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