Modulating CO2 Electrocatalytic Conversion to the Organics Pathway by the Catalytic Site Dimension

• DOI: 10.1021/jacs.3c12722
• Publication Date: 2024-04-04T18:18:33Z
• Authors: Haiping Xu; Jianxin Wang; Haiying He; Inhui Hwang; Yuzi Liu; Chengjun Sun; Haozhe Zhang; Tao Li; John V. Muntean; Tao Xu; Di-Jia Liu

Electrochemical reduction of carbon dioxide to organic chemicals provides a value-added route for mitigating greenhouse gas emissions. We report a family of carbon-supported Sn electrocatalysts with the tin size varying from single atom, ultrasmall clusters to nanocrystallites. High single-product Faradaic efficiency (FE) and low onset potential of CO2 conversion to acetate (FE = 90% @ -0.6 V), ethanol (FE = 92% @ -0.4 V), and formate (FE = 91% @ -0.6 V) were achieved over the catalysts of different active site dimensions. The CO2 conversion mechanism behind these highly selective, size-modulated p-block element catalysts was elucidated by structural characterization and computational modeling, together with kinetic isotope effect investigation.