Dual Lewis Acid-Base Sites Regulate Silver-Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane |
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Authors: | Shimao Deng Ranhao Wang Xuezhen Feng Dr. Renji Zheng Shaokuan Gong Prof. Xihan Chen Yangzi Shangguan Lili Deng Huan Tang Hao Dai Prof. Lele Duan Prof. Chengyuan Liu Prof. Yang Pan Prof. Hong Chen |
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Affiliation: | 1. State Environmental Protection Key Laboratory of Integrated Surface Water Groundwater Pollution Control, Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control, Key Laboratory of Municipal Solid Waste Recycling Technology and Management of Shenzhen City, Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials (SKLISEM), School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055 China;2. SUSTech Energy Institute for Carbon Neutrality, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055 China;3. Department of Chemistry, Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Southern University of Science and Technology, Shenzhen, 518055 China;4. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 China |
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Abstract: | Highly selective photoreduction of CO2 to valuable hydrocarbons is of great importance to achieving a carbon-neutral society. Precisely manipulating the formation of the Metal1⋅⋅⋅C=O⋅⋅⋅Metal2 (M1⋅⋅⋅C=O⋅⋅⋅M2) intermediate on the photocatalyst interface is the most critical step for regulating selectivity, while still a significant challenge. Herein, inspired by the polar electronic structure feature of CO2 molecule, we propose a strategy whereby the Lewis acid-base dual sites confined in a bimetallic catalyst surface are conducive to forming a M1⋅⋅⋅C=O⋅⋅⋅M2 intermediate precisely, which can promote selectivity to hydrocarbon formation. Employing the Ag2Cu2O3 nanowires with abundant Cu⋅⋅⋅Ag Lewis acid-base dual sites on the preferred exposed {110} surface as a model catalyst, 100 % selectivity toward photoreduction of CO2 into CH4 has been achieved. Subsequent surface-quenching experiments and density functional theory (DFT) calculations verify that the Cu⋅⋅⋅Ag Lewis acid-base dual sites do play a vital role in regulating the M1⋅⋅⋅C=O⋅⋅⋅M2 intermediate formation that is considered to be prone to convert CO2 into hydrocarbons. This study reports a highly selective CO2 photocatalyst, which was designed on the basis of a newly proposed theory for precise regulation of reaction intermediates. Our findings will stimulate further research on dual-site catalyst design for CO2 reduction to hydrocarbons. |
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Keywords: | Ag⋅⋅⋅C=O⋅⋅⋅Cu Intermediate Lewis Acid-Base Dual Sites Methane Selective Reduction |
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