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过程工程学报 ›› 2017, Vol. 17 ›› Issue (4): 873-878.DOI: 10.12034/j.issn.1009-606X.216336

• 环境与能源 • 上一篇    下一篇

季铵盐对煤层气水合物相平衡条件的影响

郭 迎, 梁海峰*, 关 钰, 贺博   

  1. 太原理工大学化学化工学院,山西 太原 030024
  • 收稿日期:2016-10-26 修回日期:2017-01-03 出版日期:2017-08-20 发布日期:2017-08-16
  • 通讯作者: 梁海峰
  • 基金资助:
    基于孔隙网络模型的天然气水合物分解特性模拟研究;基于孔隙网络模型的CO2驱替煤层CH4机理研究

Effect of Quaternary Ammonium Salts on Phase Equilibrium Condition of Coal Mine Methane Gas Hydrate

Ying GUO,  Haifeng LIANG*,  Yu GUAN,  Bo HE   

  1. College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan, Shanxi 030024, China
  • Received:2016-10-26 Revised:2017-01-03 Online:2017-08-20 Published:2017-08-16

摘要: 对四甲基氟化铵(TMAF)、四甲基氯化铵(TMAC)、四甲基溴化铵(TMAB)、四丁基氟化铵(TBAF)和四丁基氯化铵(TBAC)五种季铵盐在低浓度含氧煤层气[30% CH4+65% N2+5% O2 (mol)]中形成水合物的热力学促进作用进行了实验研究,采用恒容压力搜索法得到每种季铵盐在浓度0.17%, 0.29%, 0.62%, 1.38%, 3.5%(mol)、温度282.3~304.5 K、压力0.919~8.435 MPa条件下的水合物相平衡数据. 从季铵盐浓度、季铵盐卤素离子种类及季铵盐烷基种类3个方面综合比较了5种季铵盐的热力学促进效果. 结果表明,5种季铵盐均能改善煤层气水合物形成的热力学条件,最佳促进效果3.5% TBAF>0.62% TMAF>3.5% TBAC>1.38% TMAB>1.38% TMAC,季铵盐卤素离子的促进作用氟离子>氯离子或溴离子,季铵盐烷基的影响丁基>甲基.

关键词: 水合物, 煤层气, 季铵盐, 热力学, 相平衡

Abstract: The thermodynamic effects were researched in hydrate formation experiments for low-concentration coal mine methane gas (CMM , the mole fraction is 30% CH4, 65% N2, and 5% O2) with five kinds of quaternary ammonium salts (QASs) including tetramethyl ammonium fluoride (TMAF), tetramethyl ammonium chloride (TMAC), tetramethyl ammonium bromide (TMAB) and tetrabutyl ammonium fluoride (TBAF), tetrabutyl ammonium chloride (TBAC). The molar concentration of each quaternary ammonium salt was 0.17%, 0.29%, 0.62%, 1.38%, and 3.5%. Under the conditions of phase equilibrium temperature from 282.3 to 304.5 K. Phase equilibrium pressure changed from 0.919 to 8.435 MPa, an isochoric pressure-search method was used to obtain the phase equilibrium data. Comparing the thermodynamic promoting effects of these five kinds of QASs from three aspects: concentration, species of halogen ion and species of alkyl in quaternary ammonium salts. The results showed that these QASs can improve the thermodynamic condition of CMM hydrate formation, the order of the best promoting effects about the three aspects was 3.5% TBAF>0.62% TMAF>3.5% TBAC>1.38% TMAB>1.38% TMAC, fluorine ion quaternary ammonium salts>chloride quaternary ammonium salts or bromide ion quaternary ammonium salts and tetrabutyl quaternary ammonium salts>tetramethyl quaternary ammonium salts.

Key words: hydrate, coal mine methane gas, quaternary ammonium salt, thermodynamics, phase equilibrium