Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate
Jie Ding,
Fuhua Li,
Xinyi Ren,
Yuhang Liu,
Yifan Li,
Zheng Shen,
Tian Wang,
Weijue Wang,
Yang-Gang Wang,
Yi Cui,
Hongbin Yang (),
Tianyu Zhang () and
Bin Liu ()
Additional contact information
Jie Ding: City University of Hong Kong
Fuhua Li: City University of Hong Kong
Xinyi Ren: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yuhang Liu: Suzhou University of Science and Technology
Yifan Li: Chinese Academy of Sciences
Zheng Shen: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Tian Wang: National University of Singapore
Weijue Wang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yang-Gang Wang: Southern University of Science and Technology
Yi Cui: Chinese Academy of Sciences
Hongbin Yang: Suzhou University of Science and Technology
Tianyu Zhang: Beijing Forestry University
Bin Liu: City University of Hong Kong
Nature Communications, 2024, vol. 15, issue 1, 1-9
Abstract:
Abstract Electrochemical carbon dioxide/carbon monoxide reduction reaction offers a promising route to synthesize fuels and value-added chemicals, unfortunately their activities and selectivities remain unsatisfactory. Here, we present a general surface molecular tuning strategy by modifying Cu2O with a molecular pyridine-derivative. The surface modified Cu2O nanocubes by 4-mercaptopyridine display a high Faradaic efficiency of greater than 60% in electrochemical carbon monoxide reduction reaction to acetate with a current density as large as 380 mA/cm2 in a liquid electrolyte flow cell. In-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy reveals stronger *CO signal with bridge configuration and stronger *OCCHO signal over modified Cu2O nanocubes by 4-mercaptopyridine than unmodified Cu2O nanocubes during electrochemical CO reduction. Density function theory calculations disclose that local molecular tuning can effectively regulate the electronic structure of copper catalyst, enhancing *CO and *CHO intermediates adsorption by the stabilization effect through hydrogen bonding, which can greatly promote asymmetric *CO-*CHO coupling in electrochemical carbon monoxide reduction reaction.
Date: 2024
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DOI: 10.1038/s41467-024-47913-1
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