Light‐Induced Redox Looping of a Rhodium/CexWO3 Photocatalyst for Highly Active and Robust Dry Reforming of Methane

Abstract Dry reforming of methane (DRM) has provided an effective avenue to convert two greenhouse gases, CH 4 and CO 2 , into syngas. Here, we design a DRM photocatalyst Rh/Ce x WO 3 that invokes both photothermal and photoelectric processes, which overcomes the thermodynamic limitation of DRM under conventional conditions. In contrast to plasmonic or UV‐response photocatalysts, our photocatalyst produces a superior light‐to‐chemical energy efficiency (LTCEE) of 4.65 % with a moderate light intensity. We propose that a light‐induced metal‐to‐metal charge transfer plays a crucial role in the DRM reaction, which induces a redox looping between Ce to W species to lower the activation energy. Quantum mechanical studies reveal that a high oxygen mobility of Ce x WO 3 , accompanied with the formation of oxo‐bridge species, results in a substantial elimination of deposited C species during the reaction. Our catalyst design strategy could offer a promising energy‐efficient industrial process for DRM.