Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts

The electrochemical reduction of carbon dioxide (CO<sub>2</sub>) to carbon monoxide (CO) is challenged by a selectivity decline at high current densities. Here we report a class of indigo-based molecular promoters with redox-active CO<sub>2</sub> binding sites to enhance the high-rate conversion of CO<sub>2</sub> to CO on silver (Ag) catalysts. Theoretical calculations and in situ spectroscopy analyses demonstrate that the synergistic effect at the interface of indigo-derived compounds and Ag nanoparticles could activate CO<sub>2</sub> molecules and accelerate the formation of key intermediates (*CO<sub>2</sub><sup>-</sup> and *COOH) in the CO pathway. Indigo derivatives with electron-withdrawing groups further reduce the overpotential for CO production upon optimizing the interfacial CO<sub>2</sub> binding affinity. By integrating the molecular design of redox-active centres with the defect engineering of Ag structures, we achieve a Faradaic efficiency for CO exceeding 90% across a current density range of 0.10 - 1.20 A cm<sup>-2</sup>. The Ag mass activity toward CO increases to 174 A mg<sup>-1</sup><sub>Ag</sub>. This work showcases that employing redox-active CO<sub>2</sub> sorbents as surface modification agents is a highly effective strategy to intensify the reactivity of electrochemical CO<sub>2</sub> reduction.

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Publication Details

Journal
Nature Communications
Published
2025-04-03
DOI
https://doi.org/10.1038/s41467-025-58593-w
Citations
18
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
6.54

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Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts

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Nature Communications
CO2 Reduction Techniques and Catalysts
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article

Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts

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article en
18 citations

Abstract

The electrochemical reduction of carbon dioxide (CO<sub>2</sub>) to carbon monoxide (CO) is challenged by a selectivity decline at high current densities. Here we report a class of indigo-based molecular promoters with redox-active CO<sub>2</sub> binding sites to enhance the high-rate conversion of CO<sub>2</sub> to CO on silver (Ag) catalysts. Theoretical calculations and in situ spectroscopy analyses demonstrate that the synergistic effect at the interface of indigo-derived compounds and Ag nanoparticles could activate CO<sub>2</sub> molecules and accelerate the formation of key intermediates (*CO<sub>2</sub><sup>-</sup> and *COOH) in the CO pathway. Indigo derivatives with electron-withdrawing groups further reduce the overpotential for CO production upon optimizing the interfacial CO<sub>2</sub> binding affinity. By integrating the molecular design of redox-active centres with the defect engineering of Ag structures, we achieve a Faradaic efficiency for CO exceeding 90% across a current density range of 0.10 - 1.20 A cm<sup>-2</sup>. The Ag mass activity toward CO increases to 174 A mg<sup>-1</sup><sub>Ag</sub>. This work showcases that employing redox-active CO<sub>2</sub> sorbents as surface modification agents is a highly effective strategy to intensify the reactivity of electrochemical CO<sub>2</sub> reduction.

Nature CommunicationsVol. 16(1)
Johns Hopkins University (US), City University of Hong Kong (HK), Brookhaven National Laboratory (US), Johns Hopkins Medicine (US), Stony Brook University (US), Rice University (US), The University of Texas at Austin (US), Indian Institute of Technology Kanpur (IN)
National Science Foundation, David and Lucile Packard Foundation, U.S. Department of Energy, Arnold and Mabel Beckman Foundation, Johns Hopkins University, Indian Institute of Technology Kanpur, Office of Science, Division of Chemistry, Basic Energy Sciences, Brookhaven National Laboratory, National Renewable Energy Laboratory
Openalex Percentile: Top 3%
CO2 Reduction Techniques and Catalysts
6.54
DOIOpen Access PDFOpenAlex
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