Efficient dry reforming of methane realized by photoinduced acceleration of oxygen migration rate

Abstract

Methane dry reforming (DRM) can consume greenhouse gases (CH₄ and CO₂) to produce valuable Fischer-Tropsch syngas (CO and H₂). However, conventional thermally driven DRM consume large amounts of energy and face problems such as catalyst sintering and carbon deposition leading to insufficient catalytic activity. In this study, a photothermal synergistic TiO₂/CeO₂/Ru catalyst with high efficiency was designed. Under the light condition, the yields of H₂ and CO reached 496.3 mmol g⁻¹ h⁻¹ and 522.4 mmol g⁻¹ h⁻¹, respectively. In addition, the catalyst demonstrated excellent stability after 100 h cyclic stability test. In-situ X-ray photoelectron spectroscopy (IS-XPS) and density functional theory (DFT) calculations revealed that the heterojunction interface formed by TiO₂/CeO₂/Ru is favourable for capturing photogenerated electrons and suppressing the recombination rate of photons and holes, thus improving the photocatalytic performance. Furthermore, light-induced metal-to-metal charge transfer (MMCT) accelerated oxygen migration, which not only improved the catalytic activity, but also suppressed the formation of carbon deposits on the catalyst surface, thereby enhancing the cycling stability. This study explores the mechanism of photothermally synergistic DRM, which provides a new pathway for the efficient use of solar energy.