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

Zhengyuan Li (), Xing Li, Ruoyu Wang, Astrid Campos Mata, Carter S. Gerke, Shuting Xiang, Anmol Mathur, Lingyu Zhang, Dian-Zhao Lin, Tianchen Li, Krish N. Jayarapu, Andong Liu, Lavanya Gupta, Anatoly I. Frenkel, V. Sara Thoi, Pulickel M. Ajayan, Soumyabrata Roy, Yuanyue Liu and Yayuan Liu ()
Additional contact information
Zhengyuan Li: Johns Hopkins University
Xing Li: Johns Hopkins University
Ruoyu Wang: The University of Texas at Austin
Astrid Campos Mata: Rice University
Carter S. Gerke: Johns Hopkins University
Shuting Xiang: Stony Brook University
Anmol Mathur: Johns Hopkins University
Lingyu Zhang: Johns Hopkins University
Dian-Zhao Lin: Johns Hopkins University
Tianchen Li: Johns Hopkins University
Krish N. Jayarapu: Johns Hopkins University
Andong Liu: Johns Hopkins University
Lavanya Gupta: Johns Hopkins University
Anatoly I. Frenkel: Stony Brook University
V. Sara Thoi: Johns Hopkins University
Pulickel M. Ajayan: Rice University
Soumyabrata Roy: Rice University
Yuanyue Liu: The University of Texas at Austin
Yayuan Liu: Johns Hopkins University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract The electrochemical reduction of carbon dioxide (CO2) 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 CO2 binding sites to enhance the high-rate conversion of CO2 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 CO2 molecules and accelerate the formation of key intermediates (*CO2– and *COOH) in the CO pathway. Indigo derivatives with electron-withdrawing groups further reduce the overpotential for CO production upon optimizing the interfacial CO2 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–1Ag. This work showcases that employing redox-active CO2 sorbents as surface modification agents is a highly effective strategy to intensify the reactivity of electrochemical CO2 reduction.

Date: 2025
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DOI: 10.1038/s41467-025-58593-w

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