AN ABSTRACT OF THESIS OF Diana Djokotoe for the degree of Master of Science in Chemical Engineering presented on January 8, 2004. Title: Burning Emulsified Sulfur to Stabilize Sodium Compounds in a Lime Kiln Abstract approved: Redacted for privacy Willie B. Rochefort Weyerhaeuser's Paper Mill in Albany, Oregon has been experiencing frequent ring formation in the # 3 rotary lime kiln. Rings form when lime mud (CaCO3) or product lime (CaO) particles adheres to the walls of the lime kiln and become resistant to the abrasive action of the sliding motion of product lime particles ( Notidis,1994). Ring formation has resulted in frequent shut downs to remove (blast) the rings and caused a significant loss of productivity and revenue to the company. A careful analysis of the production process in the mill revealed that concentration of sodium was high and that of sulfur low in the lime mud. The high sodium was due to the low sulfur input to the kiln resulting in high sodium to sulfur ratio. The use of natural gas as a fuel source in the kiln partly causes low sulfur levels in the mud. This study examines the effects of burning emulsified sulfur in the # 3 rotary lime kiln to reduce sodium enrichment in the solids, and examine its effect on kiln operation and SO2 emissions from the # 3 rotary lime kiln. A four day trial of burning emulsified sulfur to reduce sodium concentration in the # 3 rotary lime kiln was planned. Tote bins of 70% solution of emulsified sulfur was fed into the # 3 rotary lime kiln. The sulfur feed was controlled to ensure an excess of sulfur by observing the SO2 concentration in the kiln stack and maintaining a concentration above 100 ppm corrected to 10% oxygen. The results show that while burning emulsified sulfur had no significant effect on kiln operation, it resulted in a high reduction of sodium in the dust caught in the electrostatic precipitator and an increase SO2 emission from the stack. The reduction of sodium in the dust was 50%, which is an enrichment factor of 2. Although lime can effectively remove SO2, the removal efficiency decreased from 96.0% to 73.0% when emulsified sulfur was burned in the # 3 rotary lime kiln. The results of this trial are promising, since it demonstrates that burning emulsified sulfur significantly lowers the sodium enrichment in the kiln. The reduced levels of sodium can potentially lead to a reduction in ring formation in the #3 rotary lime kiln in the Albany Paper Mill. © Copyright by Diana Djokotoe January 8, 2004 All Rights Reserved Burning Emulsified Sulfur to Stabilize Sodium Compounds in a Lime Kiln by Diana Djokotoe A THESIS Submitted to Oregon State University in partial fulfillment of the requirement for the degree of Master of Science Presented January 8, 2004 Commencement June 2004 Master of Science thesis of Diana Djokotoe presented on January 8, 2004. Redacted for privacy Major Professor, representing Engineering Redacted for privacy 'ci Head of Department of Chemical Engineering Department Redacted for privacy Dean of th Oi'a&'iate School I understand that my thesis will become part of the permanent collection of Oregon State University libraries. My signature below authorizes release of my thesis to any reader upon request. Redacted for privacy Djokotoe, Author ACKNOWLEDGEMENTS I would like to acknowledge Dr. Skip Rocherfort, my major advisor, for his interest in, and enthusiastic support for this study. I wish to express my sincere gratitude to Dr. Honghi Tran for his immense contribution to the success of this work. I must also thank the staff and people of the Chemical Engineering Department for the support and encouragement I received during the time I spent in the department. To all the members of my committee, I would like to express my highest gratitude for your willingness to help my dream come true. I will also like to thank Kweku Wilson for encouraging and putting up with me throughout the challenging times. From the depths of my heart, I thank my parents and the rest of my family for all the support given me throughout my life. My effort would not have yielded much without the invaluable support from The Parnell' s, Ralph and Wilma Hull. I owe my life to you all. I thank God for giving me the grace to endure all that came my way to this end. This work would not have taken place but for the help and support of the entire staff of the Albany Paper Mill, Oregon, especially Jim Pruett, Chuck Mihalko, Brian Brazil and Eric Hekkala I thank you with all of my heart. TABLE OF CONTENTS Page Chapter 1. Introduction ....................................................................................... 1 1.1 Overview of kraft pulping process ...................................................... 1 1.2 Kraft recovery cycle ........................................................................... 3 1.3 Brief description of recausticizing process .......................................... 4 1.4 Lime kiln ............................................................................................ 5 1.5 Lime kiln ring formation ..................................................................... 7 1.6 Impurities in lime mud ..................................................................... 10 1.6 Role of sodium compounds to ring formation ................................... 12 Chapter 2. Background ..................................................................................... 15 Chapter3. Methodology .................................................................................... 17 Chapter 4. Results and Discussions .................................................................... 23 4.1 Effect of burning sulfur on solid composition ................................... 23 4-1.1 Sodium .............................................................................. 23 4-1.2Sulfur ................................................................................ 24 4-1.3 Phosphorous ...................................................................... 25 4-1.4 Silicon ............................................................................... 26 4-1.5 Aluminum ......................................................................... 27 TABLE OF CONTENTS (Continued) 4-1.6 Magnesium ........................................................................ 28 4-1.7 Carbon dioxide .................................................................. 29 4-1.8 Residual Carbonate ............................................................ 30 4.2. Effect of burning sulfur on gaseous emissions ................................. 31 Chapter 5. Conclusions ...................................................................................... 33 Chapter 6 Recommendations .............................................................................. 34 References ......................................................................................................... 35 Appendix ........................................................................................................... 36 LIST OF FIGURES Figure Pge 1.1 B lock diagram of kraft pulping process ........................................ 2 1.2 Kraft chemical recovery cycle ...................................................... 3 1.3 #3 Rotary lime kiln at Albany Paper Mill ...................................... 6 1.4 Ring formation in a lime kiln ........................................................ 