高含氮量煤层气吸附—液化过程研究
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摘要
我国煤层气资源相当丰富,储量相当于450亿吨标准煤。煤层气开发利用既为我国国民经济提供一种优质清洁能源,又对增进煤矿安全、降低温室气体排放等有重要意义。煤层气利用面临的一个主要障碍是单个矿井煤层气产量较小,且煤层气产地往往远离现有天然气管网,即使离管网较近也由于气质差别较大不能直接入网。采用液化方法是解决煤层气从产地向使用地运输的一种有效手段。
煤层气本身可能含有较多氮气,或者在开采过程中有可能注入氮气,因而煤层气相对一般的天然气很可能含有更多氮气。高含氮量煤层气的液化与一般天然气的液化方案会有明显不同。本文重点分析先通过吸附方式分离氮气再进行浓缩甲烷液化的技术方案。针对特定组分的煤层气从预处理到液化做了实验和理论两方面的探讨,为解决高含氮量煤层气液化提供了一条技术途径。
本文根据现有条件以及相关资料对高含氮量的煤层气的吸附-液化过程开展了以下研究工作:
(1)利用氮气替代甲烷使用吸附实验台进行了脱水和脱二氧化碳研究。实验使用水分仪和气相色谱仪分别测出脱水过程吸附曲线和脱二
Currently, our country boasts its abundant coalbed gas resources, which can be converted to 45 billion tons of standard coal. The development and applications of this alternative clean and premium energy resource will also contribute to the promotion of coal mine safety as well as the lowering of green house gases emissions. The primary obstacle faced by coalbed methane utilization is the low production of single coalbed mine. At the same time, the production sites of coalbed methane are usually far from gas pipe network, and the gas quality variation also make it impossible to inlet the gas into the pipeline, even though is the sites are near the pipe network. The adoption of liquefaction is an effective method to transport coalbed methane from production site to the customers.
Coalbed methane itself may contain larger amount of nitrogen compared with natural gas. Nitrogen may also be added into coalbed methane during
煤层气本身可能含有较多氮气,或者在开采过程中有可能注入氮气,因而煤层气相对一般的天然气很可能含有更多氮气。高含氮量煤层气的液化与一般天然气的液化方案会有明显不同。本文重点分析先通过吸附方式分离氮气再进行浓缩甲烷液化的技术方案。针对特定组分的煤层气从预处理到液化做了实验和理论两方面的探讨,为解决高含氮量煤层气液化提供了一条技术途径。
本文根据现有条件以及相关资料对高含氮量的煤层气的吸附-液化过程开展了以下研究工作:
(1)利用氮气替代甲烷使用吸附实验台进行了脱水和脱二氧化碳研究。实验使用水分仪和气相色谱仪分别测出脱水过程吸附曲线和脱二
Currently, our country boasts its abundant coalbed gas resources, which can be converted to 45 billion tons of standard coal. The development and applications of this alternative clean and premium energy resource will also contribute to the promotion of coal mine safety as well as the lowering of green house gases emissions. The primary obstacle faced by coalbed methane utilization is the low production of single coalbed mine. At the same time, the production sites of coalbed methane are usually far from gas pipe network, and the gas quality variation also make it impossible to inlet the gas into the pipeline, even though is the sites are near the pipe network. The adoption of liquefaction is an effective method to transport coalbed methane from production site to the customers.
Coalbed methane itself may contain larger amount of nitrogen compared with natural gas. Nitrogen may also be added into coalbed methane during
引文
[1] 李汉林, 马士坤, 连承波. 煤层气勘探开发现状及展望. 西部探矿工程. 2006,128(12):85~86
[2] 柳正. 加快煤层气开发,提高我国能源自供能力. 西部资源. 2006,10(1):13~16
[3] Arastoopour H.University of Indonesia Gas Engineering Program.Institute of Gas Technology. Chicago, Illinois 60616, U.S.A, 1982.
