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Ternary Sn-Ti-O Electrocatalyst Boosts the Stability and Energy Efficiency of CO2 Reduction |
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| Authors: | Dr Guobin Wen Dr Bohua Ren Dr Moon G Park Dr Jie Yang Dr Haozhen Dou Dr Zhen Zhang Dr Ya-Ping Deng Prof Zhengyu Bai Prof Lin Yang Prof Jeff Gostick Prof Gianluigi A Botton Prof Yongfeng Hu Prof Zhongwei Chen |
| Institution: | 1. School of Chemistry and Chemical Engineering, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, Xinxiang, 453007 China
Department of Chemical Engineering, Waterloo Institute for Nanotechnology, Waterloo Institute for Sustainable Energy, University of Waterloo, Waterloo, Ontario, N2L 3G1 Canada These authors contributed equally to this work.;2. Department of Chemical Engineering, Waterloo Institute for Nanotechnology, Waterloo Institute for Sustainable Energy, University of Waterloo, Waterloo, Ontario, N2L 3G1 Canada These authors contributed equally to this work.;3. Department of Chemical Engineering, Waterloo Institute for Nanotechnology, Waterloo Institute for Sustainable Energy, University of Waterloo, Waterloo, Ontario, N2L 3G1 Canada;4. Department of Materials Science and Engineering and Canadian Centre for Electron Microscopy, McMaster University, 1280 Main Street West, Hamilton, Ontario, L8S 4M1 Canada;5. School of Chemistry and Chemical Engineering, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, Xinxiang, 453007 China;6. Department of Materials Science and Engineering and Canadian Centre for Electron Microscopy, McMaster University, 1280 Main Street West, Hamilton, Ontario, L8S 4M1 Canada Canadian Light Source, University of Saskatchewan, Saskatoon, Saskatchewan, S7N 0X4 Canada;7. Canadian Light Source, University of Saskatchewan, Saskatoon, Saskatchewan, S7N 0X4 Canada |
| Abstract: | Simultaneously improving energy efficiency (EE) and material stability in electrochemical CO2 conversion remains an unsolved challenge. Among a series of ternary Sn-Ti-O electrocatalysts, 3D ordered mesoporous (3DOM) Sn0.3Ti0.7O2 achieves a trade-off between active-site exposure and structural stability, demonstrating up to 71.5 % half-cell EE over 200 hours, and a 94.5 % Faradaic efficiency for CO at an overpotential as low as 430 mV. DFT and X-ray absorption fine structure analyses reveal an electron density reconfiguration in the Sn-Ti-O system. A downshift of the orbital band center of Sn and a charge depletion of Ti collectively facilitate the dissociative adsorption of the desired intermediate COOH* for CO formation. It is also beneficial in maintaining a local alkaline environment to suppress H2 and formate formation, and in stabilizing oxygen atoms to prolong durability. These findings provide a new strategy in materials design for efficient CO2 conversion and beyond. |
| Keywords: | carbon dioxide fixation electrochemistry interfaces materials science mesoporous materials |