CH4 Gas Extraction by CO2: Substitution in Clathrate Hydrate through Bimolecular Iteration

doi:10.1088/0256-307X/37/4/048201

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	CH4 Gas Extraction by CO2: Substitution in Clathrate Hydrate through Bimolecular Iteration
	Yu, Xiao-Hui ; Liu, Yuan ; Du, San-Ya ; Zheng, Xu ; Zhu, Jin-Long ; Xu, Hong-Wu ; Zhang, Jian-Zhong ; Du, Shi-Yu ; Zeng, Xiao-Cheng ; Francisco, J. S.
刊名	CHINESE PHYSICS LETTERS
	2020
卷号	37 期号:4
关键词	CARBON-DIOXIDE METHANE HYDRATE REPLACEMENT STORAGE
DOI	10.1088/0256-307X/37/4/048201
英文摘要	Methane clathrate hydrate (MCH) is a promising energy resource, but controllable extraction of CH4 from MCH remains a challenge. Gradually replacing CH4 in MCH with CO2 is an attractive scheme, as it is cost efficient and mitigates the environmentally harmful effects of CO2 by sequestration. However, the practicable implementation of this method has not yet been achieved. In this study, using in situ neutron diffraction, we confirm that CH4 in the 5(12)6(2) cages of bulk structure-I (sI) MCH can be substituted by gaseous CO2 under high pressure and low temperature with a high substitution ratio (similar to 44%) while conserving the structure of the hydrate framework. First-principles calculations indicate that CO2 binds more strongly to the 5(12)6(2) cages than methane does, and that the diffusion barrier for CH4 is significantly lowered by an intermediate state in which one hydrate cage is doubly occupied by CH4 and CO2. Therefore, exchange of CO2 for CH4 in MCH is not only energetically favorable but also kinetically feasible. Experimental and theoretical studies of CH4/CO2 substitution elucidate a method to harness energy from these combustible ice resources.
学科主题	Physics
内容类型	期刊论文
源URL	[http://ir.nimte.ac.cn/handle/174433/19820]
专题	2020专题
作者单位	1.Zhu, JL 2.Zhao, YS (corresponding author), Southern Univ Sci & Technol SUSTech, Dept Phys, Shenzhen 518055, Peoples R China. 3.Li, H (corresponding author), Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China. 4.Zhu, JL (corresponding author), Ctr High Pressure Sci & Technol Adv Res HPSTAR, Beijing 100094, Peoples R China.
推荐引用方式 GB/T 7714	Yu, Xiao-Hui,Liu, Yuan,Du, San-Ya,et al. CH4 Gas Extraction by CO2: Substitution in Clathrate Hydrate through Bimolecular Iteration[J]. CHINESE PHYSICS LETTERS,2020,37(4).
APA	Yu, Xiao-Hui.,Liu, Yuan.,Du, San-Ya.,Zheng, Xu.,Zhu, Jin-Long.,...&Li, Hui.(2020).CH4 Gas Extraction by CO2: Substitution in Clathrate Hydrate through Bimolecular Iteration.CHINESE PHYSICS LETTERS,37(4).
MLA	Yu, Xiao-Hui,et al."CH4 Gas Extraction by CO2: Substitution in Clathrate Hydrate through Bimolecular Iteration".CHINESE PHYSICS LETTERS 37.4(2020).