[4] 程林峰. 煤层气注入增产法的探讨. 中国煤层气.2006,3(3):40~43
[5] Anderson R B ,Bayer J ,Hofer L J E. Equilibrium sorption studies of methane on Pittsburgh Seam and Poca2hontas No. 3 Seam Coal. Coal Science ,1966 :326.
[6] Daines M E. Apparatus for the determination of methane sorption on coal at high pressures by a weighing method . Journal of Rock Mechanics and Mining Science ,1968 ,5 :27.
[7] Ruppel T C , Grein C T , Bienstock D. Adsorption of methane/ethane mixture on dry coal at elevate pressure . Fuel ,1972 ,51 :297.
[8] Ruppel T C , Grein C T , Bienstock D. Adsorption of methane on dry coal at elevate pressure . Fuel ,1974 ,53 :152.
[9] Joubert J I ,Grein C T ,Bienstock D. Sorption of methane in moist coal .Fuel ,1973 , 52 (3) :181.
[10] Joubert J I , Grein C T ,Bienstock D. Effect of moisture on the methane capacity of American coals . Fuel ,1974 ,53 (3) :186.
[11] Kim A G. Estimating methane content of bituminous coal beds from adsorption data . US Bureau of Mines Report of Investigations .No. 8247 ,1977.
[12] Lee Y H. Methane recovery from coalbeds Effects of monolayer capacity and pore structure on gas content . NM: Univ of NM .Albuquerque ,May 1982.
[13] Ralph T Yang ,John T Saunders. Adsorption of gases on coals and heattreated coals at elevated temperature and pressure . Fuel ,1985 ,64 :616 ~625.
[14] Gregory J Bell , Karen C Rakop. Hysteredis of methane/coal sorption isotherms.SPE 15454 ,1986.
[15] Mavor M J ,Owen L B , Pratt T J . Measurement and evaluation of coal sorption isotherm data. SPE 20728 ,1990.
[16] Beamish B B , O’Donnell G. Microbalance applications to sorption testing of coal . Proceedings of Symposium on Coalbed Methane Research and Development in Australia, Townsville, Queensland ,1992.
[17] Levine J R ,Johnson P W , Prakash G. A gravimetric method of measuring gas sorption in coal . Proceeding Abstracts of the Eighth Annual Meeting of the Society for Organic Petrology, Lexington ,Kentucky ,1991.
[18] Levine J R ,Johnson P ,Beamish B B. High Pressure Microbalance Sorption Stedes. No 9342 , Proceedings of the 1993 International coalbed methane symposium,The University of Alabama / Tuscloosa ,May 17~21 ,1993.
[19] Stevenson M D. Adsorption/ desorption of multiOcomponent gas mixtures at in seam conditions [ C ] . SPE 23026 ,1991.
[20] Greaves K H ,Owen L B. MultiOcomponent gas adsorption/ desorptionbehavior of coal . No 9353 ,the International Coalbed Methane Symposium , The University of Alabama/ Tuscloosa , 1993.
[21] Arri L E ,Dan Yee. Modeling coalbed methane production with binary gas sorption. SPE 24363 ,1992.
[22] Harpdani S ,Pariti U M. Study of coal sorption isotherms using a multicomponent gas mixture . No 9356 , the 1993 International Coalbed Methane Symposium , The University of Alabama/ Tuscloosa ,1993.
[23] Anbarci K,Ertekin T. A simplified for inOsitu characterization of desorption properties of coal seams . SPE 21808 ,1991.
[24] Hawkins J M ,Schraufnagel R A ,Olszewski A J . Estimating coalbed gas content and sorption isotherm using well log data. SPE 24909 ,1992.
[25] Hall F E ,ChunOhe Zhou ,Gasem K A M ,et al. Adsorption of pure methane , nitrogen , and carbon dioxide and their binary mixtures on wet fruitland coal . SPE 29194 ,1994.
[26] Chaback J J ,Morgan D ,Yee D.Sorption irreversibilities and mixture compositional behavior during enhanced coalbed methane recovery processes. SPE 35622 ,1996.
[27] 吴俊. 表面能的吸附法计算及研究意义 .煤田地质与勘探.1994 ,22(4):18~23.
