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Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts
by
Wang, Ruoyu
, Ajayan, Pulickel M.
, Liu, Yayuan
, Li, Tianchen
, Jayarapu, Krish N.
, Li, Xing
, Zhang, Lingyu
, Liu, Andong
, Roy, Soumyabrata
, Lin, Dian-Zhao
, Gupta, Lavanya
, Liu, Yuanyue
, Mathur, Anmol
, Thoi, V. Sara
, Xiang, Shuting
, Frenkel, Anatoly I.
, Gerke, Carter S.
, Campos Mata, Astrid
, Li, Zhengyuan
in
119/118
/ 140/131
/ 147/135
/ 147/143
/ 639/301/299/886
/ 639/638/161/886
/ 639/638/77/886
/ Binding sites
/ Carbon dioxide
/ Carbon monoxide
/ Catalysts
/ Chemical reduction
/ Current density
/ electrocatalysis
/ Electrochemistry
/ High current
/ Humanities and Social Sciences
/ Indigo
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Intermediates
/ multidisciplinary
/ Nanoparticles
/ Science
/ Science (multidisciplinary)
/ Silver
/ Sorbents
/ Spectroscopy
/ Synergistic effect
2025
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Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts
by
Wang, Ruoyu
, Ajayan, Pulickel M.
, Liu, Yayuan
, Li, Tianchen
, Jayarapu, Krish N.
, Li, Xing
, Zhang, Lingyu
, Liu, Andong
, Roy, Soumyabrata
, Lin, Dian-Zhao
, Gupta, Lavanya
, Liu, Yuanyue
, Mathur, Anmol
, Thoi, V. Sara
, Xiang, Shuting
, Frenkel, Anatoly I.
, Gerke, Carter S.
, Campos Mata, Astrid
, Li, Zhengyuan
in
119/118
/ 140/131
/ 147/135
/ 147/143
/ 639/301/299/886
/ 639/638/161/886
/ 639/638/77/886
/ Binding sites
/ Carbon dioxide
/ Carbon monoxide
/ Catalysts
/ Chemical reduction
/ Current density
/ electrocatalysis
/ Electrochemistry
/ High current
/ Humanities and Social Sciences
/ Indigo
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Intermediates
/ multidisciplinary
/ Nanoparticles
/ Science
/ Science (multidisciplinary)
/ Silver
/ Sorbents
/ Spectroscopy
/ Synergistic effect
2025
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Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts
by
Wang, Ruoyu
, Ajayan, Pulickel M.
, Liu, Yayuan
, Li, Tianchen
, Jayarapu, Krish N.
, Li, Xing
, Zhang, Lingyu
, Liu, Andong
, Roy, Soumyabrata
, Lin, Dian-Zhao
, Gupta, Lavanya
, Liu, Yuanyue
, Mathur, Anmol
, Thoi, V. Sara
, Xiang, Shuting
, Frenkel, Anatoly I.
, Gerke, Carter S.
, Campos Mata, Astrid
, Li, Zhengyuan
in
119/118
/ 140/131
/ 147/135
/ 147/143
/ 639/301/299/886
/ 639/638/161/886
/ 639/638/77/886
/ Binding sites
/ Carbon dioxide
/ Carbon monoxide
/ Catalysts
/ Chemical reduction
/ Current density
/ electrocatalysis
/ Electrochemistry
/ High current
/ Humanities and Social Sciences
/ Indigo
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Intermediates
/ multidisciplinary
/ Nanoparticles
/ Science
/ Science (multidisciplinary)
/ Silver
/ Sorbents
/ Spectroscopy
/ Synergistic effect
2025
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Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts
Journal Article
Electro-activated indigos intensify ampere-level CO2 reduction to CO on silver catalysts
2025
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Overview
The electrochemical reduction of carbon dioxide (CO
2
) 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
2
binding sites to enhance the high-rate conversion of CO
2
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
2
molecules and accelerate the formation of key intermediates (*CO
2
–
and *COOH) in the CO pathway. Indigo derivatives with electron-withdrawing groups further reduce the overpotential for CO production upon optimizing the interfacial CO
2
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
–2
. The Ag mass activity toward CO increases to 174 A mg
–1
Ag
. This work showcases that employing redox-active CO
2
sorbents as surface modification agents is a highly effective strategy to intensify the reactivity of electrochemical CO
2
reduction.
It is challenging to maintain the CO selectivity under high current densities in CO
2
electro-reduction process. Here the authors report the synergistic interface between redox active CO
2
organic sorbents and defective Ag catalysts that can enable an ampere level CO
2
-to-CO conversion.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Springer Science and Business Media LLC,Nature Portfolio
Subject
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