Role of interfacial oxygen vacancies in low-loaded Au-based catalysts for the low-temperature reverse water gas shift reaction

Abstract

Gold-based catalysts have shown high catalytic activity for reverse water gas shift (RWGS) reactions at low temperatures. Despite extensive studies, the RWGS reaction on Au-based catalysts with very low Au content (< 0.1 wt%) has not yet been investigated. In this study, TiO2 and ZrO2 supported gold catalysts with such low gold loading have been synthesized and tested for RWGS. The catalysts were investigated by a series of in/ex-situ characterization techniques, including ICP-OES, XRD, BET, XPS, STEM, STEM-EELS, TAP, in-situ DRIFTS and in-situ EPR. At 250 oC, the Au/TiO2 catalyst showed almost 10 times higher activity than Au/ZrO2. In-situ DRIFTS results suggest that the formate mechanism is the predominant mechanism over Au/ZrO2, while over Au/TiO2 the reaction proceeds via the formation of hydroxycarbonyl intermediates. A combined study including STEM, STEM-EELS, XPS, and in-situ EPR suggests that the interfacial Au–Ov–Ti3+ sites are responsible for the superior activity of Au/TiO2.