[28] 周胜国,郭淑敏. 煤储层吸附/ 解吸等温线测试技术.石油实验地质.1999 ,21(1):76~80.
[29] 高绪晨,张炳,羡法. 煤层工业分析、吸附等温线和含气量的测井解释. 测井技术.1999 ,23(2): 108~111.
[30] 崔永君. 煤等温吸附特性测试中体积校正方法探讨. 煤田地质与勘探,1999 ,27(5):29~32.
[31] 刘红林,王红岩,张建博. 煤层气吸附时间计算及其影响因素分析. 石油实验地质.2000,23(4): 365~367.
[32] 辜敏,陈昌国,鲜学福. 抽放煤层气变压吸附过程的数学模拟. 煤炭学报.2001,26(3):323~326.
[33] 辜敏,陈昌国,鲜学福. 混合气体的吸附特征. 天然气工业.2001 ,21(4):91~94.
[34] 蔺金太,郭勇义,吴世跃. 煤层气注气开采中煤对不同气体的吸附作用. 太原理工大学学报.2001,32(1):18~20.
[35] Haq N, Ruthven D M, Colloid J. Interf. Sci. 1986,112:164.
[36] Haq N, Ruthven D M, Colloid J. Interf. Sci. 1986,112:164.
[37] Ruthven D M,. AIChE J. 1976,22:753.
[38] Tezel F H, Apolonatos G. Gas Sep. Purif. 1993,7:11.
[39] Ackley M.W., R.T. Yang, AIChE J. 1990,36:1229.
[40] Delgado J A, Uguina M A, Sotelo J Letc. Modelling of the fixed-bed adsorption of methane/nitrogen mixtures on silicalite pellets.Separation and Purification Technology. 2006,50(2):192~203.
[41] Cavenati S, Grand C A, Rodrigues A E. Separation of CH4/CO2/N2 mixtures by layered pressure swing adsorption for upgrade of natural gas. Chemical Engineering Science. 2006, 61(12):3893~3906.
[42] 付永兴,李化治,郭桂彬等.煤层气液化装置流程及经济性分析.低温与特气.2004, 22(4):10~13.
[43] 曹文胜,鲁雪生,石玉美等.小型天然气液化流程.天然气工业.2005, 25(5):109~111.
[44] 王遇冬,陈慧芳.天然气处理与加工工艺.西安石油学院.1993.
[45] Kosseim A J et al.New Development in Gas Purification for LNG Plants.Tenth international Conference & Exhibition on Liquefied Natural Gas, Chicago, Illinois, USA, 1992, Session Ⅱ, paper 11.
[46] 郑大振.LNG 工厂的天然气净化工艺及其新发展. 天然气工业. 1994,14(4):67~72.
[47] Peterson K S 著,郭天民译. 石油与天然气的性质. 中国石化出版社. 1992.
[48] 邹仁筠. 石油化工分离原理与技术.北京:化学工业出版社, 1988.
[49] Purvin, Gertz Inc. Nitrogen Removal Requirements from Natural Gas, Report prepared,Dallas, Texas, for Kellogg Brown & Root, Gas Research Institute, May 1999.
[50] 谭建宇,李红艳,王莉等.小型天然气液化装置工艺流程数值模拟和优化.天然气工业.2005,25 (5) :112~114.
[51] 顾安忠,鲁雪生,汪荣顺,等. 液化天然气技术.北京:机械工业出版社,2003.1~190
[52] 辜敏,鲜学福. 提高煤矿抽放煤层气甲烷浓度的变压吸附技术的理论研究. 天然气化工. 2006,31(6):6~10.
[53] 苏现波,林萌,林晓英等. 吸附势理论在煤层甲烷吸附中的应用. 中国煤层气. 2006,3(2)期29~30.
[54] 傅国旗,周理. 甲烷在活性炭上吸附等温线的测定及分析. 天然气工业. 2004,24(1):92~94.
[55] Kouvelos E, Kesore K, Steriotis T,et al. High pressure N2/CH4 adsorption measurements in clinoptilolites. Microporous and Mesoporous Materials. 2007, 99(1):106~111.
