Few-Atom Copper Catalyst for the Electrochemical Reduction of CO to Acetate: Synergetic Catalysis between Neighboring Cu Atoms

Journal Article · Tue Jun 14 00:00:00 EDT 2022 · CCS Chemistry

DOI:https://doi.org/10.31635/ccschem.022.202201910· OSTI ID:1879431

Rong, Weifeng ^[1]; Zou, Haiyuan ^[1]; Tan, Sha ^[2]; Hu, Enyuan ^[2]; Li, Fan ^[1]; Tang, Chao ^[1]; Dai, Hao ^[1]; Wei, Shuting ^[1]; Ji, Yongfei ^[3]; Duan, Lele ^[1]

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1. Southern University of Science and Technology, Shenzhen (China)
2. Brookhaven National Lab. (BNL), Upton, NY (United States)
3. Guangzhou University (China)

Single-atom catalysts (SACs) are gaining increasing recognition because of their superior catalytic properties for various reactions. However, the performance of SACs is often limited by the lack of neighboring metal centers to cooperate in catalysis. Herein, a synergetic interaction between neighboring Cu atoms of a few-atom catalyst (FAC) on graphdiyne is found to greatly enhance the production of acetate in CO electroreduction reaction relative to Cu SACs. In a 1.0 M KOH electrolyte, this Cu FAC exhibits an acetate Faradaic efficiency of 53.8±1.5 % and an ultrahigh relative purity of up to 97 wt% for liquid products, and excellent stability of over 23 h continuous electrolysis at -0.8 V versus reversible hydrogen electrode (RHE). Theoretical studies suggest that the intersite catalytic communication between two neighboring metal atoms confined in each pore of GDY facilitates the formation of acetic acid through either stepwise hydrogenation of CH₂CO* or the direct reaction of H₂O with CH₂CO*. Our study demonstrates the unprecedented synergetic catalysis of Cu FAC in promoting the selective CO electroreduction toward acetate production.

• Research Organization: Brookhaven National Laboratory (BNL), Upton, NY (United States)
• Sponsoring Organization: Educational Commission of Guangdong Province; National Natural Science Foundation of China; Shenzhen Natural Science Fund; Shenzhen R&D; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
• OSTI ID: 1879431
• Report Number(s): BNL-223199-2022-JAAM
• Journal Information: CCS Chemistry, Journal Name: CCS Chemistry Journal Issue: 5 Vol. 5; ISSN 2096-5745
• Publisher: Chinese Chemical Society Publishing
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO electroreduction
acetate
few-atom catalyst
graphdiyne
synergetic catalysis