Density functional theory study of acetic acid steam reforming on Ni(111)

Abstract

Catalytic steam reforming of bio-oil is a promising process to convert biomass into hydrogen. To shed light on this process, acetic acid is selected as the model compound of the oxygenates in bio-oil, and density functional theory is applied to investigate the mechanism of acetic acid steam reforming on the Ni(111) surface. The most favorable pathway of this process on the Ni(111) surface is suggested as CH3COOH*→CH3COO*→CH3CO*→CH2CO*→CH2*+CO*→CH*→CHOH*→CHO*→CO*, followed by the water gas shift reaction to produce CO2 and H2. CH* species are identified as the major carbon deposition precursor, and the water gas shift reaction is the rate-determining step during the whole acetic acid steam reforming process, as CO*+OH*→cis-COOH* is kinetically restricted with the highest barrier of 1.85eV. Furthermore, the formation pathways and initial dissociation of important intermediates acetone and acetaldehyde are also investigated.