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In Situ Deposited Polyaromatic Layer Generates Robust Copper Catalyst for Selective Electrochemical CO₂ Reduction at Variable pH

Watkins, Nicholas B. and Wu, Yueshen and Nie, Weixuan and Peters, Jonas C. and Agapie, Theodor (2023) In Situ Deposited Polyaromatic Layer Generates Robust Copper Catalyst for Selective Electrochemical CO₂ Reduction at Variable pH. ACS Energy Letters, 8 (1). pp. 189-195. ISSN 2380-8195. doi:10.1021/acsenergylett.2c02002. https://resolver.caltech.edu/CaltechAUTHORS:20221209-478595000.6

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Abstract

Electrochemical reduction of CO₂ (CO₂R) by Cu metal holds promise to convert CO₂ to valuable C₂₊ chemicals at scale using electricity and water but suffers from poor selectivity. Coating of metal electrodes with small organic molecules or polymers has been shown to effectively enhance catalytic performance but remains underexplored. Herein, facile modification of Cu surfaces by a polyaromatic layer was found to boost both selectivity and activity toward C₂₊ products. Using phenyldiazonium or diphenyliodonium salts to graft an organic layer onto the surface of Cu foil electrodes resulted in up to 75% Faradaic efficiency (FE) for C₂₊ at neutral pH. Modified electrodes have electrochemical active surface areas and proton diffusion coefficients similar to those of bare Cu. High CO₂R performance was maintained in a gas diffusion electrode, with a pH ≈ 1 electrolyte (1 M H₃PO₄, 1 M KCl; −100 mA/cm²), producing 65% FE for C₂₊ over 5 h, with no delamination.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsenergylett.2c02002DOIArticle
ORCID:
AuthorORCID
Watkins, Nicholas B.0000-0001-7251-9387
Wu, Yueshen0000-0002-3784-0594
Nie, Weixuan0000-0003-2094-6840
Peters, Jonas C.0000-0002-6610-4414
Agapie, Theodor0000-0002-9692-7614
Alternate Title:In Situ Deposited Polyaromatic Layer Generates Robust Copper Catalyst for Selective Electrochemical CO2 Reduction at Variable pH
Additional Information:Research was in part carried out at the Molecular Materials Research Center in the Beckman Institute; accordingly, we thank Bruce Brunschwig for the assistance with surface FT-IR measurements and Jake Evans for the assistance with XPS measurements. We also thank Aidan Fenwick for the assistance with AFM measurements and Matthias Richter for the assistance with XPS measurements. This material is based on work performed by the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award Number DE-SC0021266. The Resnick Sustainability Institute at Caltech is also acknowledged for its support of enabling infrastructure and facilities.
Group:Liquid Sunlight Alliance, Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0021266
Resnick Sustainability InstituteUNSPECIFIED
Issue or Number:1
DOI:10.1021/acsenergylett.2c02002
Record Number:CaltechAUTHORS:20221209-478595000.6
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20221209-478595000.6
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:118283
Collection:CaltechAUTHORS
Deposited By: Research Services Depository
Deposited On:12 Jan 2023 17:37
Last Modified:25 Jan 2023 23:36

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