7 1.5 Comparison of "major" impurities in lime mud ........................... 11 1.6 Sodium enrichment in a lime kiln ............................................... 13 2.1 Histogram showing kiln shut down due to ring blasting .............. 15 3.1 70% emulsified sulfur tote bin and emulsified sulfur input ......... 17 3.2 Diagram of #3 lime kiln showing sampling location ................... 19 3.3 Mud and solids flow data from 7/26/03 to 8/7/03 at Albany PaperMill ................................................................................... 20 3.4 Front and backend temperature profile from 7/26/03 to 8/7/03 at Albany Paper Mill ........................................................ 21 3.5 Gas flow and ID fan speed from 7/26/03 to 8/7/03 at Albany Paper Mill................................................................... 21 3.6 Percent excess oxygen data from 7/26/03 to 8/7/03 atAlbany Paper Mill ................................................................... 22 4.1 Chart showing changes in sodium concentration before, during and after sulfur trial .................................................................... 23 4.2 Chart showing changes in sulfur concentration before, during and after sulfur trial .......................................................................... 24 LIST OF FIGURES (Continued) Figure 4.3 Chart showing changes in phosphorous concentration before, during and after sulfur trial ............................................................. 25 4.4 Chart showing changes in silicon concentration before, during and after sulfur trial ............................................................................... 26 4.5 Chart showing changes in aluminum concentration before, during and after sulfur trial ......................................................................... 27 4.6 Chart showing changes in magnesium concentration before, during and after Sulfur trial ........................................................................ 28 4.7 Chart showing changes in carbon dioxide concentration before, during and after sulfur trial ............................................................. 29 4.8 Chart showing changes in residual carbonate concentration before and after sulfur trial ....................................................................... 30 4.9 SO2 emission and emulsified sulfur input before, during and after trial ................................................................................................. 32 4.10 SO2 emission and mud flow before, during and after trial ............. 32 LIST OF APPENDIX FIGURES Figure Pg A.1.1 Chart showing gas flow vs. kiln shut as blast marker ................. 37 A. 1.2 Chart showing back end or feed temperature vs. kiln shut as blast marker ..................................................................... 38 A.1.3 Chart showing mud density vs. kiln shut as blast marker ......................................................................................... 39 A.1.4 Chart showing percent oxygen vs. kiln shut as blast marker .......................................................................................... 40 A.1.5 Chart showing fan speed vs. kiln shut as blast marker .......................................................................................... 41 A. 1.6 Chart showing front end temperature vs. kiln shut as blastMarker ................................................................................ 42 A. 1.7 Chart showing mud flow vs. kiln shut as blast marker ......................................................................................... 43 A.l.8 Chart showing ambient temperature vs. kiln shut asBlast Marker ............................................................................ 44 A. 1.9 Chart showing turbidity vs. kiln shut as Blast Marker ............................................................................ 45 A.1.10 Lime production rate vs. ring blasting ........................................ 46 LIST OF APPENDIX TABLES Appendix Page A.2. 1 Total material balance for solids before and after trial ................... 47 A.2.2 Process information data for solids during sulfur triall ................. 48 A.2.3 Process information data for solids during sulfur trial (cont.) ...... 49 A.2.4 Process information data for solids during sulfur trial (cont.) ....... 50 A.2.5 Process information data for solids during sulfur trial (cont.) ...... 51 A.2.6 ICP analysis data for solids during sulfur trial .............................. 52 A.2.7 ICP analysis data for solids during sulfur trial (cont.) ................... 53 A.2.8 ICP analysis data for solids during sulfur trial (cont.) ................... 54 A.2.9 ICP analysis data for solids during sulfur trial (cont.) ................... 55 Dedicated in memory of Cephas Kwaku Djokotoe and Ralph Hull My heroes. Burning Emulsified Sulfur to Stabilize Sodium Compounds in a Lime Kiln Chapter 1. Introduction. 1.1. Overview of kraft pulping process The kraft process is a pulp producing method in which wood chips are treated with an aqueous solution of NaOH and Na2SO4 at temperatures above 170°C to remove lignin so that fibers can be separated from one another to make pulp. The kraft chemical recovery process is shown schematically in Figure 1.1 and is described below. A mixture of wood chips and cooking liquor all heated in a large pressure vessel called a digester; the pulp out of the digester contains fiber and black liquor. The black liquor removed is sent to chemical recovery where it is burned to form a molten smelt of sodium sulfide and sodium carbonate (green liquor). During the combustion process, the organic component of the wood contained in the black liquor is burned to generate heat and produce carbon dioxide, which is subsequently absorbed by the alkaline residue to form sodium carbonate. The conversion of sodium carbonate to caustic soda is one of the oldest chemical processes in kraft pulp mill and is carried out in the recausticizing 2 plant. Sodium carbonate in green liquor from the recovery smelt dissolving tank, is reacted with quick lime, Ca(OH)2 to form sodium hydroxide (white liquor) and calcium carbonate (lime mud). The white liquor is separated from the mud and sent to a digester as cooking liquor. The mud is washed and sent to the lime kiln where it is converted into lime, and recycled.(Boniface, 1992) WASH WATER l 11GESTER I BROWNSTOCK WASHERS HIGH DENSITY STORAGE l WOOD CHIPS PULP WEAK BLACK LIQUOR STEAM RECOVERY BOILER EVAPORATORS STRONG BLACK LIQUOR I STEAM SMELT SMELT DISSOLVING TANK MAKEUP LIME I I I i WEAK LIQUOR WHITE LIQUOR GREEN LIQUOR STICIZI PLANT (SLAKER, CAUSTICIZERS) I I LIME LIME MUD FUEL LIME KILN Figure 1.1. Block flow diagram of the kraft pulping process. CAUSTIC up 3 1. 2 Kraft recovery cycle The kraft recovery cycle consists of six main stages: pulping, washing, evaporation, combustion, causticizing and calcining. The main objective of the kraft recovery process is to minimize, as efficiently as possible, the loss and subsequent makeup of chemicals used in the preparation of white liquor. The process is illustrated in Figure 1.2. An in depth look at the calcination of CaCO3 to produce GaO in the lime kiln will be discussed in section 1.3, as it is the central point of this thesis work. Wood ninJCaO NaOH Na2S CaCO3 (7&a,s Causticizing tuoJ I Na,S Combustion Figure 1.2. Kraft recovery cycle. 