title: Hole-mediated hydrogen spillover mechanism in metal-organic frameworks.
abstract: 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.
authors.affiliation: Department of Physics, Applied Physics and Astronomy, Rensselaer Polytechnic Institute, Troy, New York 12180, USA.
authors.forename: Kyuho
authors.initials: K
authors.lastname: Lee
authors.forename: Yong-Hyun
authors.initials: YH
authors.lastname: Kim
authors.forename: Y Y
authors.initials: YY
authors.lastname: Sun
authors.forename: D
authors.initials: D
authors.lastname: West
authors.forename: Yufeng
authors.initials: Y
authors.lastname: Zhao
authors.forename: Zhongfang
authors.initials: Z
authors.lastname: Chen
authors.forename: S B
authors.initials: SB
authors.lastname: Zhang