First principles study on the origin of the different selectivity for methanol steam reforming on Cu(111) and Pd(111)

摘要

Methanol steam reforming (MSR) is an important industrial process for hydrogen production, and fundamental understanding of the reaction mechanism is crucial to improve the catalytic activity and selectivity. Despite of the numerous investigations on the MSR reaction, the controversy remains, and a number of mechanisms including methanol decomposition followed by water gas shift reaction, mechanism via methyl formate or formaldehyde, have been proposed. Experimentally, the remarkable different CO2 selectivity of the MSR reaction over supported copper and group VIII metals have been reported too. Theoretically, to best of our knowledge, detailed mechanistic study on the activity and selectivity of the whole MSR reaction on Cu and Pd and the origin of their different selectivity are not available yet. To shed light on the activity and selectivity of the overall MSR reaction, we present here a detailed density functional theory study of the MSR reaction mechanism on Cu(111) and Pd(111) surfaces.