Hole-Mediated Hydrogen Spillover Mechanism in Metal-Organic Frameworks

作     者：Kyuho Lee Yong-Hyun Kim Y. Y. Sun D. West Yufeng Zhao Zhongfang Chen S. B. Zhang 

作者机构：Department of Physics Applied Physics and Astronomy Rensselaer Polytechnic Institute Troy New York 12180 USA National Renewable Energy Laboratory Golden Colorado 80401 USA Graduate School of Nanoscience and Technology (WCU) Korea Advanced Institute of Science and Technology Daejeon 305-701 Korea Department of Chemistry Institute for Functional Nanomaterials University of Puerto Rico San Juan Puerto Rico 00931 

出 版 物：《Physical Review Letters》 (Phys Rev Lett)

年 卷 期：2010年第104卷第23期

页      面：236101-236101页

核心收录：

学科分类：07[理学] 0702[理学-物理学] 

基　　金：DOE/OS/BES DOE/EERE [DE-AC36-08GO28308, J30546/J90336] NSF [CHE-0716718] Institute for Functional Nanomaterials (NSF) NRFK [R31-2008-000-10071-0] 

主　　题：Gibbs free energy 

摘      要：Hydrogen spillover on carbon-based systems has been proposed as a viable alternative for room-temperature storage. Given the strength of the C-H bonds, however, it is unclear if spillover indeed takes place in such materials. We performed a first-principles study of H spillover on IRMOF-1. Spillover becomes thermodynamically stable only at high H coverage with a calculated Gibbs free energy of −14 kJ/mol at ambient condition. In general, however, spillover may not proceed due to high-energy states at lower H coverage. We propose that hole doping can substantially lower the energies as well as barriers to enable spillover at ambient conditions.