The Processes of Three Natural Decay Series in Underground Strata and Their Common Characteristics Wei Zhang Associate researcher, IoT Perception Mine Research Center, China University of Mining & Technology, Xuzhou, Jiangsu, 221008, China; The National and Local Joint Engineering Laboratory of Internet Technology on Mine, China University of Mining & Technology, Xuzhou, Jiangsu 221008, China; School of Environment Science and Spatial Informatics, China University of Mining & Technology, Xuzhou, Jiangsu, 221116, China Corresponding author, e-mail: zhangwei@cumt.edu.cn Dongsheng Zhang Professor, School of Mines, China University of Mining & Technology, Xuzhou, Jiangsu 221116, China e-mail:dshzhang123@126.com Lixin Wu Professor, IoT Perception Mine Research Center, China University of Mining & Technology, Xuzhou, Jiangsu, 221008, China; The National and Local Joint Engineering Laboratory of Internet Technology on Mine, China University of Mining & Technology, Xuzhou, Jiangsu 221008, China; School of Environment Science and Spatial Informatics, China University of Mining & Technology, Xuzhou, Jiangsu, 221116, China e-mail: awulixin@263.net Xufeng Wang Professor, School of Mines, China University of Mining & Technology, Xuzhou, Jiangsu 221116, China e-mail: wangxufeng@cumt.edu.cn ABSTRACT In order to apply the radon technique to the detection of mining-induced fractures in overlying strata with greater confidence, some fundamental knowledge of high energy physics must be understood. In this paper, based on composition of substance (including atom and nucleus), the types and basic rules for radioactive decay of a nuclide had been summarized. Moreover, the processes of three natural decay series in underground strata and its common characteristics had been analyzed. The analysis results indicate that all of their initial nuclides have relatively long lifetimes, all of their final products are stable isotopes of plumbum after undergoing a series of radioactive decays, all of their mass numbers follow a trend and all of these decay processes produce radioactive gases. KEYWORDS: coal mining; radon detection; mining-induced fractures; radioactive decay; natural decay series - 709 - Vol. 21 [2016], Bund. 02 710 INTRODUCTION Radon is a chemical element with a chemical symbol Rn, it is a direct decay product of radium. In nature, radon has three kinds of common radioactive isotopes. The three natural isotopes of radon are 219 Rn, 220Rn and 222Rn, with half-lives of 3.96 s, 55.6 s and 3.82 d, respectively. Due to the extremely low concentration of 219Rn in the crust [1] and its short half-life, this isotope is usually undetectable. Similarly, only a small amount of 220Rn is released from the crust, and it decays quickly due to its short half-life. Indeed, the concentration of 220Rn in the crust is only 10% that of 222Rn, and the overall quantity of natural 222Rn is significantly larger than that of natural 219Rn and 220Rn. Additionally, the half-life of 222Rn is much longer than that of the other two isotopes. In general, radon refers to 222Rn. It has a half-life of 3.82 days. Direct parent of 222Rn is radium isotope (226Ra), and the indirect parent is uranium isotope (238U). The elemental form of radon element is usually gaseous, which is the only radioactive heaviest inert gas in contact with human. In normal state, it is colorless and tasteless and odorless, soluble in water and organic matter. The chemical properties of radon are relatively stable, and it is difficult to produce chemical reaction with other substances [2]. As radon is eventually from uranium decay, while uranium exists in coal, rock, soil and water with certain content in nature, therefore, radon is ubiquitous in natural environment. The activity of radon is very strong, and it has good migration ability in natural conditions. In geological environment, radon can migrate by gaseous or dissolved form with ground and soil water. Radon usually migrates by diffusion and convection effect in overlying strata, and the migration distance from underground strata to surface depends on different lithological characters. For example, the vertical migration distance in homogeneous sand is 360-420 m [3-5]. Moreover, the phenomenon of increased radon concentration in surface oil above spontaneous coal combustion area at 400 m depth had been observed in China [6]. These show that radon can migration to surface from underground coal strata of 400-500 m depth. Because radon has radioactivity, even if its concentration is very low, it also can be measured. Meanwhile, radon has the geophysical-chemical properties of inert gas, thus it can migrate and accumulate in micropores or microfractures. Radon formed by radioactive decay in underground coal strata can penetrate surface into air, which