[56] Li P Y and Tezel F H. Adsorption separation of N2, O2, CO2 and CH4 gases by β-zeolite. Microporous and Mesoporous Materials. 2007, 98(3):94~101.
[57] Carrott P J, Cansado L P and Carrott R. Carbon molecular sieves from PET for separations involving CH4, CO2, O2 and N2. Applied Surface Science. 2006, 252(17):5948~5952.
[58] Moon S H and Shim J W. A novel process for CO2/CH4 gas separation on activated carbon fibers-electric swing adsorption. Journal of Colloid and Interface Science.2006, 298(2):523~528.
[59] Nabais J M, Carrott P J, Carrott P, et al. Dominguez and A.L. Ortiz.New acrylic monolithic carbon molecular sieves for O2/N2 and CO2/CH4 separations. Carbon. 2006,44(7): 1158~1165.
[60] Cavenati S, Grande C A and Rodrigues A E. Separation of CH4/CO2/N2 mixtures by layered pressure swing adsorption for upgrade of natural gas. Chemical Engineering Science. 2006, 61(12):3893~3906.
[61] Busch A, Gensterblum Y, Krooss B M,et al. Investigation of high-pressure selective adsorption/desorption behaviour of CO2 and CH4 on coals: An experimental study. International Journal of Coal Geology. 2006,66(1): 53~68.
[62] Harlick P J, and Tezel F H. An experimental adsorbent screening study for CO2 removal from N2. Microporous and Mesoporous Materials. 2004, 76(3):71~79.
[63] Cui X J, Bustin R M and Dipple G. Selective transport of CO2, CH4, and N2 in coals: insights from modeling of experimental gas adsorption data. Fuel. 2004, 83(3):293~303.
[2] 柳正. 加快煤层气开发,提高我国能源自供能力. 西部资源. 2006,10(1):13~16
[3] Arastoopour H.University of Indonesia Gas Engineering Program.Institute of Gas Technology. Chicago, Illinois 60616, U.S.A, 1982.
[4] 程林峰. 煤层气注入增产法的探讨. 中国煤层气.2006,3(3):40~43
[5] Anderson R B ,Bayer J ,Hofer L J E. Equilibrium sorption studies of methane on Pittsburgh Seam and Poca2hontas No. 3 Seam Coal. Coal Science ,1966 :326.
[6] Daines M E. Apparatus for the determination of methane sorption on coal at high pressures by a weighing method . Journal of Rock Mechanics and Mining Science ,1968 ,5 :27.
[7] Ruppel T C , Grein C T , Bienstock D. Adsorption of methane/ethane mixture on dry coal at elevate pressure . Fuel ,1972 ,51 :297.
[8] Ruppel T C , Grein C T , Bienstock D. Adsorption of methane on dry coal at elevate pressure . Fuel ,1974 ,53 :152.
[9] Joubert J I ,Grein C T ,Bienstock D. Sorption of methane in moist coal .Fuel ,1973 , 52 (3) :181.
[10] Joubert J I , Grein C T ,Bienstock D. Effect of moisture on the methane capacity of American coals . Fuel ,1974 ,53 (3) :186.
[11] Kim A G. Estimating methane content of bituminous coal beds from adsorption data . US Bureau of Mines Report of Investigations .No. 8247 ,1977.
[12] Lee Y H. Methane recovery from coalbeds Effects of monolayer capacity and pore structure on gas content . NM: Univ of NM .Albuquerque ,May 1982.
[13] Ralph T Yang ,John T Saunders. Adsorption of gases on coals and heattreated coals at elevated temperature and pressure . Fuel ,1985 ,64 :616 ~625.
[14] Gregory J Bell , Karen C Rakop. Hysteredis of methane/coal sorption isotherms.SPE 15454 ,1986.
[15] Mavor M J ,Owen L B , Pratt T J . Measurement and evaluation of coal sorption isotherm data. SPE 20728 ,1990.
