Comprehensive Mechanism for CO Electroreduction on Dual-Atom-Catalyst-Anchored N-Doped Graphene |
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Authors: | Di Liu Jia Zhao Youchao Kong Haoqiang Ai Haoyun Bai Chon Chio Leong Kin Ho Lo Shuangpeng Wang Weng Fai Ip Sen Lin Hui Pan |
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Institution: | 1. Institute of Applied Physics and Materials Engineering, University of Macau, Macao SAR, China;2. State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002 China;3. Department of Electromechanical Engineering, Faculty of Science and Technology, University of Macau, Macao SAR, China;4. Department of Electrical and Computer Engineering, Faculty of Science and Technology, University of Macau, Macao SAR, China;5. Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao SAR, China |
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Abstract: | Carbon neutrality has drawn increasing attention for realizing the carbon cyclization and reducing the greenhouse effect. Although the C1 products, such as CO, can be achieved with a high Faraday efficiency, the targeted production of C2 fuels as well as the mechanism have not been systematically investigated. In this work, we carry out a first-principles study to screen dual-atom catalysts (DACs) for producing C2 fuels through the electrocatalytic carbon monoxide reduction reaction (e-CORR). We find that methanol, ethanol and ethylene can be produced on both DAC?Co and DAC?Cu, while acetate can be achieved on DAC?Cu only. Importantly, methanol and ethylene are preferred on DAC?Co, while acetate and ethylene on DAC?Cu. Furthermore, we show that the explicit solvent can enhance the adsorption and influence the protonation steps, which subsequently affects the protonation and dimerization behavior as well as the performance and selectivity of e-CORR on DACs. We further demonstrate that the C?C coupling is easy to be formed and stabilized if the Integrated Crystal Orbital Hamilton Population (ICOHP) is low because of the low energy barrier. Our findings provide not only guidance on the design of novel catalysts for e-CORR, but an insightful understanding on the reduction mechanism. |
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Keywords: | C2 products DACs-anchored graphene DFT calculations e-CORR explicit solvent model |
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