in uranium ore of suspect natural reactor areas. There were iodine, krypton and xenon due to fission in the natural reactor area as well. Fission products which were water soluble such as rubidium, cesium, strontium, barium, and cadmium were not found, but zirconium, 90Zr, resulting from decay of strontium, 90Sr, was found. These findings supported their conclusions, and there had been many international studies on the Oklo phenomenon. About 1.8 billion years ago, the 235U abundance would have been about 3%, like some slightly enriched uranium today. It had been hypothesized that organisms in water increased oxygen levels that oxidized the uranium making it soluble. The flow of water and die off of the organisms concentrated uranium in certain areas, developing favorable conditions for natural fission reactions. Water is a natural moderator, and the reactors were left to natural control. For example, when the core temperature was too high, water would have boiled away. Reduced moderation slowed fission rate. The presence of some fission products such as xenon might have added to the slow down. When 235U was depleted, the chain reaction could no longer be sustained, and the natural reactor died off (Cowan, 1976, Maurette, 1976). 267 Fast neutrons should have been present in 239 Pu natural nuclear reactors, and they caused nuclide mutations aside from fission. 239 Np Reactions such as 235 235 236 238 239 U (n, ) 236U ( , ) 232Th, U U U U and 238 U (n, ) 239Np ( , ) 239Np ( , ) 239Pu should have taken place. The 232 Th (n, ) transmutation of nuclides is shown here. Note that 239Pu contributed to the fission as well. The estimated neutron flux Transmutation of nuclides in natural fission process intensity was 1.5x1021 n/cm2. The French director of the Oklo study group, R. Naudet estimated an energy release of 15,000 Mw-years in the reactor zones, and 6 tons of 235 U consumed. The reactor life spanned for about 150,000 years. Sites of natural fission reactors can provide valuable information such as the pattern of distribution and migration of fission products. Data on the stability of geological structure might also contribute to our needs in view of radioactive waste disposal (AECL, 1992). After the discovery of a natural reactor, many hot spring sites were studied. The Cluff Lake deposit in Saskatchewan, Canada, had similar conditions as those in Oklo (Libby, 1979). However, there was no firm evidence pointing to a natural reactor in Cluff Lake. Skill Building Questions 1. If the abundance of 235U is 0.72% today, what was its abundance 1.8 billion years ago? 2. What are the evidences for the existence of natural nuclear reactors in Oklo area? 3. How much energy had been released if 6 tons of 235 U were consumed? Exercises 1. Who discovered nuclear fission? What was the social background and international condition at the time? What was the implication of the discovery? 2. How was the element neptunium produced? Which isotope of neptunium has the longest half-life? How was the element plutonium produced? 3. What particles should be used to bombard uranium to make transuranium elements? Write the reaction equation and describe the cross section as a function of the energy of the incident particle. 268 4. Assume the thermal-neutron-induced fission of 235U (mass = 235.0439) gives two fragments of mass 140 and 93 (plus 3 neutrons). A check on the properties of nuclides indicates that 140Ce (mass = 139.90539) and 93Nb (mass = 92.90638) are stable isotopes. Estimate the total energy (including energies of beta-decay of the fission products) available in this fission process. (Ans. 200 MeV). 5. In a fission reaction, the isotope 235U after capturing a neutron, splits into two fragments plus on the average 2.5 neutrons. Assume the reaction produced two fragments, one identified as 137Te (Z = 52), and two neutrons. What are the atomic and mass numbers of the other fragment? What is the decay scheme for 137Te that would lead to a stable isotope 137 Ba (Z = 56)? Make up a simplified chart of nuclides to show the decay relationship. 6. In a nuclear fission reaction of 235U, three neutrons and a 147La nucleus are identified. What is the third product X in this reaction? Hint: use the Periodic Table of Elements and check the mass number from a handbook listing all nuclides. 