provides a basis for detecting radon on surface. For instance, German scholars found that abnormal radon concentration in surface soil above the mininginduced area of deep shaft mining [7]. In this literature, the specific mining depth did not been explained, but we also could deduce that vertical migration distance is more than 400 m at least. At present, attempting to apply the geophysical-chemical properties of radon in the field of mining engineering, importing the radioactive measurement methods to detect the dynamic development process of mining-induced fractures and its aquosity in overlying strata of underground coal mining, which is still in preliminary stage [8-14]. In order to apply the radon technique to the detection of mining-induced fractures in overlying strata with greater confidence, some fundamental knowledge of high energy physics must be understood. In this paper, based on composition of substance (including atom and nucleus), the types and basic rules for radioactive decay of a nuclide had been summarized. Moreover, the processes of three natural decay series in underground strata and its common characteristics had been analyzed. Vol. 21 [2016], Bund. 02 711 COMPOSITION OF SUBSTANCE Atom Elements in nature are composed of atoms. Atoms have different masses and sizes whose radii are in the range of 10-10~10-12 m. Generally, each atom is composed of a nucleus and electrons orbiting around the nucleus, so it has no net electric charge. Nucleus A nucleus consists of nucleons, in which neutrons and protons are the fundamental building blocks of nucleon. These nucleons move along different orbits inside the nucleus. Nucleus has a positive charge because neutrons are neutral while proton has a positive charge. The amount of charges possessed by the nucleus is equivalent to the charges of electrons orbiting around the nucleus. Generally, e (e=1.6021×10-19 C) represents the number of charges of a single electron. The mass of a single electron is 9.1091×10-25 kg. The mass of a single proton is 1.6725×10-21 kg, which is 1836 times heavier than an electron. The mass of a single neutron is 1.6748×10-21 kg, which is slightly heavier than a proton. Generally, an atom bears no net charge because the number of surrounding electrons equals to the number of proton in the nucleus. The mass of an atom is concentrated on nucleus and hence, its mass is the sum of proton (Z) and neutron (N) in nucleus and is termed mass number (A = Z + N). The radius of a nucleus R is 1.5x10-13 A1/3, indicating that the volume of a nucleus is also proportional to A. For an element (X), all protons (Z) and neutrons (N) located inside a nucleus are generalized as nucleon. Atomic number (Z) represents the number of proton inside a nucleus and hence, the total charge of a nucleus is Ze. Nucleuses with same atomic number (Z) are surrounded by the same number of electrons and those elements show similar chemical properties. In other words, same element must have the same number of proton but could have different number of neutron (N). Thus, their mass numbers (A = Z + N) could be different. Atoms or nucleuses containing a certain number of protons and neutrons are called nuclides, which notation can be expressed as AZ X . Nuclides with same number of protons but different number of neutron are called isotopes. For example, isotopes of 238 uranium are 235 92 U and 92 U . RADIOACTIVE DECAY Energy level of nucleus The nuclear stability is tied with the neutron-to-proton ratios inside the nucleus, in which excess number of proton or neutron causes nuclear instability. Modern high energy physics indicates that a particle system can only take on certain discrete and discontinuous values of energy state. Each discrete energy state represents different energies and the amount of energy possessed by the atoms at certain state can be described as energy level. Generally, ground state is the lowest possible energy level and all the nuclides in this state are stable. Any energy state that is higher than ground state is called excited state. Nucleuses in an excited state are unstable and tend to return back to ground state by dissipating excess energy using different ways. As illustrated in Figure 1, the excited states of a Vol. 21 [2016], Bund. 02 712 nucleus can be categorized according to their energy levels, such as first excited state, second excited state, third excited state, etc. … … … The fourth excitation level The third excitation level Excitation state The second excitation level The first excitation level Ground state Figure 1: Excitation level of atomic nucleus Radioactive decay Some elements are unstable in nature because their nuclei are in an excited state. These nuclei tend to undergo structural change and transform into another kind of