4 1.3. Brief description of the recausticizing process. The recausticizing process is important to this thesis because the calcium oxide (CaO) produced from the lime kiln is the main raw material used in the recausticizing plant. The recausticizing process produces white liquor from the digestion process from the green liquor of the smelting process. This process consumes lime (CaO) and produces lime mud, principally CaCO3, as a by-product. The lime mud is washed to reduce its chemical content before it is fed into the lime kiln. The weak wash, (filtrate) generated from washing off all the white liquor from the lime mud is recycled to dissolve the smelt generated from the recovery boiler to produce green liquor. Slaking, causticizing, and calcining form a closed ioop process for converting the recovered green liquor into white liquor. (Sanchez, 2001) The major reactions are as follows: Slaking: CaO +1120 - Ca(OH)2 Causticizing: Ca (OH)2 +Na2CO3 Calcining: CaCO3 + heat -* CaCO 2 NaOH -* CaO + CO2 (2-1) (2-2) (2-3) Calcining, the conversion of lime mud to lime in the lime kiln can be performed in either a rotary kiln or a fluidized bed calciner. The rotary kiln is predominantly used due its thermal efficiency. (Boniface, 1992) 5 1.4. Lime kiln. A rotary lime kiln is an important piece of equipment for the recausticing process in a kraft pulp mill. It is a large steel tube lined with refractory bricks. The kiln typically has a length of approximately 250 ft, and a diameter of 10 ft, it is slightly inclined horizontally and slowly rotated on a set of riding rings. It is used to convert lime mud (CaCO3) to product lime (CaO). Lime mud is introduced at the uphill end (backend) and slowly, it makes its way to the discharge end aided by the inclination and rotation of the kiln. Heat is introduced at the downhill side (front end) of the kiln by a burner. Kilns are typically fueled by either natural gas or low sulfur fuel oil. Impurities from these sources cause problems (e.g. ring formation) with kiln operation and white liquor quality. The gases exiting from the kiln must be treated to remove particulate matter before they enter the atmosphere. This is done with either an electrostatic precipitator, or wet scrubber or a combination of both. The precipitator is particularly effective in reducing particulate, but the sulfur dioxide levels may be above environmental standards without the use of a follow-up scrubber. (Boniface,1992) Figure 1.3 is a picture of the #3 rotary lime kiln at the Albany Paper Mill. 6 Figure 1.3. Picture of #3 Rotary lime kiln at Albany Paper Mill. Ring formation in lime kilns is a persistent problem in many kraft mills. It limits kiln production capacity and in severe cases, cause unscheduled shutdowns for clean-up after less than a month of operation. Ringing may also cause severe mechanical damage to the kiln, such as warping, and shell cracking associated with massive mud buildup.(Notidis and Tran, 1993) 7 1.5. Lime kiln ring formation The production of reburned lime from lime mud is accomplished in the lime kiln and can be classified into three stages: drying, heating and calcining. In the drying stage, water evaporates essentially completely from the mud. The dry mud then enters the heating stage where it is heated to the calcining teniperature of about 800°C. Calcining is the process of driving CO2 from the CaCO3 to produce CaO (reburned lime). During the production of lime, rings sometimes form on the refractory surface of the kiln, and gradually decrease the cross-sectional area of the kiln and thereby reducing the passage of lime mud through the kiln. (Tran, 2001) Figure 1.4 shows the formation of rings in a lime kiln. Figure 1.4. Ring firmation in a lime kiln. 8 The location of rings is believed to be a function of the specific mechanism of ring formation. Rings form quickly near the cold-end of the kiln due to high moisture content in the lime mud, while rings near the hot-end of the kiln, are believed to form as a result of the flame impinging directly on the refractory surface. Mid-kiln rings, the most difficult to clean, are very distinct and are believed to form as a result of recarbonation of CaO particles to CaCO3. (Tran, Mao and Baharm, 1992) When a ring of sufficient diameter forms in the rotary lime kiln forms, the kiln must be shut down and the rings literally "blasted" out. This can keep the rotary lime kiln off line for about 24-48 hours. Ring formation occurs when lime mud or product lime adheres to the kiln wall. The ability of the particle to adhere is a function of particle size and the amount of liquid phase that covers the particle surface. In general, small wet particles tend to adhere more rapidly than large dry particles. The stickiness of lime mud is dictated by the presence of a liquid phase that is either water at low temperatures or molten material at high temperatures. Lime mud containing low solids may not be completely dry after passing through the chain section this situation contributes to mud ring formation.(Tran, 2001) From the calcination zone onward, the melting of water-soluble sodium and guarded sodium (bound sodium) compounds in the mud may contribute to increases in the stickiness of the lime mud and/or product lime particles, and lead to the formation of mid-kiln and front-end rings. The different zones of in the lime kin mentioned above can be seen in Figure 1.6 below. 10 1.6. Impurities in lime mud Lime mud consists of about 95 wt% CaCO3, and 5 wt% of impurities, while product lime consists of 82.7 wt% CaO and 17.3 wt% impurities. Ring deposits composition lies between the lime mud and product lime and contains large amounts of CaO and occasionally CaSO4. The composition of the rotary lime kiln ring is a function of the mechanism of formation and it is the topic of this thesis work. In these studies the impurities (elements other than Ca) in all lime mud and ring deposit samples were quantified, they included: Na (sodium), Mg (magnesium), S (sulfur), P (phosphorus), Si (silicon), Al (aluminum), K (potassium), Fe (iron), Cl (chlorine), Mn (manganese, Sr (strontium), Ba (barium), Cr (chromium), Ti (titanium), Y (yttrium), Zr (zirconium), Nb (niobium), and Rb (rubidium). The elements of highest concentrations (>0.1 wt %) were found to be: Na, Mg, S, Al, P, Si, Fe, and K. Figure 1.5 shows the comparison between the concentrations of oxides of the major impurities in the lime mud and ring deposits, expressed as percent of CaO in the individual samples. In the lime mud, Na20, MgO, SO3 and P205, had the highest concentrations (>0.8 wt %), followed by Si02, Al203, Fe203 and K20. For ring deposits similar results were obtained, except that the Na20 content was much lower and the SO3 content was much higher than in the lime mud. This can 11 be due to vaporization of Na compounds and the suiphation of CaO after ring formation. (Tran, 2001) 1.2 1.0 0 CD 0.6 0 0.4 0.2 U 0 o Figure 1.5. Comparison of "major" impurities in lime mud. o o 12 1.7. Role of sodium compounds in ring formation. The sodium enrichment process is illustrated in Figure 1.6. Sodium compounds inside the kiln are likely to be in the form of Na2CO3. The melting point of these sodium compounds when mixed is approximately 820°C. The sodium content in the lime mud is usually less than 1 wt% Sodium may be enriched in the kiln via a vaporization/condensation mechanism. Due to the high temperature at