Multifunctional Binding Interface Drives Near‐Unity CO Selectivity in Acidic CO<sub>2</sub> Electrolysis
The electrocatalytic carbon dioxide (CO<sub>2</sub>) reduction is challenged by the parasitic hydrogen evolution reaction (HER) especially in acidic media. Here, we elaborate that redox-active isoindigo, acting as a multifunctional co-catalyst, can pre-activate CO<sub>2</sub>-bound intermediates and suppress HER upon the synergistic effects of Lewis acid-base adduct formation, intramolecular hydrogen-bond interaction, and interfacial water structure modulation. Modifying a silver catalyst with isoindigo substantially decreases the energy barrier for CO<sub>2</sub>-to-*COOH conversion, which is regarded as the potential-limiting step of carbon monoxide production. Accordingly, superior catalytic performances are obtained at pH 2, where Faradaic efficiencies surpass 99% at industrial-relevant current densities. Moreover, we find that assembling an additional polyamine-coated layer in front of gas flow channels improves CO<sub>2</sub> transport to the catalyst layer, optimizing the trade-off of conversion and selectivity at low flow rates.
Authors
- Zhengyuan Li (ORCID: https://orcid.org/0000-0002-1525-4981)
- LC Gupta (ORCID: https://orcid.org/0009-0003-8172-2143)
- Zhiyao Qi
- Gregory D. Foley (ORCID: https://orcid.org/0000-0002-7340-7149)
- Dian‐Zhao Lin (ORCID: https://orcid.org/0000-0003-1177-2308)
- Andong Liu (ORCID: https://orcid.org/0000-0003-3999-0657)
- Carter S. Gerke (ORCID: https://orcid.org/0000-0002-6035-1043)
- Anmol Mathur (ORCID: https://orcid.org/0000-0001-8343-731X)
- Fanglin Che (ORCID: https://orcid.org/0000-0001-5109-8296)
- V. Sara Thoi (ORCID: https://orcid.org/0000-0003-0896-4077)
- Yuting Xu (ORCID: https://orcid.org/0000-0003-2091-3854)
- Krish N. Jayarapu (ORCID: https://orcid.org/0000-0002-5822-4133)
- Long Chen (ORCID: https://orcid.org/0000-0002-8992-0625)
- Xing Li (ORCID: https://orcid.org/0000-0002-5470-1043)
- Lingyu Zhang (ORCID: https://orcid.org/0000-0002-4297-903X)
- Yayuan Liu (ORCID: https://orcid.org/0000-0002-0718-4784)
Institutions
- Worcester Polytechnic Institute (US)
- Johns Hopkins University (US)
- City University of Hong Kong (HK)
- Johns Hopkins Medicine (US)
- Yale University (US)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-09-04
- DOI
- https://doi.org/10.1002/anie.202514111
- Citations
- 3
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 1.09
Funders
- National Science Foundation
- David and Lucile Packard Foundation
- U.S. Department of Energy
- Arnold and Mabel Beckman Foundation
- Johns Hopkins University