Light‐Induced Redox Looping of a Rhodium/CexWO3 Photocatalyst for Highly Active and Robust Dry Reforming of Methane. Issue 21 (23rd March 2022)

• Record Type: Journal Article
• Authors: Yang, Yuying; Chai, Zhigang; Qin, Xuetao; Zhang, Zhenzhen; Muhetaer, Aidaer; Wang, Cong; Huang, Hanlin; Yang, Chaoran; Ma, Ding; Li, Qi; Xu, Dongsheng
• Is Part Of: Angewandte Chemie international edition. Volume 61:Issue 21(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-03-23
• Subjects: Dry Reforming of Methane -- Metal-to-Metal Charge Transfer -- Oxygen Migration -- Photocatalysis; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202200567
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Dry reforming of methane (DRM) has provided an effective avenue to convert two greenhouse gases, CH4 and CO2, into syngas. Here, we design a DRM photocatalyst Rh/Ce x WO3 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 WO3, 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. Abstract : A photocatalyst for dry reforming of methane, Rh/Ce x WO3, invokes both photothermal and photoelectric activation processes. Light‐induced metal‐to‐metal charge transfer takes place in the photocatalyst, which induces a redox looping between Ce to W species. High oxygen mobility of Ce x WO3, accompanied with the formation of oxo‐bridge species, results in a substantial elimination of deposited C species during the reaction.