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Organic Additive‐derived Films on Cu Electrodes Promote Electrochemical CO2 Reduction to C2+ Products Under Strongly Acidic Conditions
Journal article   Peer reviewed

Organic Additive‐derived Films on Cu Electrodes Promote Electrochemical CO2 Reduction to C2+ Products Under Strongly Acidic Conditions

Weixuan Nie, Gavin P. Heim, Nicholas B. Watkins, Theodor Agapie, Jonas C. Peters and California Institute of Technology (CalTech), Pasadena, CA (United States)
Angewandte Chemie International Edition, v 62(12), pp e202216102-n/a
13 Mar 2023
PMID: 36656130

Abstract

Carbon Dioxide Reduction CO2R at Low pH C−C Coupling from CO2 Film-Modified Electrodes HER Suppression ESI Highly Cited Paper (Incites)
Electrochemical CO2 reduction (CO2R) at low pH is desired for high CO2 utilization; the competing hydrogen evolution reaction (HER) remains a challenge. High alkali cation concentration at a high operating current density has recently been used to promote electrochemical CO2R at low pH. Herein we report an alternative approach to selective CO2R (>70 % Faradaic efficiency for C2+ products, FEC2+) at low pH (pH 2; H3PO4/KH2PO4) and low potassium concentration ([K+]=0.1 M) using organic film‐modified polycrystalline copper (Modified‐Cu). Such an electrode effectively mitigates HER due to attenuated proton transport. Modified‐Cu still achieves high FEC2+ (45 % with Cu foil /55 % with Cu GDE) under 1.0 M H3PO4 (pH≈1) at low [K+] (0.1 M), even at low operating current, conditions where HER can otherwise dominate. Modified copper electrodes with N‐tolyl pyridinium additive‐derived films show boosted selectivity of the CO2 reduction to C2+ products (>70 % Faradaic efficiency) and great suppression of the hydrogen evolution reaction in strongly acidic electrolytes with low alkali cation concentrations.

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UN Sustainable Development Goals (SDGs)

This publication has contributed to the advancement of the following goals:

#13 Climate Action
#7 Affordable and Clean Energy

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Web of Science research areas
Chemistry, Multidisciplinary
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