Investigation on methane recovery from low-concentration coal mine gas by tetra-n-butyl ammonium chloride semiclathrate hydrate formation
Investigation on methane recovery from low-concentration coal mine gas by tetra-n-butyl ammonium chloride semiclathrate hydrate formation
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四正丁基氯化铵半笼形水合物回收低浓度煤矿瓦斯甲烷的研究
DOI：
10.1016/j.apenergy.2017.08.069
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发表时间：
2017-08
期刊：
影响因子：
11.2
通讯作者：
Ding Kun
中科院分区：
文献类型：
--
作者：
Zhong Dong-Liang;Wang Wen-Chun;Zou Zhen-Lin;Lu Yi-Yu;Yan Jin;Ding Kun
本文研究了用四正丁基氯化铵(TBAC)水合物从低浓度的煤矿瓦斯中分离甲烷，该气体含有30%甲烷、60%氮和10%氧。测定并报道了在浓度为0.49%~3.3%的低浓度煤矿瓦斯存在下生成的TBAC水合物的相平衡数据。用高压差示扫描量热仪(HPµ-DSC)研究了矿用瓦斯中TBAC浓度固定为3.3%(TBAC半胶酸盐的化学计量浓度)时生成的TBAC半胶酸盐水合物的相行为。结果表明，在1.4~6.2℃的压力范围内，单一的TBAC半胶束水合物与TBAC-煤矿瓦斯混合水合物共存。此外，还进行了动力学实验，考察了TBAC浓度、过冷度和十二烷基硫酸钠(十二烷基硫酸钠)浓度对甲烷分离效率的影响，筛选出了以半水甘油为基础的甲烷回收的最佳实验条件。CH4的回收率和分离系数在0.49g/L的丁二酸丁二醇酯、T=8.8g/L、900g/L的十二烷基硫酸钠的条件下达到最大。结果表明，在0.49%TBAC和0.29%TBAB条件下得到的CH4回收率相当，而从TBAC水合物中释放出的混合气体的CH4浓度(49.6%)比在0.29%TBAB(42.5%)下的甲烷浓度有很大提高。
This work presents an investigation of using tetra-n-butyl ammonium chloride (TBAC) semiclathrate hydrate to separate CH4from a low-concentration coal mine gas containing 30 mol% CH4, 60 mol% N2, and 10 mol% O2. Phase equilibrium data of TBAC semiclathrate hydrate formed in the presence of low-concentration coal mine gas with TBAC concentration ranging from 0.49 mol% to 3.3 mol% were measured and reported. A high pressure micro-differential scanning calorimeter (HP µ-DSC) was employed to characterize the phase behaviors of TBAC semiclathrate hydrate formed in the presence of coal mine gas with TBAC concentration fixed at 3.3 mol% (the stoichiometric concentration of TBAC semiclathrate). It was found that pure TBAC semiclathrate hydrate coexists with the TBAC-coal mine gas mixed hydrate in the pressure range of (1.4–6.2 MPa). In addition, kinetic experiments were performed to elucidate the effects of TBAC concentration, subcooling, and sodium dodecyl sulfate (SDS) concentration on CH4separation efficiency and an optimum experimental condition for semiclathrate-based CH4recovery was screened. The highest CH4recovery and separation factor were obtained at the conditions of 0.49 mol% TBAC, △T= 8 K, and 900 ppm SDS. It was found that CH4recovery obtained at 0.49 mol% TBAC is comparable with that obtained at 0.29 mol% TBAB, whereas CH4concentration of the gas mixture released from the TBAC hydrate (49.6 mol%) is increased substantially comparing to that obtained at 0.29 mol% TBAB (42.5 mol%).
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