摘要
Recently,a new phase C'_(1) H_(2) hydrate was experimentally identified.In this work,the diffusive behaviors of H_(2) in C'_(1)phase clathrate hydrate are explored using classic molecular dynamics(MD)simulations.It reveals that the cage occupancy by H_(2) molecule negligibly influences the C'_(1) phase clathrate structure but greatly dictates the diffusion coefficient of H_(2)molecule.Due to the small cage size and small windows connecting the neighboring cages in C'_(1) phase clathrate,nonoccupancy of the neighboring cages is demanded to enable the diffusion of H_(2) molecule that is primarily dominated by hopping mechanism.Moreover,the analysis of diffusive free energy landscape reveals lower energy barrier of H_(2) molecule in C'_(1) phase clathrate hydrate than that of other gases in conventional clathrate hydrates,and that H_(2) molecule travels through the windows between neighboring cages with preferential molecular orientation.This study provides critical physical insights into the diffusion behaviors of H_(2) in the C'_(1) phase clathrate hydrate,and implies that the C'_(1) clathrate hydrate is a promising solid structure for the next-generation H_(2) storage.
作者
宋姿璇
周子岳
林演文
石桥
郝勇超
付越群
张志森
吴建洋
Zixuan Song;Ziyue Zhou;Yanwen Lin;Qiao Shi;Yongchao Hao;Yuequn Fu;Zhisen Zhang;Jianyang Wu(Department of Physics,Research Institute for Biomimetics and Soft Matter,Jiujiang Research Institute and Fujian Provincial Key Laboratory for Soft Functional Materials Research,Xiamen University,Xiamen 361005,China;PoreLab,the Njord Centre,Department of Physics,University of Oslo,Oslo 0313,Norway;NTNU Nanomechanical Laboratory,Norwegian University of Science and Technology(NTNU),Trondheim 7491,Norway)
基金
Project supported by the National Natural Science Foundation of China(Grant Nos.12172314,11772278,and 11904300)
the Jiangxi Provincial Outstanding Young Talents Program(Grant No.20192BCBL23029)
the Fundamental Research Funds for the Central Universities(Xiamen University:Grant Nos.20720210025 and 20720220023)
the Research Council of Norway(Grant No.262644)
the 111 project(Grant No.B16029)。
