TBAB半笼型水合物法分离CO2/CH4混合气的过程研究  

TBAB Semi-Clathrate Hydrate Formation and its Application in CO_2 Separation from CO_2/CH_4 Mixture Gases

作　　者：臧小亚[1,2,3] 梁德青[1,2,3] 吴能友[4] ZANG Xiao-ya;LIANG De-qing;WU Neng-you(CAS Key Laboratory of Natural Gas Hydrate, CAS Key Laboratory of Renewable Energy,Guangzhou 510640, China;Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences,Guangzhou 510640, China;Guangdong Key Laboratory of New and Renewable Energy Research and Development, Guangzhou 510640, China;Qingdao Institute of Marine Geology, China Geological Survey,Qingdao 266000, China)

机构地区：[1]中科院天然气水合物重点实验室,中科院可再生能源重点实验室,广东广州510640 [2]中国科学院广州能源研究所,广东广州510640 [3]广东省新能源和可再生能源研究开发与应用重点实验室,广东广州510640 [4]中国地质调查局青岛海洋地质研究所,山东青岛266000

出　　处：《高校化学工程学报》2017年第4期802-809,共8页Journal of Chemical Engineering of Chinese Universities

基　　金：国家自然科学基金(51676197);国家海洋地质专项项目(GHZ2012006003);中国科学院知识创新工程重要方向项目(KGZD-EW-301);国家高技术研究发展计划项目(2012AA061403-03)

摘　　要：水合物法气体分离技术是一种新型的CO_2分离方法,不同的分离条件对CO_2气体分离的效果影响显著。四丁基溴化铵(TBAB)的添加能显著改善CO_2/CH_4混合气水合物的相平衡条件,促进CO_2水合物的生成。作者主要研究在质量浓度为40%的TBAB水溶液体系中,压力为3.2 MPa下,不同过冷度及气水比例的条件对CO_2/CH_4混合气水合物的生成过程及CO_2的分离效果的影响规律。实验结果表明,当压力为3.2 MPa时,气水比越小,CO_2分离效果越好。同时,存在最佳的过冷度使得反应过程中气体消耗量最大以及CO_2分离效果最好,而且CO_2分离效果并非与过冷度完全成正比。当气水比为0.54,过冷度为6 K时,反应结束后气相中CH_4的摩尔比例为81.59%,CO_2的摩尔比例为18.41%,CO_2气体分离系数为4.43,CO_2分离效果最好。Hydrate based gas separation(HBGS)technology is a relatively new approach for CO2removal.Different operation conditions can significantly influence CO2separation.Addition of tetrabutylammoniumbromide(TBAB)can reduce the hydrate phase equilibrium requirements of CO2/CH4mixture gases andenhance CO2hydrate formation.Gas hydrate formation from a CO2/CH4mixture in distilled water with40%mass fraction of TBAB was examined at3.2MPa and different temperatures.The results indicate that CO2separation factor increases with the decrease of gas/liquid ratio under same pressure and temperature.Meanwhile,CO2separation factor is not fully proportio(mol)at3.2MPa and286K(supercooling degree is6K)with a gas/liquid volume ratio(Vg/Vl)of0.54.CO2gas separation factor is4.43under this condition.

关 键 词：水合物 CO2分离 TBAB 半笼型 混合气 

分 类 号：TE64[石油与天然气工程—油气加工工程]