the front-end of the kiln, sodium vaporizes from the product lime, flows with the flue gas, and condenses on the mud particles at the feed-end, where temperature is low. Sodium may also condense on the cooler refractory brick surface beneath a thick layer of ring deposits. (Tran 2001) This suggests that the sodium compounds in the kiln melts, makes the kiln dust sticky and accelerates the rate and size of ring build-ups. (Notidis, 1994) It is therefore important to be able to accurately determine and control the sodium content in the lime. 13 Dust Chains Mid Kiln Burner Na Na Mud Back end Lime Front Temperature end High Na2CO3 ' NaO + CO2 Low High Na2CO3 + H20 2 NaOH + CO2 Low Figure 1.6. Sodium enrichment in a lime kiln. The Weyerhaeuser Albany Paper Mill is one of the few mills that burn natural gas as fuel source for the kiln. Most Mills burn concentrated non condensable gases (CNCG), #6 Diesel fuel and coal. Natural gas contains very low levels of sulfur; as a result, the sodium to sulfur ratio becomes high in the mud. In cases where there are low levels of sulfur in the lime mud, less thermally stable sodium compounds in the form of Na2CO3, causing vaporization in the burning zone. The vapor then recirculates to the feed end of the kiln. Compounds in the vapor then condense, causing sticky buildups that form rings in specific areas of the 14 kiln. In an attempt to stabilize the sodium content in the kiln, emulsified sulfur is burned to react with the sodium to form Na2SO4, which is more thermally stable than Na2CO3 and can be purged from the kiln as a more stable compound. The objectives of this thesis work, examine the effect of burning emulsified sulfur in the kiln to stabilize the sodium enrichment in the solids and evaluate the effect of sulfur addition on kiln chemistry and SO2 emission in the stack gas out of the #3 rotary lime kiln. 15 Chapter 2. Background. The burning of emulsified sulfur (sulfur trial) at the Weyerhaeuser Albany Paper Mill was in response to a recurring problem of ring formation in the #3 Rotary lime kiln. The ring formation had resulted in periods of shut down to remove (blast) the rings. Figure 2.1 shows the number of times kiln was shut down to blast ring within a 15 month period. Kiln Shut due to Ring Blast. 33 0 z 0 F (<1°'' s' I cF' I F Figure 2.1. Histogram showing kiln shut down due to Ring Blasting. 16 Typically ring formation in lime kilns is associated with high levels of sodium in the lime mud due to poor mud washing. The problem of ring formation at the Albany Paper Mill is different because of low sodium levels. The sodium level in the lime mud is on the average less than 0.3 wt% water soluble sodium and 0.8 wt% total sodium, and is originally derived from NaOH, Na2CO3, Na2S and Na2SO4, in the residual white liquor in the mud. While the total sodium levels are not high it has been determined that the sulfur levels are equally very low, resulting in a much higher sodium to sulfur ratio. This may be contributing to ring formation because there is not enough sulfur available to tie up the sodium as sodium sulfate (Na2SO4) which is a more thermally stable compound. 17 Chapter 3. Methodology. A 4-day trial of emulsified sulfur addition was planned for July 29 through August 1, 2003. Tote bins of 70% solution of emulsified sulfur were purchased and a feed system consisting of a positive displacement pump, a filter to remove any crystallized sulfur, and an atomizing spray nozzle (with pressurized air atomization) was constructed for the trial. The diesel burner was temporarily removed from the kiln and the sulfur nozzle was installed in its place. Figure 3.1 shows a tote bin containing 70% solution of emulsified sulfur and the point at which it was fed to the kiln. Figure 3.1. 70% emulsified sulfur tote bin and emulsified sulfur input. 18 Sulfur feed was started on the morning of July 29 at rates from 44 to 50 quarts per hour or approximately 100 to 120 pounds of sulfur per hour. The sulfur feed was controlled to assure an excess of sulfur by observing the SO2 concentration in the # 3 rotary lime kiln stack and maintaining a concentration above 100 ppm corrected to 10% oxygen. Several sets samples of the following; lime mud feed, pre-coat filter filtrate, reburned lime, and precipitator dust were collected prior to the trial (4/7/03 through 7/29/03) and once following the trial (8/4/03). Samples were taken every 3 hours during the emulsified sulfur trial. Lime samples were also collected from 3 different locations: after the chain section, north sample port and south sample ports across the length of the kiln for analysis three times prior to the trial (5/30/03, 7/2/03, 7/24/03), twice during the trial (7/31/03, 8/1/03), and once after the trial (8/4/03). The trial was completed on the morning of August 1, 2003. Locations of sample collection are shown in the Figure 3.2 below. 19 Dust Figure 3.2. Picture of #3 Rotary lime kiln showing sampling locations High production rates were planned for the trial period but could not be maintained throughout the entire trial period. Production rates averaged from 100 to 165 TPD (tons per day) over the course of the 3-day trial, with 7/29/03 averaging 100 TPD, 7/30/03 averaging 150 TPD, and 8/31/03 at 165 TPD. An ICP (inductively coupled plasma) optical emission was used to analyze the samples. The basic technique involves the measurement of atomic emission by optical spectroscopy. Samples in solution or fine particles suspended in solution are nebulized and the resulting aerosol is transported to the plasma where element- specific emission spectra is produced. A grating spectrometer then disperses the resulting spectra. The spectral energy is measured at selected wavelengths and 20 compared with standards. The moisture content in the sample was accounted for by drying the sample at 1050 for 24 hours before samples were analyzed. The mud flow rate before and during the sulfur trial, ranged between 120 - 180 GMP (gallons per minute) as shown in Figure 3.3. The front and feed end temperatures were very consistent throughout the period of this study, the front end temperature was observed at about 2000°F while the feed end temperature was about 550°F. This is shown in Figure 3.4. II 1:iii 160 -hAOw 140 - &u Flow 120 .2 100 8O 6O 4o 20 0 L..... 7/26/03 7/28/03 7/30/03 8/1/03 8/3/03 8/5/03 8i7/03 Date Figure 3.3. Mud and solid flow data from 7/26/03 to 8/7/03 at Albany Paper Mill. 21 2500 2000 1500 1000 I- 500 nv 7/26/03 Figure 3.4. 7/28/03 7/30/03 1/)3 8/5/03 8/3/03 8/7/03 Front and backend temperature profile from 7/26/03 to 8/7/03 at Albany Paper Mill. The flue gas flow and induced draft (ID) fan speed ranged between 20-40 and 20-60 thousand standard cubic feet hour (KSCFH) respectively. 70 -G Fb* 10 n 7/26 7/28 7/30 .B/1 uate 8/3 8/5 8/7 Figure 3.5. Gas flow and ID fan speed data from 7/26/03 to 8/7/03 at Albany Paper Mill. 22 Excess oxygen was maintained below 10% during the duration of the study. Figure 3-6 illustrates the excess oxygen levels during the trial. 12 10 2 0' 7/27/0 7/28/0 7/29/0 7/30/0 7/31/0 8/1/03 8/2/03 8/3/03 8/4/03 8/5/03 8/6/03 3 3 3 3 3 Date Figure 3.6. Percent excess oxygen data from 7/26/03 to 8/7/03 at Albany Paper Mill. 23 Chapter 4. Results and Discussion. 4-1 Effect of burning sulfur on solid composition. 