Pulsed Electrolysis Promotes CO2 Reduction to Ethanol on Heterostructured Cu2O/Ag Catalysts
© 2023 Wiley‐VCH GmbH..
The electrochemical conversion of carbon dioxide (CO2) into ethanol with high added value has attracted increasing attention. Here, an efficient catalyst with abundant Cu2O/Ag interfaces for ethanol production under pulsed CO2 electrolysis is reported, which is composed of Cu2O hollow nanospheres loaded with Ag nanoparticles (named as se-Cu2O/Ag). The CO2-to-ethanol Faradaic efficiency is prominently improved to 46.3% at a partial current density up to 417 mA cm-2 under pulsed electrolysis conditions in a neutral flow cell, notably outperforming conventional Cu catalysts during static electrolysis. In situ spectroscopy reveals the stabilized Cu+ species of se-Cu2O/Ag during pulsed electrolysis and the enhanced adsorbed CO intermediate (*CO)coverage on the heterostructured catalyst. Density functional theory (DFT) calculations further confirm that the Cu2O/Ag heterostructure stabilizes the *CO intermediate and promotes the coupling of *CO and adsorbed CH intermediate (*CH). Meanwhile, the stable Cu+ species under pulsed electrolysis favor the hydrogenation of adsorbed HCCOH intermediate (*HCCOH) to adsorbed HCCHOH intermediate (*HCCHOH) on the pathway to ethanol. The synergistic effect between the enhanced generation of *CO on Cu2O/Ag and regenerated Cu+ species under pulsed electrolysis steers the reaction pathway toward ethanol. This work provides some insights into selective ethanol production from CO2 electroreduction via combined catalyst design and non-steady state electrolysis.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:20 |
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| Enthalten in: |
Small (Weinheim an der Bergstrasse, Germany) - 20(2024), 12 vom: 29. März, Seite e2307637 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Wu, Xiuju [VerfasserIn] |
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| Links: |
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| Themen: |
Electrochemical CO2 reduction |
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| Anmerkungen: |
Date Revised 23.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1002/smll.202307637 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM364380721 |
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| 520 | |a © 2023 Wiley‐VCH GmbH. | ||
| 520 | |a The electrochemical conversion of carbon dioxide (CO2) into ethanol with high added value has attracted increasing attention. Here, an efficient catalyst with abundant Cu2O/Ag interfaces for ethanol production under pulsed CO2 electrolysis is reported, which is composed of Cu2O hollow nanospheres loaded with Ag nanoparticles (named as se-Cu2O/Ag). The CO2-to-ethanol Faradaic efficiency is prominently improved to 46.3% at a partial current density up to 417 mA cm-2 under pulsed electrolysis conditions in a neutral flow cell, notably outperforming conventional Cu catalysts during static electrolysis. In situ spectroscopy reveals the stabilized Cu+ species of se-Cu2O/Ag during pulsed electrolysis and the enhanced adsorbed CO intermediate (*CO)coverage on the heterostructured catalyst. Density functional theory (DFT) calculations further confirm that the Cu2O/Ag heterostructure stabilizes the *CO intermediate and promotes the coupling of *CO and adsorbed CH intermediate (*CH). Meanwhile, the stable Cu+ species under pulsed electrolysis favor the hydrogenation of adsorbed HCCOH intermediate (*HCCOH) to adsorbed HCCHOH intermediate (*HCCHOH) on the pathway to ethanol. The synergistic effect between the enhanced generation of *CO on Cu2O/Ag and regenerated Cu+ species under pulsed electrolysis steers the reaction pathway toward ethanol. This work provides some insights into selective ethanol production from CO2 electroreduction via combined catalyst design and non-steady state electrolysis | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a electrochemical CO2 reduction | |
| 650 | 4 | |a ethanol | |
| 650 | 4 | |a heterostructure | |
| 650 | 4 | |a multi‐carbon products | |
| 650 | 4 | |a pulsed electrolysis | |
| 700 | 1 | |a Li, Xiaotong |e verfasserin |4 aut | |
| 700 | 1 | |a Lv, Jiabao |e verfasserin |4 aut | |
| 700 | 1 | |a Lv, Xiangzhou |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Angjian |e verfasserin |4 aut | |
| 700 | 1 | |a Qi, Zhifu |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Hao Bin |e verfasserin |4 aut | |
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