[16] Beamish B B , O’Donnell G. Microbalance applications to sorption testing of coal . Proceedings of Symposium on Coalbed Methane Research and Development in Australia, Townsville, Queensland ,1992.
[17] Levine J R ,Johnson P W , Prakash G. A gravimetric method of measuring gas sorption in coal . Proceeding Abstracts of the Eighth Annual Meeting of the Society for Organic Petrology, Lexington ,Kentucky ,1991.
[18] Levine J R ,Johnson P ,Beamish B B. High Pressure Microbalance Sorption Stedes. No 9342 , Proceedings of the 1993 International coalbed methane symposium,The University of Alabama / Tuscloosa ,May 17~21 ,1993.
[19] Stevenson M D. Adsorption/ desorption of multiOcomponent gas mixtures at in seam conditions [ C ] . SPE 23026 ,1991.
[20] Greaves K H ,Owen L B. MultiOcomponent gas adsorption/ desorptionbehavior of coal . No 9353 ,the International Coalbed Methane Symposium , The University of Alabama/ Tuscloosa , 1993.
[21] Arri L E ,Dan Yee. Modeling coalbed methane production with binary gas sorption. SPE 24363 ,1992.
[22] Harpdani S ,Pariti U M. Study of coal sorption isotherms using a multicomponent gas mixture . No 9356 , the 1993 International Coalbed Methane Symposium , The University of Alabama/ Tuscloosa ,1993.
[23] Anbarci K,Ertekin T. A simplified for inOsitu characterization of desorption properties of coal seams . SPE 21808 ,1991.
[24] Hawkins J M ,Schraufnagel R A ,Olszewski A J . Estimating coalbed gas content and sorption isotherm using well log data. SPE 24909 ,1992.
[25] Hall F E ,ChunOhe Zhou ,Gasem K A M ,et al. Adsorption of pure methane , nitrogen , and carbon dioxide and their binary mixtures on wet fruitland coal . SPE 29194 ,1994.
[26] Chaback J J ,Morgan D ,Yee D.Sorption irreversibilities and mixture compositional behavior during enhanced coalbed methane recovery processes. SPE 35622 ,1996.
[27] 吴俊. 表面能的吸附法计算及研究意义 .煤田地质与勘探.1994 ,22(4):18~23.
[28] 周胜国,郭淑敏. 煤储层吸附/ 解吸等温线测试技术.石油实验地质.1999 ,21(1):76~80.
[29] 高绪晨,张炳,羡法. 煤层工业分析、吸附等温线和含气量的测井解释. 测井技术.1999 ,23(2): 108~111.
[30] 崔永君. 煤等温吸附特性测试中体积校正方法探讨. 煤田地质与勘探,1999 ,27(5):29~32.
[31] 刘红林,王红岩,张建博. 煤层气吸附时间计算及其影响因素分析. 石油实验地质.2000,23(4): 365~367.
[32] 辜敏,陈昌国,鲜学福. 抽放煤层气变压吸附过程的数学模拟. 煤炭学报.2001,26(3):323~326.
[33] 辜敏,陈昌国,鲜学福. 混合气体的吸附特征. 天然气工业.2001 ,21(4):91~94.
[34] 蔺金太,郭勇义,吴世跃. 煤层气注气开采中煤对不同气体的吸附作用. 太原理工大学学报.2001,32(1):18~20.
[35] Haq N, Ruthven D M, Colloid J. Interf. Sci. 1986,112:164.
[36] Haq N, Ruthven D M, Colloid J. Interf. Sci. 1986,112:164.
[37] Ruthven D M,. AIChE J. 1976,22:753.
[38] Tezel F H, Apolonatos G. Gas Sep. Purif. 1993,7:11.
[39] Ackley M.W., R.T. Yang, AIChE J. 1990,36:1229.
[40] Delgado J A, Uguina M A, Sotelo J Letc. Modelling of the fixed-bed adsorption of methane/nitrogen mixtures on silicalite pellets.Separation and Purification Technology. 2006,50(2):192~203.