7. Describe the four methods used for separating 235U from natural uranium. Can these methods be used for separating isotopes of other elements? How was the isotope deuterium separated from natural hydrogen? 8. Assume the abundance of 235U to be 5.0% when the earth was created. Calculate the age of the earth from the distribution of 235U and 238U (now 0.72 % and 99.28). Note that the assumption may not be valid. 9. Assume the percentage to be 0.72 % today. Calculate the percentage of 235U 1.8×109 years ago. The half lives are: 235U, 7.038×108 y, 238U, 4.468×109 y. (Ans. 3.1%, see Natural Fission Reactor in Text). 10. Assume that the average of all fission reactions is represented by the reaction. 235 U + n 136Te + 97Zr + 3 n. And a check for stable isotopes with mass numbers 136 and 97 indicates that 136Ba56, 97 Mo42 are stable. The atomic masses are: 235U = 235.0439, 136Ba = 135.9044, 97Mo = 96.9058. Other required constants can be found elsewhere in the lecture notes. (a) Calculate the energy released in the fission process, including energy from radioactive decay of the fission products. (Ans. 201 MeV or 3.36 x 10-11 J per fission) (b) A nuclear power plant is required to generate 100 megawatts, (108 J per second). Calculate the 235U consumption in grams per second. (Ans. 1.2 microgram) (c) If the efficiency of energy conversion is 60 percent, what is the consumption rate of 235 U? 11. What is the cross section of a nuclear reaction? Why are cross section data of various nuclides required for the design and construction of atomic bombs and nuclear reactors? 12. What are moderators? What properties make some compounds good moderators? Why are heavy water and graphite good moderators for nuclear reactors using natural uranium as fuel, but normal distilled water not a suitable moderator? 269 13. From the atomic mass of He, 235U and 207Pb on the chart of the nuclides or Table of Isotopes, calculate the total energy released for the (4n + 3) series of the four families of radioactive series. Further reading and work cited Brown, A.C. and MacDonald, C.B. (Editors) (1977), The secret history of the atomic bomb, Dial Press/James Wade. Clough, P.N. (1987), The Chernobyl accident -- source terms and related characteristics, in The Three Mile Island accident - diagnosis and prognosis, ACS Symposium Series 293, Edited by Toth etc., American Chem. Sociity Publication Cowan, G.A. (1976), A natural fission reactor, Sci. Am. 235 (1), 36 (July) Maurette, M, (1976), Fossil nuclear reactors, Ann. Rev. Nucl. Sci. 26, 319 Fermi, L., (1954), Atoms in the family, University of Chicago Press. Libby, L.M. (1979), The uranium people, Crane Russak & Co., Charles Scribner's Sons, New York Martin, D., (1980), Three mile island: prologue or epilogue?, Ballinger Publishing Co. Shea, W.R. (1983) Otto Hahn and the rise of nuclear physics. Several essays edited by Reidel, 1983. (QC773.078) Thomas, G.K. (1980), Description of the accident in The Three Mile Island accident - diagnosis and prognosis, ACS Symposium Series 293, Edited by Toth etc., American Chem. Sociity Publication Rhodes, R. (1986), The making of the atomic bomb, Simon and Schuster. US (1977), Official history of the Manhattan project, Government Publication. Voillequé, P.G. (1980) Fission product behavior, in The Three Mile Island accident - diagnosis and prognosis, ACS Symposium Series 293, Editors: Toth, L.M. etc. American Chem. Society Publication Young, J.D. (1987), Chernobyl -- the accident sequence in Chernobyl, a technical appraisal, Proceedings, British Nuclear Energy, London, October 3. pp. 27 - 42 (TK1362.S65.C479) Hahn, O. (1966), Otto Hahn: a scientific autobiography. Translated by W. Ley, Charles Scribner's Sons (QD22H2A313) Groueff, S., (1967), Manhattan project, the untold story of the making of the atomic bomb, Little, Brown & Company (QD22H2A313) Izumi, K. and Izumi, T. (1968), Uranium requirement, long-term nuclear power generation program in Japan, Symposium on the economics of nuclear fuels held by Internation Atomic Energy Agency, Viena, 1968 Masche, G., (1971), Systems summary of a Westinghouse pressurized water reactor nuclear power plant, Nagashima, Westinghouse Electric Corp Wilson, D., (1983), Rutherford, simple genius. Hodder and Stoughton (QC16R8W5x) 270