Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate

Ding，Jie1; Li，Fuhua1; Ren，Xinyi2; Liu，Yuhang3; Li，Yifan4; Shen，Zheng2; Wang，Tian5; Wang，Weijue2; Wang，Yang Gang6; Cui，Yi4; Yang，Hongbin3; Zhang，Tianyu7; Liu，Bin1,8

2024-12-01

10.1038/s41467-024-47913-1

Nature Communications   影响因子和分区

2041-1723

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 CuO with a molecular pyridine-derivative. The surface modified CuO 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/cm 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 CuO nanocubes by 4-mercaptopyridine than unmodified CuO 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.

SCI

英语

其他

2-s2.0-85191808508

Scopus

1.Department of Materials Science and Engineering,City University of Hong Kong,Hong Kong
2.CAS Key Laboratory of Science and Technology on Applied Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,China
3.School of Materials Science and Engineering,Suzhou University of Science and Technology,Suzhou,China
4.Vacuum Interconnected Nanotech Workstation,Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences,Suzhou,China
5.Department of Chemical & amp; Biomolecular Engineering,National University of Singapore,Singapore,Singapore
6.Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis,Southern University of Science and Technology,Shenzhen,China
7.College of Environmental Science and Engineering,Beijing Forestry University,Beijing,China
8.Department of Chemistry & amp; Center of Super-Diamond and Advanced Films (COSDAF),City University of Hong Kong,Hong Kong

Ding，Jie,Li，Fuhua,Ren，Xinyi,et al. Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate[J]. Nature Communications,2024,15(1).

Ding，Jie.,Li，Fuhua.,Ren，Xinyi.,Liu，Yuhang.,Li，Yifan.,...&Liu，Bin.(2024).Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate.Nature Communications,15(1).

Ding，Jie,et al."Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate".Nature Communications 15.1(2024).