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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 and Jonas C. Peters
Angewandte Chemie, v 135(12), pn/a
13 Mar 2023
DOI: https://doi.org/10.1002/ange.202216102
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https://doi.org/10.1002/ange.202216102View
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Abstract

Carbon Dioxide Reduction CO2R at Low pH C−C Coupling from CO2 Film-Modified Electrodes HER Suppression
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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