4-1.1 Sodium The results show a decrease in the sodium concentration of the mud fed to the kiln during the trial, compared to the baseline samples. There was a significant reduction of sodium in the dust samples compared to the rest of the mud samples. This result is illustrated in Figure 4.1. Sodium 4.0 3.5 Mud 3.0 Dust 2.5 o Chain 2.0 o North South Lim 0.5 0.0 Before During After Sulfur Trial Figure 4.1. Changes in sodium concentration before, during and after sulfur trial. 24 4-1.2 Sulfur As expected, the sulfur concentration in the product lime and the precipitator dust was higher during the trial than it was in the samples collected during the baseline sampling. It was also significantly higher than the sulfur content in the mud fed to the kiln. Figure 4.2 shows the sulfur concentration before and after the sulfur trial. Sulfur enrichment factor ranged from 7-12, the high sulfur enrichment was caused by the sulphation of NaOH or Na2CO3. There was an increase in the sulfur content in the solids as it moved through the kiln. Estimated kiln stack SO2 emissions averaged 13 pounds per hour with SO2 for sulfur loss averaging less than 7 pounds per hour. The remaining sulfur was bound to the sodium and calcium of the lime produced during the trial. Sulfur 1.2 1.0 0.8 0.6 IiiiiiiiiiiiiiiiiiIiiI.I [ZIZIZIZIiiiZIIJ 0.4 Mud Dust o Chain o North South Lime 0.2 0.0 Before During After Sulfur Trial Figure 4.2. Changes in concentration of sulfur before, during and after sulfur trial. 25 The addition of sulfur did not have any effect on phosphorus, silicon, aluminum or magnesium. As shown in the Figures 4.3, 4.4, 4.5 and 4.6 respectively. 4-1.3 Phosphorus Phosphorus 5.0 IVk.id Dust o chain a North South 2.0 Lirre 1.0 Before During After Sulfur Trial Figure 4.3. Changes in concentration of phosphorus before, during and after sulfur trial. I 4-1.4 Silicon Silicon [1111 0 Mid Dust o Chain D North South 0.20 Lime 0.10 [111111 Before During After Sulfur Trial Figure 4.4. Changes in concentration of silicon before, during and after sulfur trial. 27 4-1.5 Aluminum Aluminum 0.50 od Co 0.40 0 Dust 0 0 o Chain x o North 0 0 South Co oLJ 0 0.10 Before During After Sulfur Trial Figure 4.5. Changes in concentration of aluminum before, during and after sulfur trial. 4-1.6 Magnesium Magnesium 2.5 0 [1ud ( 0 Dust o Chain o North South o Line O.5 Before During After Sulfur Trial Figure 4.6. Changes in concentration of magnesium before, during and after sulfur trial. 29 4-1.7 Carbon dioxide The results obtained show there is no calcination occurring beyond the south sample port. It appears that lime mud, chain section, north, and south samples contain significant amounts of carbon dioxide in the kiln, this is an indication that calcinations has not yet taken place. It also confirms that the two stages; drying and heating, take place between the mud samples and the south samples at the Albany Paper Mill. Figure 4.7 shows the concentration of carbon dioxide before and after the sulfur trial. Co2 80 60 R Mud EXist o chain .4o 0 North South Lirre 20 0 Before During After Sulfur Trial Figure 4.7. Changes in concentration of carbon dioxide before, during and after trial. 30 4-1.8 Residual Carbonate Residual carbonate is a measure of the calcium carbonate in reburned lime, it is used as a measure of the conversion efficiency of the calcium carbonate in lime mud to calcium oxide in reburned lime. As shown in Figure 4.8, mud samples analyzed from the chain section, north port, dust and south port all had residual carbonate levels of more than 70%. This is an indication that recarbonation did not occur until the south port. Residual Carbonate 100 Md I- 80 60 0 Chain 40 o North 20 South C-) C) C5 Lime U) 0 Before During After Sulfur Trial Figure 4.8. Changes in concentration of residual carbonate before, during and after trial 31 4-2 Effect of burning sulfur on SO2 emission Burning emulsified sulfur resulted in high SO2 emissions from the kiln stack but this was within Department of Environmental Quality (DEQ) standard. SO2 generated from adding emulsified sulfur to the #3 rotary lime kiln picked up sodium inside the kiln and resulted in low levels of SO2 emission during the first 36 hours of the trial. Lime production rate and sodium concentration increased after 38 hours of the trial, when the shower water used in washing the mud was reduced. This resulted in high levels of SO2 emission in the stack gas. This observation indicates that lime mud had a shorter residence time in the kiln as the production rate increased, as a result, suiphation reaction between CaO/ CaCO3 and SO2 could not take place. This is shown in Figure 4.9. The rate of mud and SO2 input are shown in Figure 4.10. 32 14 500 a a. a 400 j 300 a. ...... 12 10# - S02 8c1) Emulsified_Sj " 200 4- 100 2 0 7/29 7/30 7/31 8/1 Date Figure 4.9. SO2 emission and emulsified sulfur input before, during and after trial. 500 500 -S02 400 400 -Mud Flow 300 300 200 Cl) 4fI -o 100 lULl ti 0L 7/29 Cl) 7/30 7/31 Date Figure 4.10. SO2 emission and mud flow before, during and after trial. 33 Chapter 5. Conclusion. This study has shown a valuable phenomeno logical review of the possibility of reducing sodium concentration in the kiln by burning emulsified sulfur in the # 3 rotary lime kiln, as shown in the sulfur trial results. The trial demonstrated a significant reduction of the sodium levels in the precipitation dust samples. The reduction of sodium in the dust was 50% which is an enrichment factor of 2 and a little less than 33% reduction or an enrichment factor of 1.3 for the rest of the solids, as shown in Figure 4.1. Although lime can effectively remove SO2, the removal efficiency decreased from 96.0% to 73.0% when emulsified sulfur was burned in the # 3 rotary lime kiln. It also demonstrates that recarbonation occurs right before calcination begins. This phenomenon is shown in Figure 4.8. A longitudinal study of all the variables related to the production of lime in the # 3 rotary lime kiln at Albany Paper mill, Oregon was analyzed to determine their relationships to ring formation, the results are shown in appendix A, Figures A.1.1 to A.1.10. 34 Chapter 6. Recommendations. This study provides a first look at the effects of burning 70% emulsified sulfur in the # 3 rotary lime kiln at the Albany Paper Mill in Oregon. However, further work needs to be done. A longer trial should be performed during periods when most of the rings form, this will help to directly relate burning emulsified sulfur to ring formation. During this next trial, fewer samples could be taken at greater time intervals to analyze the following metals: Na, Ca and S. The rest of the impurities could be ignored since they are inert in the production of lime. A pilot scale could be set up in the laboratory for further experimentation on a lime kiln proto type, where experiments could be performed at different conditions in order to minimize all risks involved in adding too much sulfur to the kiln while it is in operation. This will eliminate the possibility of forming sulfur related rings which are very difficult to remove from the kiln. Ring deposits may harden if too much sulfur is fed through the kiln to react with lime. Lime reacts with SO2, SO3 and 02 to form CaSO4. (Tran and Mao, 2001) This is shown in the following reactions: CaO(s) + SO2 (g) + ½ 02 (g) -* CaSO4 (s) 6-1 CaO(s) + SO3 (g) -* CaSO4 (s) 6-2 35 References. Boniface, A, "Introduction and Principals of Chemical Recovery", Chemical Recovery in the Alkaline Pulping Processes, 3141 Edition, p.1 -4 (1992) Doris, G. M. and Allen, L.H., Journal Pulp Paper Science 11(4): J89-98 (1985). Gorog P. and Adams T.N., "Design and Performance of Rotary Lime Kilns in the Pulp and Paper Industry - Parts 1 to 3". Kraft Recovery Operations Seminar, TAPPI PRESS, p. 41-62 (1987). Grace, T. M, Malcolm, E. W., "Pulp and Paper Manufacture", Canadian Pulp and Paper Association, Vol. 5, p 3- 14. Notidis, E. "The Formation of Guarded Sodium in Lime Mud", Masters Thesis, Graduate Department of Chemical Engineering and Applied Chemistry, University of Toronto, 1994. NOTIDIS, E. and Tran, H.N., "Survey of Lime Kiln Operation and Ringing Problems". TAPPI, Vol.76, No. 5, 1993, p.125. Sanchez, D. R., "Recausticizing Principles and Practice", 2001 Kraft Recovery Short Course, TAPPI PRESS, p. 2.1-1. Tran, H. N, "Lime Kiln Chemistry", 2001 Kraft Recovery Short Course, TAPPI PRESS, p. 2.3-1 2.3-8. Tran, H. N, Mao, X., and Barharm, D., "Mechanism of Ring Formation in Lime Kilns", International Conference on Chemical Recovery, June 7-11, 1992. Tran, H. N, Barharm, D., "An Overview of Ring Formation in Lime Kilns", TAPPI Pulping Conference, Toronto, October 1990, p. 2. Appendix. 37 Appendix A. Determination of correlation of variables with ring formation. Al. A longitudinal study was carried out to determine which variables are correlated with ring formation in the # 3 rotary lime kiln. Selected correlation variables include gas flow, back end temperature, front end temperature, mud density, ID Fan speed, ambient temperature, percent oxygen, mud flow, turbidity and lime production rate. Figures A. 1.1 through A. 1.10 illustrates the relationship between these variables and the days the # 3 rotary lime kiln was shut due to ring formation. 12 70 66 10 60 55 a 4 2 F Figure A.1.1. Gas flow vs. kiln shut as blast marker 1 CD 1 3 0 rt; CD - 3 CD CD 1 C CD N > CD -t .I1 1/11/03 100PM 1/27/03 900 PM 12/26/02 300AM 12/11/02 3:00AM 11/25/02 9:00 PM 11/9/02 3:00AM 10/26/02 9:00 AM 10/10/02 300 AM 9/24/02 5:00 PM 9/9/02 300 AM 8/28/02 1:00 PM 8/11/02 1:00AM 7/26/02 300 PM 7/9/02 3:00 AM 6/26/02 3:00 PM 6/16/02 9:00AM 6/4/02 100 PM 5/13/02530 PM 5/23/02 11:00PM 5/4/02 1:00 AM 4/19/02 7:00 AM 3/29/02 1 00 PM 3/12/02700 AM 2/23/02 3:00 AM 217/02 7:00 AM 1/18/02 7:00 PM 1/2102 7:00 AM a a a o 0 Feed Temp. 0 Blast Marker 0 0 0 - 00 -n CD t t B ci) cc) CD > cJ 1/17/033 00 AM 1/4/03 900AM 12/20/027.00 PM 12/7/02 300PM 11/22/027:00 PM 11/8/02300 PM 10/26/02 900AM 10/11/02 3 00 AM 9/27/02 3 00 PM 9/13/02 11.00 AM 9/2/02 5 00 PM 8/19/02 1:00 PM 8/4/02 1 00 PM 7/19/02 3:00AM 7/5/02 5 00 PM 6/15/02 700PM 6/24/02 900 PM 6/4/02 1 00 PM 5/14/02 1:00AM 5/24/02 3.00 AM 5/7/02 900 PM 4/25/02 7:00 AM 4/5/02 700 PM 3121/02 1:00AM 3/6/02 100 PM 2119/02 7:00 AM 214/02 100 PM 1/17/02 9:00 AM 1/2/02700 AM Mud Density - Blast Marker - 0 11 12 10 10 9 8 8 7 4 4 3 2 0 Figure A. 1.4. Percent oxygen vs. kiln shut as blast marker 2 0 i t 3 Cl') Cl') Cl') ct ri > r1 1/17/033:00 AM 1/4/03 9:00 AM 12/20/02 7:00 PM 1217/02 3:00 PM 11/22/027:00 PM 11/8/02 3:00 PM 10/26102 9:00 AM 10/11/02 3:00AM 9/27/02 3:00 PM AM 9/2/02 5:00 PM 6/19/02 1:00 PM 814/02 1:00 PM 7/19/02 3:00 AM 7/5102 5:00 PM 6/24/02 9:00 PM 6/15/02 7:00 PM 6/4/021:00 PM 5/24/02 3 00 AM 5/14/02 1 00 AM 517/02 9:00 PM 4/25/02 700 AM 4/5/02 7:00 PM 3/21/02 1:00 AM 3/6/02 1:00 PM 2/19/02 7:00 AM 2/4/02 100 PM 1/17/02 9:00 AM 112/02 700 AM Fan Speed Blast Marker U U I U U U U U U U U C 4 a t t B CI CD t CD t CD CD t 0 p.11 > CD t 1/25/03 300 PM 1/10/03 9.00 PM 12/27/02 9:00 AM 12/131027:00 PM 11/28/02 7:00 PM 11/13/021100 10/31/02 7.00 AM 10/16/02 3:00 AM 10/2102 3:00 PM 9/1 7102 3:00 PM 9/5/02 900 AM 8/23/02 7.00 PM 8/8/02 1.00 PM 7/23/02 3.00 AM 7/8102 300 AM 6/26/02 500 PM 6/16/02 1 00 AM 6/6/02 700 PM 5/26/02 1:00 AM 5/16/02 9:00AM 5/9/02 7:00 AM 4/26/02 1.00 AM 417/02 7 00 AM 3/23/02 700 AM 317/02 1 00 PM 2119/02 3:00 AM 214/02 3:00 AM 1/17102 1:00 PM 112102 7:00 AM Front Temp 0) Blast Marker 0) 0 t t çj 0 a; I1 1/17/03 3:00AM 1/4/03 9:00AM 12120/02 7:00PM 1217/02 3:00 PM 11/221027:00 PM 1 1/02 3:00 PM 10/26/02 9:00 AM 10/11/023.00 AM 9,27/02 300 PM 9/13/02 11:00AM 9/2/02 5:00 PM 8/19/02 1 00 PM 814/02 1:00 PM 7/19/02 3:00AM 6/24/02 900 PM 7/5/02 5:00 PM 6/15/02 7 00 PM 6/4/02 1 00 PM 5,24/02 300 AM 5/14/02 1:00AM 5/7/02 9:00 PM 4125/02 7 00 AM 3/21/02 1:00AM 4/5/02 7:00 PM 3/6/02 1:00 PM 2119/02 7:00 AM 214102 1.00 PM 1/17/02 9:00 AM 1,2/02 7:00 AM Mud Flow (gpm) Blast Marker 0 44 It appears that there are fewer ringing events in summer than in winter, which may be related to ambient temperatures. This is illustrated in Figure A.I.8. 12 140 120 10 100 80 I-. 80 40 2 20 0 r-c0coc' .ocor- r. I()C0C0(W) Figure A. 1.8. Ambient temperature vs. kiln shut as blast marker 45 River turbidity might contain certain impurities in the water used for mud washing. Figure A. 1.9 shows the relationship between turbidity and days the #3 rotary lime kiln was shut to blast a ring. Turbidity Vs. Blast 90 12 80 a... - 10 S S S S 70 80 Blast Ma,lt.r 50 Turbidity 40 30 20 2 10 0 0 88888888888888888888888888888 (tOt Bit B B B B Figure A. 1.9. Turbidity vs. kiln shut as blast marker 01 B B 46 Lime production rate, could be contributing to ring formation; this can be seen on Figure A.1.1O, where production rate is plotted showing ringing events. Ring formation increases during periods when lime production rates are sustained over 150 tons per day (TPD) for extended periods, but ring formation has also occurred at lower production rates. 200 180 160 I i 100 ' 01/01/02 04/11/02 07/20/02 I.. 10/28/02 Figure A.1.10 Lime production vs. ring blasting _80 02/05/03 05/18/03 08/24/03 I 47 A.2 Total material balance for solids during and after trial. Table A.2. 1. Total material balance for solids before and after trial. Sample CaO SO3 Na20 I(20 A1203 Fe203 S102 P205 MgO CO2 Total Name wt% wt% wt% wt% wt% wt% wt% wt% wt% wt% wt% LIME Before 79.99 0.053 1.851 0.022 0.295 0.069 0.275 2.654 1.234 13.53 99.97 During 91.06 1.108 1.413 0.018 0.342 0.061 0.362 2.911 1.231 1.50 100.00 After 93.28 0.083 1.590 0.018 0.295 0.060 0.263 2.909 1.255 0.24 99.99 CHAIN SECTION Before 55.23 0.035 1.099 0.012 0.142 0.038 0.135 1.649 0,769 40.91 100.02 During 59.52 0.333 0.939 0.012 0.191 0.037 0.201 1.687 0.752 40.94 99.97 After 54.32 0.045 0.822 0.020 0.157 0.031 0.173 1.672 0.498 41.53 99.97 Before 53.35 0.312 2.034 0.028 0,130 0.034 0.210 2.197 0.675 41.04 100.0 During 55.59 0.799 0.919 0.013 0.164 0.028 0.196 1.695 0.666 40.20 100.27 After 55.72 0.123 1.119 0.014 0.151 0.029 0.173 1.855 0.662 40,92 100.76 Before 53.74 0.027 1.007 0.010 0.125 0.031 0.141 1.453 0,677 42.79 100.00 During 55.23 0.051 0.832 0.012 0.173 0.029 0.197 1.683 0.653 41.14 100.