Synergy of Cu/C3 N4 Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid

Xupeng Yan; Menglu Zhang; Yizhen Chen; Yahui Wu; Ruizhi Wu; Qiang Wan; Chunxiao Liu; Tingting Zheng; Rongjuan Feng; Jing Zhang; Chunjun Chen; Chuan Xia; Qinggong Zhu; Xiaofu Sun; Qingli Qian; Buxing Han

doi:10.1002/anie.202301507

Synergy of Cu/C₃ N₄ Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid

Angew Chem Int Ed Engl. 2023 May 22;62(22):e202301507. doi: 10.1002/anie.202301507. Epub 2023 Apr 25.

Authors

Xupeng Yan^{1

2

3}, Menglu Zhang^{4

5}, Yizhen Chen⁶, Yahui Wu^{1

2}, Ruizhi Wu^{1

2}, Qiang Wan^{1

2}, Chunxiao Liu⁵, Tingting Zheng^{5

7}, Rongjuan Feng¹, Jing Zhang⁸, Chunjun Chen^{1

2}, Chuan Xia^{5

7}, Qinggong Zhu^{1

2}, Xiaofu Sun^{1

2}, Qingli Qian^{1

2}, Buxing Han^{1

2

9

10}

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
² School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
³ China Huaneng Clean Energy Research Institute, Beijing, 102209, China.
⁴ Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, P. R. China.
⁵ School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, P. R. China.
⁶ Department of Chemical Engineering, University of California, Davis, CA, 95616, USA.
⁷ Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou, P. R. China.
⁸ Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
⁹ Physical Science Laboratory, Huairou National Comprehensive Science Center, No. 5 Yanqi East Second Street, Beijing, 101400, China.
¹⁰ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China.

PMID: 37005226
DOI: 10.1002/anie.202301507

Abstract

Electrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g-C₃ N₄ ) supported Cu nanoparticles (Cu-CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm^-2 in CORR. In situ experimental and density functional theory calculation studies revealed that the Cu/C₃ N₄ interface and metallic Cu surface synergistically promoted CORR into acetic acid. The generation of pivotal intermediate -*CHO is advantage around the Cu/C₃ N₄ interface and migrated *CHO facilitates acetic acid generation on metallic Cu surface with promoted *CHO coverage. Moreover, continuous production of acetic acid aqueous solution was achieved in a porous solid electrolyte reactor, indicating the great potential of Cu-CN catalyst in the industrial application.

Keywords: Acetic Acid; Carbon Monoxide; Electrocatalysis; Green Chemistry; Porous Solid Electrolyte.

Abstract

Grants and funding