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Light‐Induced Redox Looping of a Rhodium/Ce<sub><i>x</i></sub>WO<sub>3</sub> Photocatalyst for Highly Active and Robust Dry Reforming of Methane

Yuying Yang, Zhigang Chai, Xuetao Qin, Zhenzhen Zhang, Aidaer Muhetaer, Cong Wang, Hanlin Huang, Chaoran Yang, Ding Ma, Qi Li, Dongsheng Xu

2022Angewandte Chemie International Edition124 citationsDOI

Abstract

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.

Topics & Concepts

PhotocatalysisMethaneSyngasRedoxCatalysisPhotochemistryQuantum efficiencyRhodiumChemistryMaterials scienceChemical looping combustionChemical engineeringNanotechnologyOxygenInorganic chemistryOptoelectronicsOrganic chemistryEngineeringAdvanced Photocatalysis TechniquesCatalytic Processes in Materials ScienceAmmonia Synthesis and Nitrogen Reduction
Light‐Induced Redox Looping of a Rhodium/Ce<sub><i>x</i></sub>WO<sub>3</sub> Photocatalyst for Highly Active and Robust Dry Reforming of Methane | Litcius