nuclei. At the same time, the nuclei dissipate excess energy by emitting radiations (α-ray, β-ray, γ-ray). This phenomenon is termed radioactive decay or nuclear decay. Elements that undergo nuclear decay are called radioactive nuclides (isotopes). Generally, nuclei with proton number Z > 82 are categorized as radioactive nuclides because they are unstable in nature. In general, there are three common types of radiation decays: 1. α-decay α-decay is a type of radioactive decay in which a nucleus ejects an α-particle spontaneously and thereby transforms into another kind of nucleus. The α-particle that consists of 2 protons and 2 neutrons is identical to a high-velocity helium nucleus, 42 He . It is a positively charged particle with kinetics energy of about 4~9 MeV. The mass number, A, of a parent nuclide is reduced by 4 and its atomic number, Z (nuclear charge), is reduced by 2 after α-decay. Therefore, a new element that is 2 places to the left in the periodic table than the original element is formed. The generic equation of a α-decay can be represented as follows: A Z X → Y + 42 He A -4 Z-2 (1) In this equation, X, Y, A, and Z represent the parent nucleus, the daughter nucleus, the mass number of the parent nucleus (atomic weight), and the atomic number of the parent nucleus (proton number). Vol. 21 [2016], Bund. 02 713 2. β-decay β-decay is a type of radioactive decay in which a nucleus ejects a β-particle (electron) spontaneously or captures an electron and thereby transforms into another kind of nucleus. There are three types of β-decays which are known as β‾-decay, β+-decay, and electron capture. β‾-decay is a process that a neutron in the parent nuclide converts into a proton and simultaneously induces the emission of an electron (β‾) and electron antineutrino ( v ). β‾ particle is a high-velocity electron that has identical mass with a stationary electron and bears a negative charge. The mass of a β‾ particle is far lighter than a nucleus, thus, the mass number of a parent nuclide is identical its daughter nuclide. A new element that is 1 place to the right in the periodic table than the original element is formed. The generic equation of a β‾-decay can be represented as follows: A Z X → ZA+1Y + β − + v (2) In this equation, electron antineutrino ( v ) is neutral with a mass of 1/2000 of an electron. β+-decay is a process that a proton in the parent nucleus converts into a neutron and simultaneously induces the emission of an electron (β+) and electron antineutrino ( v ). β+ particle is a high-velocity electron that have identical mass with a stationary electron but bears a positive charge. Thus, the mass number of the parent nuclide is identical with the daughter nuclide. A new element that is 1 place to the left in the periodic table than the original element is formed. The generic equation of a β+-decay can be represented as follows: A Z X → ZA−1Y + β + + v (3) The capture of orbital electron is a decay process in which a parent nuclide absorbs an atomic electron from outer shell. This process converts a proton to a neutron and simultaneously induces the emission of an electron neutrino. Thus, the mass number of the parent nuclide is identical with the daughter nuclide. A new element that is one place to the left in the periodic table than the original element is formed. The generic equation of an electron capture process can be represented as follows: A Z X + β − → ZA−1Y + v (4) 3. γ-decay γ-decay is a radioactive decay in which an unstable daughter nuclide that has been through an α/β-decay changes from a higher energy state to a lower energy state through the emission of γ-photons. Thus, the mass number (A) and atomic number (Z) remain unchanged after γ-decay. The basic rules for radioactive decay of a nuclide Everything in nature follows some basic rules. If a radioactive nuclide is collected, we will find that its amount may reduce gradually owing to radioactive decay. A radioactive nuclide changes into another kind of nuclide during a radioactive decay process. Although radioactive decay is a random process, it still follows some statistical behaviors and mathematical exponential formula. Four different physical quantities can be used to describe the basic rules for radioactive decay of a nuclide, including decay constant, half-life, mean lifetime, and radiation activity. Vol. 21 [2016], Bund. 02 714 1. Decay constant (λ) The decay rate of a radioactive nuclide can be represented as dN/dt in which dN is the number of nucleus that decays within time t to t + dt [15-16]. Experimental study showed that dN is proportional to the number of undecayed nucleus within time interval dt, which can be expressed as follows: dN = −λN dt (5) In this equation, λ represents the decay constant of a radioactive nuclide and “-” sign shows that the decay rate is decreasing. The basic rule of radioactive decay can be derived from integrating equation (5) by which t = 0 and the initial amount of nucleus is N0. It can be expressed as follows: N = N 0 e − λt (6) In this equation, N represents the number of nuclei of radioactive nuclide at a given time t, N0 represents the number of initial nuclei of radioactive nuclide at t = 0, and λ represents the decay constant of a radioactive nuclide. From equation (5) and (6), decay constant is the probability at which the nuclei decreases because of radioactive decay per unit time and thus, its unit is s-1. 