Preferential enclathration of CO2 into tetra-n-butyl phosphonium bromide semiclathrate hydrate in moderate operating conditions: Application for CO2 capture from shale gas

Preferential enclathration of CO2 into tetra-n-butyl phosphonium bromide semiclathrate hydrate in moderate operating conditions: Application for CO2 capture from shale gas
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在温和的操作条件下,CO2 优先包合为四正丁基溴化鏻半笼形水合物:页岩气 CO2 捕集应用

DOI:
10.1016/j.apenergy.2017.05.043
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发表时间:
2017-08
期刊:
影响因子:
11.2
通讯作者:
Zou Zhen-Lin
Zou Zhen-Lin
中科院分区:
工程技术1区
文献类型:
--
作者:
Li Zheng;Zhong Dong-Liang;Lu Yi-Yu;Yan Jin;Zou Zhen-Lin

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采用四正丁基溴化鏻(TBPB)半笼状水合物从CO2和CH 4摩尔分数分别为40%和60%的模拟页岩气中捕集CO2。实验在搅拌釜式反应器中进行,TBPB的质量分数(wTBPB)从5.0%变化到33.2%。测定了TBPB半笼状水合物在40%CO2/CH 4混合气体中的相平衡数据。在278.1- 284.2K温度范围内,研究了TBPB浓度对气体溶解度、水合物生成动力学和CO2分离效率的影响。结果表明,在一定的驱动力(超压)下,尽管TBPB浓度不同,诱导期气体的吸收量基本不变,而水合物的生成速率随着TBPB浓度的增加而增加。结果表明,与THF摩尔分数为1%时相比,TBPB化学计量浓度(wTBPB= 33.2%)时水合物生成动力学增强,CO2分离因子(31.7 ± 3.3)和操作温度(284.2K)提高。因此,TBPB可作为水合物法捕集模拟页岩气(CO2/CH 4混合气)中CO2的促进剂。
This work presents an investigation of using tetra-n-butyl phosphonium bromide (TBPB) semiclathrate hydrate for CO2capture from simulated shale gas that is composed of 40% CO2and 60% CH4in mole fraction. The experiments were performed in a stirred tank reactor with the mass fraction of TBPB (wTBPB) varying from 5.0% to 33.2%. The phase equilibrium data of TBPB semiclathrate hydrate formed in the presence of the 40% CO2/CH4gas mixture were measured and reported. The effects of TBPB concentration on gas solubility, hydrate formation kinetics, and CO2separation efficiency were investigated in the temperature range of 278.1–284.2 K with the initial pressure fixed at 2.8 MPa. The results indicated that at a fixed driving force (overpressure), the gas uptake obtained at the induction time was nearly constant, despite the variation in TBPB concentration, while the rate of hydrate formation increased with the increase in TBPB concentration. Compared to the results obtained at a mole fraction of 1% THF, it was found that enhanced hydrate formation kinetics, a higher CO2separation factor (31.7 ± 3.3), and a higher operating temperature (284.2 K) were obtained at the stoichiometric TBPB concentration (wTBPB= 33.2%). Therefore, TBPB may be used as a promising promoter for hydrate-based CO2capture from the simulated shale gas (CO2/CH4gas mixture).
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