高等学校化学学报2024，Vol.45Issue(1)：67-76,10.DOI:10.7503/cjcu20230383
二元包合水合物储氢及促进剂作用的理论研究
Theoretical Study on Hydrogen Storage and Promoter Effect of Binary Clathrate Hydrates
摘要
Abstract
Although clathrate hydrates(CHs)can be used as potential hydrogen storage materials for large-scale industrial applications due to their high energy storage density and environmental friendliness,major gaps in the understanding of the structures and diffusion of hydrogen gas in CHs remain.Here,we theoretically explored the hydrogen storage structure and properties of type Ⅰ CHs using density functional theory(DFT)calculations.The results show that up to two H2 molecules can be occupied in the 512 cages of the CHs,and the CH4 and C2H6 promoters have no significant effect on its structure and properties.However,inclusion of the N2 and CO2 promoters in the CHs cages could considerably change the structures and properties including the number of H2 molecules occupied in the 512 cages increased to three,stability increase,the host-guest electrostatic and hydrogen bonding interactions enhance,and the H—H stretching blue-shifts of the H2 molecules.Moreover,when hydrogen occupies up to three H2 molecules in the 512 cages of N2 and CO2 CHs,calculated energy barriers for one H2 molecule migration through the pentagonal surface are close to twice that of pure hydrogen CHs,effectively hindering the diffusion of hydrogen between the cages.关键词
包合水合物/储氢/稳定性/扩散/促进剂作用Key words
Clathrate hydrates/Hydrogen storage/Stability/Diffusion/Promoter effect分类
化学化工引用本文复制引用
张宏淑,梁攀,薛颖颖,韦瑶瑶..二元包合水合物储氢及促进剂作用的理论研究[J].高等学校化学学报,2024,45(1):67-76,10.基金项目
国家自然科学基金(批准号:22003035)和陕西省教育厅项目(批准号:22JK0334)资助.Supported by the National Natural Science Foundation of China(No.22003035)and the Shaanxi Provincial Education Department Project,China(No.22JK0334). （批准号:22003035）