2. Half-life (TB) Half-life, TB, is the time required to for the number of nuclei to fall to half of its initial amount. When half-life is defined as N = N0/2, equation (6) can be written as follows: TB = λn 2 ≈ λ 0.693 (7) λ From equation (7), the number of nuclides remains after 10 half-lives is calculated to be N = N 0e −10 lTB = N0 N = 0 . At this stage, the radioactive nuclide has been decayed completely. 10 ln2 e 1024 3. Mean lifetime (τ) The decay time of nuclides differs from each other because the radioactive decay is a random process. Thus, they have different lifetimes. Lifetime is defined as the time of existence of radioactive nuclide and mean lifetimes is referred to the average time of existence of the majority unstable nuclides. Therefore, τ can be calculated based on the following equation: t= 1 N0 ∫ ∞ 0 ∞ 1 0 λ λNtdt = ∫ te −λt dt = 4. Radiation activity (radiation intensity) ≈ 1.44TB (8) Vol. 21 [2016], Bund. 02 715 Units λ, TB, and τ are used to express the decay rate of a radioactive nuclide but they are not related to the number of nucleus. In practical application, both the decay rate and the radiation intensity or so-called radiation activity are essential. Radiation activity (radiation intensity) is the amount of nucleus that decay or the number of emitted radiation per unit time [17-20], which is generally expressed in Nλ. Therefore, radiation activity is associated with both decay constant (λ) and the number of nucleus (N) in an atomic nuclide. Previously, radiation activity is measured in units of curie (Ci), milicurie (mCi), microcurie (μCi), and picocurie (pCi) (1 Ci = 103 mCi = 106 μCi =10 12 pCi). Nowadays, becquerel (Bq) is the unit of radioactivity in the International System of units (SI), which is defined as one radioactive decay per second. Therefore, the SI unit of the concentration of Radon is Bq/m3, which refers to the number of decay per unit volume and time. The conversion between curie and becquerel is 1 Ci= 3.7e10 Bq. Natural decay series Decay series is a group of elements that consists of parent nuclide and its daughter nuclides in the periodic table. Natural decay series is referred to a collection of naturally occurring radioactive nuclides. Three main natural decay series are observed in nature, which are the uranium series (uranium-radium series), thorium series, and the actinium series (actinium-uranium series) [21-23]. Their atomic numbers are in the range of 81~92. Majority of the nuclides in these three series emit γray during α- and β-decays. 1. Uranium series (uranium-radium series) Uranium series includes 15 nuclides. The decay process is illustrated in Figure 2. This series 238 9 begins with 238 92 U which has a relatively long half-life (4.5×10 a). Beginning with the 92 U , it undergoes 8 times of α-decays and 6 times of β-decays before converting into a stable nuclide The decay process can be expressed as follows: 238 92 In uranium series, 238 92 4 0 U → 206 82 Pb +8 2 He + 6 -1 e + (γ ) 226 88 Rn include (9) Ra with a half-live of 1600 a. Then, α-decay to convert into the only gaseous radioactive nuclide nuclide Pb . U undergoes 3 times of α-decays and 2 times of β-decays before converting into a radioactive nuclide 222 86 206 82 daughter nuclides with 222 86 short 226 88 Ra undergoes an Rn in this series. The isotopes of half-live, e.g. 218 84 Po (TB=3.1 214 214 -4 min), 214 82 Pb (TB=26.8 min), 83 Bi (TB=19.7 min), 84 Po (TB=1.64×10 min) and daughter nuclides with long half-live, e.g. 210 82 Pb (TB=22.3 a), 210 83 Bi ( TB=5 d), 210 84 Po ( TB=138.4 d). Vol. 21 [2016], Bund. 02 238 234 U 4.5e9 a 716 Th 24.1 d 234 Pa 1.17 min 6.75 h 234 230 U 2.45e5 a 226 Th 7.7e4 a 222 Ra 1600 a Rn 3.82 d 218 214 Po 3.1 min 214 Nuclide symbol Atomic number A Z TB U: 92 α-decay Pa: 91 Th: 90 β-decay X X: Nuclide A: Mass number Z: Atomic number TB: Half-life Decay mode Bi 19.7 min 214 Ac: 89 Pb 26.8 min 210 Po -4 1.64e s Pb 22.3 a γ photon Ra: 88 210 Rn: 86 Bi 5.0 d Po: 84 Bi: 83 210 Pb: 82 Po 138.4 d 206 Pb Stable state Figure 2: Decay process of uranium series ( 238 92 U ) 2. Thorium series Thorium series includes 12 nuclides. The decay process is illustrated in