Promoting Water Activation via Molecular Engineering Enables Efficient Asymmetric C–C Coupling during CO2 ElectroreductionClick to copy article linkArticle link copied!
- Zi-Yu DuZi-Yu DuState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Zi-Yu Du
- Si-Bo LiSi-Bo LiState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Si-Bo Li
- Ge-Hao LiangGe-Hao LiangState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Ge-Hao Liang
- Yi-Meng XieYi-Meng XieState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Yi-Meng Xie
- Yao-Lin AYao-Lin AState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Yao-Lin A
- Yi ZhangYi ZhangState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Yi Zhang
- Hua Zhang*Hua Zhang*Email: [email protected]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Hua Zhang
- Jing-Hua TianJing-Hua TianInnovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361005, ChinaMore by Jing-Hua Tian
- Shisheng Zheng*Shisheng Zheng*Email: [email protected]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Shisheng Zheng
- Qing-Na ZhengQing-Na ZhengState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Qing-Na Zheng
- Zhou Chen*Zhou Chen*Email: [email protected]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaMore by Zhou Chen
- Weng Fai IpWeng Fai IpDepartment of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao 999078, ChinaMore by Weng Fai Ip
- Jinxuan Liu*Jinxuan Liu*Email: [email protected]State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116024, P. R. ChinaLeicester International Institute, Dalian University of Technology, Panjin 124221, P. R. ChinaMore by Jinxuan Liu
- Jian-Feng Li*Jian-Feng Li*Email: [email protected]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Materials, iChEM, Fujian Key Laboratory of Advanced Materials, College of Energy, Institute of Artificial Intelligence, Xiamen University, Xiamen 361005, ChinaInnovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361005, ChinaCollege of Chemistry, Chemical Engineering and Environment, Minnan Normal University, Zhangzhou 363000, ChinaMore by Jian-Feng Li
Abstract

Water activation plays a crucial role in CO2 reduction, but improving the electrocatalytic performance through controlled water activation presents a significant challenge. Herein, we achieved electrochemical CO2 reduction to ethene and ethanol with high selectivity by promoting water dissociation and asymmetric C–C coupling by engineering Cu surfaces with N–H-rich molecules. Direct spectroscopic evidence, coupled with density functional theory calculations, demonstrates that the N–H-rich molecules accelerate interfacial water dissociation via hydrogen-bond interactions, and the generated hydrogen species facilitate the conversion of *CO to *CHO. This enables the efficient asymmetric *CHO–*CO coupling to C2 products with a faradaic efficiency (FE) ∼ 30% higher than that of the unmodified catalyst. Moreover, by adjustment of the relative *CHO/*CO coverage via Cu surface facet regulation, the selectivity can be entirely switched between C2 products and CH4. These mechanistic insights further guided the development of a more efficient catalyst by directly modifying Cu2O nanocubes with the N–H-rich molecule, achieving remarkable C2 product (mainly ethene and ethanol) FEs of 85.7% at a current density of 800 mA cm–2 and excellent stability under nearing industrial conditions. This study advances our understanding of the CO2 reduction mechanisms and offers an effective and general strategy for enhancing electrocatalytic performance by accelerating water dissociation.
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