[41] Cavenati S, Grand C A, Rodrigues A E. Separation of CH4/CO2/N2 mixtures by layered pressure swing adsorption for upgrade of natural gas. Chemical Engineering Science. 2006, 61(12):3893~3906.
[42] 付永兴,李化治,郭桂彬等.煤层气液化装置流程及经济性分析.低温与特气.2004, 22(4):10~13.
[43] 曹文胜,鲁雪生,石玉美等.小型天然气液化流程.天然气工业.2005, 25(5):109~111.
[44] 王遇冬,陈慧芳.天然气处理与加工工艺.西安石油学院.1993.
[45] Kosseim A J et al.New Development in Gas Purification for LNG Plants.Tenth international Conference & Exhibition on Liquefied Natural Gas, Chicago, Illinois, USA, 1992, Session Ⅱ, paper 11.
[46] 郑大振.LNG 工厂的天然气净化工艺及其新发展. 天然气工业. 1994,14(4):67~72.
[47] Peterson K S 著,郭天民译. 石油与天然气的性质. 中国石化出版社. 1992.
[48] 邹仁筠. 石油化工分离原理与技术.北京:化学工业出版社, 1988.
[49] Purvin, Gertz Inc. Nitrogen Removal Requirements from Natural Gas, Report prepared,Dallas, Texas, for Kellogg Brown & Root, Gas Research Institute, May 1999.
[50] 谭建宇,李红艳,王莉等.小型天然气液化装置工艺流程数值模拟和优化.天然气工业.2005,25 (5) :112~114.
[51] 顾安忠,鲁雪生,汪荣顺,等. 液化天然气技术.北京:机械工业出版社,2003.1~190
[52] 辜敏,鲜学福. 提高煤矿抽放煤层气甲烷浓度的变压吸附技术的理论研究. 天然气化工. 2006,31(6):6~10.
[53] 苏现波,林萌,林晓英等. 吸附势理论在煤层甲烷吸附中的应用. 中国煤层气. 2006,3(2)期29~30.
[54] 傅国旗,周理. 甲烷在活性炭上吸附等温线的测定及分析. 天然气工业. 2004,24(1):92~94.
[55] Kouvelos E, Kesore K, Steriotis T,et al. High pressure N2/CH4 adsorption measurements in clinoptilolites. Microporous and Mesoporous Materials. 2007, 99(1):106~111.
[56] Li P Y and Tezel F H. Adsorption separation of N2, O2, CO2 and CH4 gases by β-zeolite. Microporous and Mesoporous Materials. 2007, 98(3):94~101.
[57] Carrott P J, Cansado L P and Carrott R. Carbon molecular sieves from PET for separations involving CH4, CO2, O2 and N2. Applied Surface Science. 2006, 252(17):5948~5952.
[58] Moon S H and Shim J W. A novel process for CO2/CH4 gas separation on activated carbon fibers-electric swing adsorption. Journal of Colloid and Interface Science.2006, 298(2):523~528.
[59] Nabais J M, Carrott P J, Carrott P, et al. Dominguez and A.L. Ortiz.New acrylic monolithic carbon molecular sieves for O2/N2 and CO2/CH4 separations. Carbon. 2006,44(7): 1158~1165.
[60] Cavenati S, Grande C A and Rodrigues A E. Separation of CH4/CO2/N2 mixtures by layered pressure swing adsorption for upgrade of natural gas. Chemical Engineering Science. 2006, 61(12):3893~3906.
[61] Busch A, Gensterblum Y, Krooss B M,et al. Investigation of high-pressure selective adsorption/desorption behaviour of CO2 and CH4 on coals: An experimental study. International Journal of Coal Geology. 2006,66(1): 53~68.
[62] Harlick P J, and Tezel F H. An experimental adsorbent screening study for CO2 removal from N2. Microporous and Mesoporous Materials. 2004, 76(3):71~79.
[63] Cui X J, Bustin R M and Dipple G. Selective transport of CO2, CH4, and N2 in coals: insights from modeling of experimental gas adsorption data. Fuel. 2004, 83(3):293~303.
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