Multifunctional Binding Interface Drives Near‐Unity CO Selectivity in Acidic CO<sub>2</sub> Electrolysis
Abstract
AbstractThe electrocatalytic carbon dioxide (CO2) 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 CO2‐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 CO2‐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 CO2 transport to the catalyst layer, optimizing the trade‐off of conversion and selectivity at low flow rates.
Article Details
Authors (16)
Zhengyuan Li
Yuting Xu
Section of Hematology and Medical Oncology, Department of Medicine, Tulane University School of Medicine
Xing Li
Interdisciplinary Science Center, State Key Laboratory of Animal Biodiversity Conservation and Integrated Pest Management, Institute of Zoology
Gregory D. Y. Foley
Department of Chemistry Johns Hopkins University Baltimore Maryland 21218 USA
Dian‐Zhao Lin
Department of Chemical and Biomolecular Engineering Johns Hopkins University Baltimore Maryland 21218 USA
Lingyu Zhang
Clinical Oncology School of Fujian Medical University, Fujian Cancer Hospital, Fujian Medical University
Krish N. Jayarapu
Long Chen
Department of Chemistry, Frontiers Science Center for New Organic Matter and State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry
Carter S. Gerke
Andong Liu
Anmol Mathur
Zhiyao Qi
Department of Chemical and Biomolecular Engineering Johns Hopkins University Baltimore Maryland 21218 USA
Lavanya Gupta
Van Sara Thoi
Department of Chemistry Johns Hopkins University Baltimore Maryland 21218 USA
Fanglin Che
Department of Chemical Engineering
Yayuan Liu