( After 59.26 0.030 0.849 0.010 0.153 0.029 0.218 1.672 0.580 37.19 99.98 Before 54.72 0.038 1.103 0.011 0.149 0.037 0.155 1.621 0.743 41.44 100.01 During 54.06 0.567 0.930 0.011 0.193 0.035 0.206 1.848 0.757 41.31 100.88 After 57.75 0.043 0.970 0.011 0.174 0.037 0.186 1.970 0.730 40.98 99.98 Before 55.79 0.038 1.130 0.012 0.157 0.037 0.157 1.686 0.772 40.23 100.01 During 58.94 0.675 0.997 0.013 0.191 0.036 0.204 1.893 0.791 38.71 101.22 After 56.11 0.053 1.065 0.011 0.151 0.031 0.154 1.626 0.726 39.66 99.59 DUST MUD NORTH SOUTH 49 A.2.3. Process information data for solids during sulfur trial (cont.). KILN BRN LMPF #3 KILN MUD CONVERSIO ZONE TEMP FEED FEED TEMP DENSITY % N TO SOLIDS TONS/HR FLOW #3KIt.NFEED PRECIPIDFAN END 02 SPD (POUT) #3 KILN River Water MAIN GAS Twtldlty SOaData. FLW Dale and Irne Units DEG.F GPM DEG.F % tonThr(shor0 %02 IKSCFH 971J I P 7/30/0315:08 1824.71 75.31 260.36 24.97 147 1.58 27.08 2663 2.60 73.72 7/30/0316:08 1821.57 126.41 586.52 23.97 237 1.73 29.97 26.66 2.54 308.86 7/30/0317:08 1973.82 143.49 572.70 23.98 269 1.97 36.87 28.82 2.48 327.99 7/30/0318:08 2019.75 158.92 564.86 23.98 298 2.07 45.68 31.42 2.42 336.70 7/30/0319:08 1969.03 16423 572.41 23.98 308 2.16 51.79 34.21 2.38 318.59 7/30/0320:00 1870.43 164.79 605.22 23.99 309 2.59 55.44 2.30 303.93 7/30/0321:08 1805.34 165.18 596.81 23.99 310 2.18 54.05 2.22 344.70 7/30/032208 1775.69 165.07 597.87 23.99 309 1.94 53.27 2.15 351.75 7/301032308 1787.76 164.97 582.52 24.00 309 1.92 52.56 3666 2.07 35624 7/31/03060 177063 164.99 585.30 23.97 309 1.49 50.43 3661 1.99 382.67 7/31/031:00 1791.08 165.14 583.65 23.93 309 1.45 51.83 3850 1.91 360.78 7/31/032:00 180666 16529 591.76 23.88 308 1.51 53.62 39.93 1.83 350.32 7/31/033:00 1814.00 165.44 596.60 23.83 308 1.50 54.00 3975 1.76 352.33 7/311034:00 1826.41 165.59 599.39 23.79 308 1.50 53.55 3955 1.71 36620 7/31/035:00 1836.03 165.74 508.05 23.74 307 1.21 52.80 3931 1.85 318.36 7/31/036:00 185163 167.68 576.05 23.70 310 1.24 53.75 39.45 2.01 379.26 7/31/03 7:00 1862.78 177.51 590.63 23.65 328 1.55 58.59 41.04 2.18 284.22 7/31/038:00 1862.77 179.01 503.60 23.69 331 1.60 59.86 41.94 2.34 250.56 7/31/03 9:00 1869.37 179.06 595.37 23.80 333 1.59 60.58 4238 2.51 32063 7/31/031060 1848.98 179.11 597.75 23.90 334 1.59 60.70 4221 2.68 298.57 7/31/031160 1835.07 17924 600.12 24.01 336 1.62 60.82 42.07 2.84 286.55 7/31/031260 1817.85 179.90 600.09 24.11 339 1.61 60.93 4266 2.93 296.87 7/31/0313:08 1379.98 60.66 564.86 13.88 66 4.11 38.91 18.07 2.86 114.96 7/3110314:08 1792.09 130.79 574.79 22.02 225 1.15 41.87 3466 2.77 172.46 7/31/0315:08 1801.08 175.40 583.97 23.42 321 1.49 5525 39.42 2.69 287.77 7/3110316:08 1859.27 179.19 577.41 23.48 329 1.59 58.22 4079 2.61 321.33 7/31/0317:08 1914.93 17922 575.81 23.54 330 1.61 58.39 41.13 2.53 363.96 7/31/0318:08 1937.64 17925 57424 23.60 330 1.60 58.31 41.24 2.45 159.37 7/31/0319:00 1913.07 17929 578.98 23.66 331 1.60 5824 4t35 2.36 110.12 7/31/032060 1907.82 17932 582.16 23.72 332 1.60 58.64 4156 228 67.92 7/31/0321:08 1929.15 17935 586.07 23.78 333 1.61 58.48 4201 2.20 7.89 7/31/032260 195532 17938 592.04 23.84 334 1.61 58.30 4205 2.12 121 7/31/032360 1953.05 179.43 59321 23.88 335 1.61 58.17 4207 2.03 028 8/1/03 0:00 193363 179.57 55324 23.92 336 1.64 58.05 4203 1.95 0.21 8/1/03160 1915.20 179.71 594.05 23.97 336 1.61 57.92 41.81 1.88 0.14 8/1/03260 1899.27 179.81 595.18 24.01 337 1.60 57.80 41.59 1.78 0.07 8/1/033:08 189429 179.78 594.99 24.06 338 1.63 57.68 41.59 1.70 060 8/11034:00 1890.93 179.74 503.80 24.10 338 1.62 57.62 42.33 1.71 -0.07 8/1/03560 1887.56 179.65 598.43 24.15 339 1.58 57.86 4293 1.85 414 8/1/03660 1885.29 17950 601.57 24.15 339 1.59 58.14 4291 1.99 -0.19 8/1/03760 1892.07 17935 602,71 24.08 337 1.60 58.42 4290 2.14 8/1/038:00 189024 17922 605.52 24.01 336 1.60 58.69 4232 228 419 419 JJL 8/1/83960 1897.57 179.64 608.30 23.94 336 1.59 58.97 4296 2.42 -0.19 8/1/0310:00 1311.07 24.12 608.74 9.48 18 6.47 32.06 993 -0.19 8/110311:00 185332 120.45 599.58 22.66 213 0.43 3921 2.71 4.19 8/1/0312:00 1912.47 14054 572.90 24.35 267 1.51 44.00 j% 2.56 3528 2.74 -0.19 8/1/031360 1894.01 141.84 592.07 23.98 286 1.45 44.81 3562 2.69 4.19 8/1/0314:08 1912.53 145.10 598.86 23.66 268 1.50 46.67 J!... 2.63 4.19 8/1/0315:00 1924.37 14427 602.18 23.42 264 1.50 47.28 3719 2.58 -0.19 8/1/0316:08 1995.39 144.00 601.14 23.50 264 1.56 4651 3675 2.53 -0.19 8/1/0317:08 2029.97 143.75 585.37 23.62 265 1.57 44.06 3443 2.47 4.19 8/1/0318:00 2034.42 144.04 571.93 23.74 267 1.68 3397 2.42 -019 8/1/0319:00 2018.69 144.75 573.12 23.86 270 Ill 4353 43.59 3367 2.36 4.19 8/1/0320:00 2011.77 14469 575.05 23.99 271 1.74 43.73 3379 2.32 4.19 8/1/0321:08 2005.31 144.80 589.05 24.11 273 1.72 42.54 3373 8/1/032200 1995.62 144.70 581.95 24.23 274 1.62 42.52 3310 228 225 4.19 -020 50 A.2.4. Process information data for solids during sulfur trial (cont.). KILNBRN ZONE TEMP Date a #3 KILN MUD FEED TEMP DENSITY % N TO SOLIDS TONS/HR FLOW r limis FEED DEG.F GPM DEGF % CONVERSIO #3KILNFEED ton,1(shorO EM) 02 PRECIPIDFAN #3 KILN River War SPD (POW) MAIN GAS Turbidity SO1DSI. FLW %02 KSCFH Nih PPM 8/1/0323:00 1981.97 I4461 572.48 24.32 275 1.65 43.10 33.88 221 .0.22 8/2/030:00 1961.67 144.76 566.88 24.29 275 1.61 45.10 3496 2.18 .0.24 8/2/031:00 1941.74 14494 571.15 2424 274 1.67 44.96 2.14 .027 8/2/032:00 1943.23 14494 576.86 24.20 274 1.64 44.82 3493 2.11 -0.29 8/2/033:00 1946.70 14474 584.55 24.15 273 1.65 44.97 35.13 2.07 431 8/21034:00 1947.45 14464 583.60 24.11 272 1.64 44.96 3533 2.05 034 8/2/035:00 1947.73 14455 585.89 24.07 272 1.67 44.76 3567 2.05 -036 812/036:00 1946.13 14451 581.48 24.02 271 1.68 44.62 2.04 -0.37 8/2/037:00 1948.18 2397 266 1.64 44.56 3526 2.04 -0.38 8/2/038:00 1923.78 583.32 23.91 261 1.66 43.55 3497 2.04 -038 8/21039:00 1919.40 596.83 23.85 242 1.74 42.45 2.03 -02 8/2/0310:00 1934.17 Jj 576.27 12520 602.18 2181 233 1.64 38.67 3310 2.03 0.38 8/210311:00 2399 235 1.66 39.21 3326 2.03 -038 1963.95 l2537 601.45 8/2/0312:00 1986.34 12481 598.30 24.00 234 1.67 38.79 3288 2.03 4.38 8/2/0313:00 2003.62 11536 594.76 24.00 216 1.72 3523 2.03 .036 8/2/0314:00 2020.90 11035 591.15 24.01 207 1.84 33.23 3113 3012 2.04 -0.37 8/2/0315:00 2038.18 10974 592.48 24.02 206 2.10 32.03 2871 2.05 -0.34 8/2/03 16:00 2055.46 10943 572.04 24.02 205 2.04 28.38 2630 2.64 -0.32 8/2/0317:00 2055.16 10994 56l.54 24.03 206 2.74 29.91 2626 2.90 -0.30 8/2/0318:00 2038.29 11048 571.98 24.04 207 2.79 30.38 2626 2.77 -0.27 8/2/03 19:00 2023.17 111.06 577.37 24.04 209 2.81 30.61 25.98 2.65 -0.25 8/2/032000 2024.32 11t80 578.69 24.03 210 2.83 30.44 2594 2.53 023 8i2/0321:00 2024.18 11000 587.32 24.03 206 2.76 29.51 25.88 2.41 -020 8/2/0322:00 2000.18 l0918 591.55 24.03 205 2.77 31.31 25.85 229 -0.19 8/2/0323:00 2009.41 10945 586.81 24.03 205 2.81 30.70 2520 2.17 -0.l9 8/3/030:00 1996.04 10979 580.92 24.03 206 2.82 31.05 2596 2.05 -0.19 8/3/031:00 1960.35 11013 584.53 24.03 207 280 31.16 26.19 2.00 -0.19 8/3/032:00 1954.99 11047 591.64 24.03 207 2.80 31.01 26A8 2.02 -0.19 8/3/033:00 1967.87 11081 591.47 24.03 208 2.79 31.96 26.73 2.04 -0.19 8/3/034:00 1965.86 11107 594.81 24.03 208 2.81 32.11 2692 2.06 -0.19 8/3/03500 1957.t5 03971 597.72 24.03 206 2.66 31.72 2711 2.06 -0.19 8/3/036:00 1955.02 109.80 594.66 24.04 206 2.47 31.02 27.30 2.10 -019 8/3/037:00 1954.71 11030 596.64 24.04 207 2.48 31.79 27.40 2.12 -0.19 8/3/038:00 l951.42 109.51 594,73 24.04 206 2.53 3l.34 27.47 2.14 -0.19 8/3/039:00 1950.62 11001 602.26 24.05 207 2.37 32.14 2.16 -0.19 8/3/0310:00 1965.61 11044 59002 JZA. 24.03 207 1.93 30.75 2786 2.17 -0.19 8/3/0311:00 1976.04 11074 591.02 23.87 206 225 32.76 2794 2.19 -0.19 81310312:00 1979.89 11074 59849 23.86 206 2.32 32.34 2807 2.56 -0.19 8/3/0313:00 1975.39 11073 600.32 2188 207 2.28 32.55 2820 3.43 -0.19 8/310314:00 197025 11085 603.53 2190 207 2.29 31.34 2811 3.30 -0.19 8/3/0315:00 1976.79 11052 599.84 2193 207 227 32.46 3.17 -0.19 8/3/0316:00 l963.16 11047 600.01 23.95 207 2.48 33.10 2795 2807 3.04 -0.19 8/3/0317:00 1985.91 11042 602.38 23.97 207 2.31 32.99 2804 291 -0.19 8/3/0318:00 1969.65 11037 603.72 24.00 207 228 32.43 2805 2.78 -0.19 8/3/0319:00 1994.05 111.78 599.76 24.02 210 228 32.94 2805 2.65 -0.19 2896 