Sulfur Changes the Electrochemical CO2 Reduction Pathway over Cu Electrocatalysts
© 2023 Wiley-VCH GmbH..
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.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:62 |
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| Enthalten in: |
Angewandte Chemie (International ed. in English) - 62(2023), 44 vom: 26. Okt., Seite e202310740 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Liang, Shuyu [VerfasserIn] |
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| Links: |
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| Themen: |
CO2 Reduction Reaction |
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| Anmerkungen: |
Date Revised 20.10.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1002/anie.202310740 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| 520 | |a © 2023 Wiley-VCH GmbH. | ||
| 520 | |a 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 | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a CO2 Reduction Reaction | |
| 650 | 4 | |a Cu-Based Electrocatalysts | |
| 650 | 4 | |a Electrocatalysis | |
| 650 | 4 | |a Formic Acid | |
| 650 | 4 | |a S Modification | |
| 700 | 1 | |a Xiao, Jiewen |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Tianyu |e verfasserin |4 aut | |
| 700 | 1 | |a Zheng, Yue |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Qiang |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Bin |e verfasserin |4 aut | |
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