Sulfur Changes the Electrochemical CO2 Reduction Pathway over Cu Electrocatalysts.
Angew Chem Int Ed Engl
; 62(44): e202310740, 2023 Oct 26.
Article
em En
| MEDLINE
| ID: mdl-37703214
ABSTRACT
Electrochemical CO2 reduction to value-added chemicals or fuels offers a promising approach to reduce carbon emissions and alleviate energy shortage. Cu-based electrocatalysts have been widely reported as capable of reducing CO2 to produce a variety of multicarbon products (e.g., ethylene and ethanol). In this work, we develop sulfur-doped Cu2 O electrocatalysts, which instead can electrochemically reduce CO2 to almost exclusively formate. We show that a dynamic equilibrium of S exists at the Cu2 O-electrolyte interface, and S-doped Cu2 O undergoes in situ surface reconstruction to generate active S-adsorbed metallic Cu sites during the CO2 reduction reaction (CO2 RR). Density functional theory (DFT) calculations together with in situ infrared absorption spectroscopy measurements show that the S-adsorbed metallic Cu surface can not only promote the formation of the *OCHO intermediate but also greatly suppress *H and *COOH adsorption, thus facilitating CO2 -to-formate conversion during the electrochemical CO2 RR.
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MEDLINE
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En
Ano de publicação:
2023
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Article