Figure 3. This series 10 begins with 232 a). Generally, 232 90 Th which has a relatively long half-life (1.4×10 90 Th undergoes 6 times of α-decays and 4 times of β-decays before converting into a stable nuclide decay process can be expressed as follows: 232 90 4 0 Th → 208 82 Pb + 6 2 He + 4 -1 e + (γ ) 208 82 Pb . The (10) The decay process of thorium series is much more simply than uranium series. In addition, the lifetime of isotopes in thorium series is also shorter than those in uranium series. In thorium series, 232 90 Th undergoes 3 times of α-decays and 2 times of β-decays before converting into a radioactive nuclide 224 88 Ra with a half-live of 3.64 a. Then, only gaseous radioactive nuclide shorter than the half-life of 222 86 220 86 224 88 Ra undergoes an α-decay to convert into the Rn in this series. However, it has a half-life of 55.6 s which is Rn (3.82 d) in uranium series. Vol. 21 [2016], Bund. 02 232 228 Th 10 717 Ra 5.75 d 1.4e a 228 Ac 6.13 h 228 Th 1.91 a 224 220 Ra 216 Rn 55.6 s 3.64 a 212 Po 10.6 h 0.15 s 212 Nuclide symbol Atomic number A Z TB Th: 90 Ac: 89 α-decay X: Nuclide A: Mass number Z: Atomic number TB: Half-life Ra: 88 Rn: 86 β-decay Po: 84 γ photon X Decay mode Pb 208 Bi 60.6 min 212 Po -7 3e s Tl 3.05 min 208 Pb Stable state Bi: 83 Pb: 82 Tl: 81 Short process Figure 3: Decay process of thorium series ( 23290Th ) 3. Actinium series (actinium-uranium series) Actinium series includes 13 nuclides. The decay process is illustrated in Figure 4. The decay process in actinium series is much more complicated than that of either uranium or thorium series. In addition, the lifetime of isotopes in actinium series is even shorter than those in thorium series. This 235 8 series begins with 235 92 U which has a half-life of 7.1×10 a. In actinium series, 92 U undergoes several times of α- and β-decays before converting into a stable nuclide series, gaseous radioactive nuclide 219 86 207 82 Pb . Similar to other Rn is also released during the decay process. It has a half-life of 3.96 s, which is much shorter than the half-life of 222 86 Rn (3.82 d) in uranium series. Vol. 21 [2016], Bund. 02 235 231 U 7.1e8 a 718 Th 25.5 a 231 227 Pa 3.25e10 a Ac 21.7 a 227 223 Th 18.8 d Ra 11.44 d 219 Rn 3.96 s Nuclide symbol Atomic number A Z TB U: 92 α-decay Pa: 91 Th: 90 β-decay X X: Nuclide A: Mass number Z: Atomic number TB: Half-life 215 211 Po -3 1.78e s 211 Decay mode 207 Bi 2.14 min 211 Po 0.52 s Ac: 89 Pb 36.1 min Tl 4.79 min 207 Pb Stable state Ra: 88 Rn: 86 Po: 84 Bi: 83 Pb: 82 Tl: 81 Figure 4: Decay process of actinium series ( 227 89 Ac ) CONCLUSION There are some common characteristics in the decay process among these three natural decay series (uranium, thorium, and actinium) as follows: (1) All of their initial nuclides have relatively long lifetimes, which are in the range of 108~1010 a. Therefore, these 3 series can exist for very long in nature. (2) All of their final products are stable isotopes of plumbum after undergoing a series of 208 207 radioactive decays, which are 206 82 Pb (uranium series), 82 Pb (thorium series), and 82 Pb (actinium series). (3) All of their mass numbers (A) follow a trend, in which the mass number of nuclides in uranium series is A=4n+2 (n=51~59), the mass number of nuclides in thorium series is A=4n (n=52~58), and the mass number of nuclides in actinium series is A=4n+3 (n =51~58). (4) All of these decay processes produce radioactive gases (emanation), which are indicated by black circles in Figure 2~4. These emanations are the isotopes of radon with an atomic number of 86, Vol. 21 [2016], Bund. 02 719 220 219 which are 222 86 Rn , 86 Rn , and 86 Rn . All of them are inert gases. They are known as uranium emanation, thorium emanation, and actinium emanation. ACKNOWLEDGEMENT The research is financially supported by the National Basic Research Program of China (No. 2015CB251600), the National Natural Science Foundation of China (No. 51404254), the China Postdoctoral Science Foundation (Nos. 2014M560465 and 2015T80604), the Jiangsu Planned Projects for Postdoctoral Research Funds (No. 1302050B), the Fundamental Research Funds for the Central Universities (No. 2013QNB24) and the Research Fund of Key Laboratory of Safety and High-efficiency Coal Mining, Ministry of Education (JYBSYS2015106). We wish to thank Doctor Wei Zhou from the Chengdu Univerisity of Technology for the assistance of literature collection. Special thanks are given to Doctor Juanjuan Li from the China University of Mining & Technology, for her language assistance. The authors are also grateful to the editor and anonymous reviewers for their helpful comments and constructive recommendation. REFERENCES 1. Baixeras, C., Erlandsson, B., Font, L., and Jonsson, G. 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