1. Photocatalytic Coupling of CH4 and CO2 to Ethanol on Asymmetric Ce-O-Zn Sites.
- Author
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Shuya Hao, Yangshen Chen, Chen Peng, Huining Wang, Qianyou Wen, Cejun Hu, Lijuan Zhang, Qing Han *, and Gengfeng Zheng *
- Subjects
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ASYMMETRIC synthesis , *CERIUM oxides , *STEAM reforming , *ELECTRON paramagnetic resonance - Abstract
Partial oxidation of methane (CH4) to value-added products is significantly challenging due to the highly inert chemical property of CH4 at ambient conditions and easy over-oxidation into carbon dioxide (CO2) or carbon monoxide (CO) at elevated temperatures and pressures. Targeting this challenge, the efficient photocatalytic coupling of CO2 and CH4 into ethanol is demonstrated, using a cerium (Ce)-doped zinc oxide (ZnO) photocatalyst with abundant Ce--O--Zn units. Under light illumination, CO2 is adsorbed on the Ce atoms and photo-reduced to CO, and CH4 is captured by the Zn atoms and photo-oxidized to hydroperoxymethane (CH3OOH). The close proximity of Ce and Zn atoms on the Ce--O--Zn units allowed to further efficiently couple the as-formed CO and CH3OOH into ethanol. Without additional Oxygen (O2) oxidant or sacrificial regent, the ethanol production rate reached 580 µmol g-1 h-1, substantially exceeding previously reports on photocatalytic CH4 oxidation. This work features to convert two greenhouse gases into value-added chemicals with adjacent and asymmetric reaction sites, suggesting attractive potentials for CH4 and CO2 utilization. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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