Description:
Pt-based catalysts are widely used for hydrogen production from methanol steam reforming (MSR), but the reaction mechanism is not well understood. In the paper, the reaction pathways of MSR on Pt(111) surface are systemically studied by using density functional theory and Kinetic Monte Carlo. Methanol direct decomposition via CHOH* and CHO* intermediates is the main reaction pathway at 373 ~ 623 K and 1 atm with 1:1 CH 3 OH:H 2 O, and the surface is covered by CO at low reaction temperature. Low feed ratio of CH 3 OH/H 2 O, small energy barriers of water scission and CO oxidation are in favor of CO coverage decreasing, and small energy barriers of bi-CHOO* → mono-CHOO* is beneficial to high TOF of H 2 . In general, efficient Pt-based catalysts for MSR should have high water dissociation, CO oxidation and CHOO decomposition capacity. These results may be useful for design and optimization of Pt-based catalysts at low temperature for MSR reaction