文献类型：期刊文献

英文题名：Development of a Density Functional Theory in Three-Dimensional Nanoconfined Space: H₂ Storage in Metal-Organic Frameworks

作者：Liu, Yu[1,2,3];Liu, Honglai[1,2];Hu, Ying[1,2];Jiang, Jianwen[3]

机构：[1]E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]E China Univ Sci & Technol, Dept Chem, Shanghai 200237, Peoples R China;[3]Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore 117576, Singapore

年份：2009

卷号：113

期号：36

起止页码：12326

外文期刊名：JOURNAL OF PHYSICAL CHEMISTRY B

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000269655300021)】；

基金：This work was supported by the National University of Singapore (R279-000-243-123), the National Natural Science Foundation of China (No. 20736002), the creative learn development project of Ministry of Education of China (No. IRT0721), and the 111 Project of Ministry of Education of China (No. B08021).

语种：英文

摘要：A density functional theory (DFT) is developed in three-dimensional nanoconfined space and applied for H-2 storage in metal-organic frameworks. Two different weighting functions based on the weighted density approximation (WDA) are adopted, respectively, for the repulsive and attractive contributions to the excess free energy. The Carnahan-Starling equation and a modified Benedicit-Webb-Rubin equation are used to calculate the excess free energy of uniform fluid. To compare with DFT predictions, grand canonical Monte Carlo simulations are carried out separately. For H-2 adsorption in MOF-5 and ZIF-8, the isotherms predicted from the DFT agree well with simulation and experiment results, and the DFT is found to be superior to the mean-field-approximation (MFA)-based theory. The adsorption energies and isosteric heats predicted are also in accord with simulation results. From the predicted density contours, the DFT shows that the preferential adsorption sites are the corners of metal clusters in MOF-5 and the top of organic linkers in ZIF-8, consistent with simulation and experimental observations.