2807 253 -019 2.46 419 2817 2.41 -0.19 2826 236 -0.19 -0.l9 8/3/032000 1992.94 11555 589.77 24.02 217 2.36 33.70 8/3/0321:00 1985.38 11500 589.40 24.02 216 2.38 33.44 8/3/0322:00 I970.26 11123 591.02 24.02 209 2.39 33.56 8/3/0323:00 1948.44 11076 601.52 2402 208 2.42 3320 8/4/030:00 1931.82 11074 603.51 2402 208 239 33.35 8/4/03196 1928.59 11073 614.47 24.01 208 221 34.51 j. 29.81 232 227 8/4/032:00 l946.17 11071 616.08 240l 208 2.03 32.13 2887 222 -0.19 8/4/03396 1979.68 11069 607.11 24.01 208 2.00 31.71 -019 1988.81 11065 60721 24.01 208 2.00 31.56 2906 2927 2.18 8/4/034:00 2.13 .0.19 8/4/035:00 1992.35 I1055 608.76 24.01 207 2.01 31.80 2948 2.13 419 8/4/036:00 1995.36 11546 607.99 24.01 207 1.99 31.89 2873 2.14 -0.17 0.19 51 A.2.5. Process information data for solids during sulfur trial (cont.). KILN BRN IMPF #3KLN MUD ZONETEMP FEED FEEDIEMP DENSffY% NT0 SOLIDS TONSIHR ftOW I CONVERSIO #3KLNFEED ENDO2 PRECIPIDFAN #3 KILN SPDOUT) YIAINGAS RerWat SO2Data. Turhiddy ftW Dale aid Tine L linils DEG.F 6PM DEG.F I bMr(sho %02 KSCFH ' 1998,92 11036 605,27 24.01 207 1.96 32.18 814/038:00 2002.34 11026 600.18 24.01 207 2.03 32.41 29.04 J ' NTtJ ' PPM 2.16 .0.11 2.17 .0.05 814/009:00 2007.27 110.16 596.85 24.01 207 127 31.73 29.00 2.59 0.01 814/03 10:00 1617.61 47.93 61025 1420 53 5.98 27.60 14.65 2.71 0.07 W431t00 842.71 aoo 502.14 7.35 0 4.30 23.00 415 2.87 0.12 814/0312:00 798.73 0 565.15 722 0 9.34 23.00 499 3.03 92.70 814/0313:00 798.73 0 587.11 7.28 0 9.36 23.00 482 3.18 265.07 8/4/0314:00 798.73 0 572.92 125 0 9.77 23.00 465 3.34 24.63 8/4/0315:00 798.73 0 575.11 721 0 10.20 23.00 448 3.58 .0.19 814/0316:00 1612.41 0 596.21 7.17 0 10.30 26,10 917 3.65 .0.19 8/4/0317:00 1788.24 591.14 8.75 7 5.37 30.85 2411 3.71 .0.19 814/0318:00 1838.15 11122 592.64 24.77 215 1.78 31.95 2539 3.49 .0.19 814/0319:00 1894.10 1105 593.20 24.70 224 2.04 38.07 293 326 .0.19 8/4/03200 1966.75 11917 500.74 24.62 229 226 32.75 2927 3.04 .0.19 814/0321.0 2001.03 11911 591.95 24.54 230 228 33.87 2926 2.81 0.19 W4/0322 202426 12022 588.93 24.47 220 2.30 33.03 29 2.58 .020 81410323:00 65 2002.81 12019 585.16 24.39 229 229 32.61 2918 2.35 .0.22 00 1979.00 119.94 500.77 24.31 228 2.30 33.55 29.23 2.13 .024 815/001:00 1952.85 11910 598.56 2424 227 2,31) 34.00 29.45 1.99 .0.27 815/002:00 1925.00 119A5 565.11 24.17 226 2.31 33.94 29.63 2.06 .0.29 8/5/003:00 1900.63 11L46 58827 24.12 221 2.30 34.98 29.62 2.13 .0.31 815/004:00 1881.87 11515 59623 24.07 217 2.31 34.53 29.57 220 .0.34 815/005:00 1880.41 11524 600.69 24.02 216 2.32 34.46 29.53 228 .0.36 8/5/006:00 1849.71 1154 600.77 23.97 216 227 34.65 2926 2.35 .0.37 8/5/03 52 A.2.6. ICP analysis data for solids during sulfur trial. Date Samp Name Na wV S K jn .PE S Fe M I Ca ppm ppm ppm ppm ppm wt 5/30/03 Lime L4 211 18 150( 267 1556 10444 6478 57. 7/2/03 Lime 1.36 270 2 163( 220 155 11400 7760 56.8 7/24/03 Lime _j 80 155 240 136 12500 7750 56. Lime 1 190 1561 240 1401 12011 77 57. _j/9 Lime Li 330 7/29 Lime 1.1 2600 7/29 Lime 1.00 7129 Lime i.0 7/30/03 Lime 7/30/03 Lime 7/30/03 _.224 if 1710 220 140 10600 6 66. 17 172 230 145' 12200 7 65. 5700 1 179 220 136 1141 64. 6300 1 170 21 139 i1 64. 0.9 6200 1 1750 240 138 130( 75 1.11 6000 11 1840 230 152 12000 7700 ...j. Lime 1.04 8000 i 17 220 145 12600 7700 65. 7/30/03 Lime t02 4500 1 17 220 152 12800 7600 65.6 7/30/03 Lime (19 6200 18 220 157 1300 74 7/30/03 Lime 0.99 5500 17 220 152 12500 6900 7/30)03 Lime (19 4600 18 220 141 12800 76 7/30/03 Lime _O.9 4000 18 220 157 1300 76 7/31/03 Lime _l.14 5400 17 181 210 30C 13300 7500 7/31/03 Lime _1.14 5400 17 181 210 30C 13300 7500 7/31)03 Lime 1.0 4000 141 187 200 204 13000 7 652 7/31/03 Lime 1,0 4400 161 17t 21 174 125( 7300 65. 7/31)03 Lime 1.1 5 221 18( 200 298 13000 7400 64.8 7/31)03 Lime 0.98 42 1 18f 220 U 12900 7400 65.5 7/31/03 Lime 0.9 4300 141 19 21 271 12900 7400 65.3 7/31/03 Lime 1. 350 1 19 21 13400 7300 65.6 7/31/03 Lime 1. 2200 1 19 2 2 13100 7800 66. 2 137C 740 65.3 13800 7000 65. l 65. _j. 62.5 _j _jj4 j.4 1/03 Lime 1.1 1400 1 18 190 W1/03 Lime 1.05 1100 1 19 220 8/1/03 Lime 1.1 1100 1 1 200 3 14100 710 64.3 8/1/03 Lime 1.1 100 1 1 200 209 14300 710 65. 8/1/03 Lime 1.1 1000 1 1 200 209 14300 7100 8/4/03 Lime 1.1 33 1 156 210 1 12700 757 ...j5 66. 53 A.2.7. ICP analysis data for solids during sulfur trial (cont.). Date Sample Name Al Fe Si _____P ppm ppm ppm ppm S Na wjamj M Ca m 7/24 Chain Section 0.82 142 9 751 132 72 7201 4 7/29 Chain Section 0.71 1600 75 99 130 970 77 4 _4 7/31 Chain Section 0.69 1200 110 102 130 112' 7200 4 _39 7/31 ChainSection 0.69 1200 110 102 130 112 7200 4 45 8/1 ChainSection 0.7 420 lii 1020 110 178 8 47 39 8/1 ChainSection 0.74 420 110 1020 110 178 81 4700 4 8/4/03 Chain Section 0.61 180 17 83 110 92 7300 39 8/4/03 Chain Section 0.61 180 17 83 110 92 7300 38 7054 37. 5/30/03 Dust 0.73 7/2103 Dust 2.4 7/24 Dust 7/24 7 215 946 39 1 667 2407 441 7 110 14 1.11 261 111 67 1 1055 Dust 1.79 2107 24 6 Dust 1,0 500 11 81 1 7 Dust 0.64 650 9 81 1 7 Dust 0.7230001 7 Dust 0.71 3000 7 Dust 0.61 2600 II 7 Dust 0.65 11 7 Dust 0. 7/30/03 Dust 0. 7/30/03 Dust 0. 7/30/03 Dust 0. 38 1 1 6600 7/30/03 Dust 0. 36 1 1 67 4 40.0 7/30/03 Dust 0. 35 1 71 3 39. 7/31/03 Dust 0. 35 4 38.4 7/31/03 Dust 0. 44 11 89 7/31/03 Dust 0. 38 1 96 7/31/03 Dust 0. 4600 7/31/03 Dust 0. 4 1 7/31/03 Dust 0. 33 1 7/31/03 Dust 0. 38 1 88 11 3 7/31/03 Dust 0. 1 1 86 117 3 1073 1 9429 37. 4 39.4 474 37. 890 39. 122 39. 7 40. 71 39. 1 7700 38. 1 7700 39. 11 1 8500 39. 1 1 81 1 1 13037 _j9. 7300 1 66 1 7 41. 39.6 3650 39.6 3 40. 40.4 90 9 40. 3680 __29 40.1 54 A.2.8. ICP analysis data for solids during sulfur trial (cont.). Date Sample Name S wt _p Al Fe ppm ppm I JE11 ___Si jpm Ca I ppm ppm wr 8/1)03 Dust 0.71 1200 120 900 87 11 8000 4020 39.6 8/1/03 Dust 0.72 1200 140 841 80 11 7600 3940 39.8 811/03 Dust 0.7 840 13 91( 90 ii 6900 811/03 Dust 0.7 780 13 8 80 104 6700 3890 39.4 490 120 801 100 92 8100 3990 39.8 40.8 8/4/03 Dust 0.6 5/30/03 Mud 0. 86 89 631 108 77 5679 2 38. 7/2/03 Mud 0. 143 99 792 117 88 7371 4892 38. 7/24/03 Mud 0.69 86 5 548 96 61 521 3 38.1 7/24)03 Mud 0.81 117 8 67t 11 796 7108 4 39. 7/29/03 Mud 0.65 _1i0 9 871 100 7100 3 j& 7/29/03 Mud 0. 110 92 840 100 108 6600 3400 38.3 7/29/03 Mud 0. 1 9 860 11 105 7700 3500 37. 7/29/03 Mud 0.54 120 86 100 108 7300 3200 37. 1/30/03 Mud 0.68 1 11 94 11 121 8200 4 42.6 7/30/03 Mud 0.6 1 10 94 10 111 8100 4200 38.9 7/30103 Mud 0.55 1 10 9f 12 8000 4400 382 7/30/03 Mud 0.64 1 11 94 114 7500 4400 382 7/30)03 Mud 0.6 1 16 9f 110 125 7800 4400.1 7/30/ Mud 0, 11 9 8 10 105 7700 3500 37. 7/30/03 Mud 0. 1 76 880 100 108 7300 3200 37, 7/30103 Mud 0. 1 8 & 100 881 6500 4000 39.0 7/31/03 Mud 0.68 230 1 97 120 113( 7 00 4300 __._ 7/31)03 Mud 0.68 260 11 9 120 141( 8200 4400 39J 7/31/03 Mud 0. 290 _9 931 7000 3760 39.5 7I31/03 Mud 0.6 360 1 91 88 1011 7 387 39. 9 8 1051 3990 46.2 9 8 1051 85 1044 6500 40 8 1051 & 39 76 7/31 Mud 0. 340 11 7/31/03 Mud 0.65 340 11 7/31/03 Mud 0.59 320 7/31/03 Mud 0. 340 7/31/03 Mud 0.65 340 811/03 Mud 0. 360 9 8/1/03 Mud 0 350 10 10 92 _8 _9 _8 8& _9 _1 3990 _j5 40. _4 87 1101 7500 3990J2. 81 Ith 68 3940 39.5 78 1081 69 39 39.8 8/1/03 Mud 8/1/03 Mud 8/4/03 Mud E/30/03 North 7/2103 North 7/24/03 North 7/24/03 North 7/30/03 North 7/31/03 North 7/31103 North 8/1/03 North 8/1/03 North 8/4/03 North 8/4/03 North 5/30/03 South 7/2/03 South 7/24103 South 7/24/03 South 7/30/03 South 7/31/03 South 7/31/03 South 8/1/03 South 8/1/03 South 8/4/03 South 8/4103 South