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Title: Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction

Abstract

Electrocatalytic CO2 reduction to higher value hydrocarbons beyond C1 products is desirable for applications in energy storage, transportation, and the chemical industry. Cu catalysts have shown the potential to catalyze C-C coupling for C2+ products, but still suffer from low selectivity in aqueous solutions. Using density functional theory, we determined the energetics of the initial C-C coupling steps on different Cu facets for CO2 reduction. The calculations suggest the Cu(100) and stepped (211) facets to favor C2+ product formation over Cu(111). Through a metal ion battery cycling method, we fabricate high surface area Cu nanocube catalysts which preferentially expose (100) facets. These Cu nanocube catalysts present a 6-fold improvement in C2+ to C1 product ratio over polished Cu foils, with the highest C2+ Faradaic efficiency of over 60 % and H2 below 20 %, and a corresponding C2+ current density of more than 40 mA/cm2.

Authors:
ORCiD logo [1];  [2];  [1];  [2];  [1];  [3];  [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Harvard Univ., Cambridge, MA (United States)
  2. Stanford Univ., Stanford, CA (United States)
  3. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1457051
Alternate Identifier(s):
OSTI ID: 1490974
Grant/Contract Number:  
AC02-76SF00515; SC0004993; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 1; Journal Issue: 2; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Jiang, Kun, Sandberg, Robert B., Akey, Austin J., Liu, Xinyan, Bell, David C., Norskov, Jens K., Chan, Karen, and Wang, Haotian. Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction. United States: N. p., 2018. Web. doi:10.1038/s41929-017-0009-x.
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Jiang, Kun, Sandberg, Robert B., Akey, Austin J., Liu, Xinyan, Bell, David C., Norskov, Jens K., Chan, Karen, & Wang, Haotian. Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction. United States. https://doi.org/10.1038/s41929-017-0009-x
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Jiang, Kun, Sandberg, Robert B., Akey, Austin J., Liu, Xinyan, Bell, David C., Norskov, Jens K., Chan, Karen, and Wang, Haotian. Mon . "Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction". United States. https://doi.org/10.1038/s41929-017-0009-x. https://www.osti.gov/servlets/purl/1457051.
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@article{osti_1457051,
title = {Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction},
author = {Jiang, Kun and Sandberg, Robert B. and Akey, Austin J. and Liu, Xinyan and Bell, David C. and Norskov, Jens K. and Chan, Karen and Wang, Haotian},
abstractNote = {Electrocatalytic CO2 reduction to higher value hydrocarbons beyond C1 products is desirable for applications in energy storage, transportation, and the chemical industry. Cu catalysts have shown the potential to catalyze C-C coupling for C2+ products, but still suffer from low selectivity in aqueous solutions. Using density functional theory, we determined the energetics of the initial C-C coupling steps on different Cu facets for CO2 reduction. The calculations suggest the Cu(100) and stepped (211) facets to favor C2+ product formation over Cu(111). Through a metal ion battery cycling method, we fabricate high surface area Cu nanocube catalysts which preferentially expose (100) facets. These Cu nanocube catalysts present a 6-fold improvement in C2+ to C1 product ratio over polished Cu foils, with the highest C2+ Faradaic efficiency of over 60 % and H2 below 20 %, and a corresponding C2+ current density of more than 40 mA/cm2.},
doi = {10.1038/s41929-017-0009-x},
journal = {Nature Catalysis},
number = 2,
volume = 1,
place = {United States},
year = {Mon Jan 15 00:00:00 EST 2018},
month = {Mon Jan 15 00:00:00 EST 2018}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41929-017-0009-x
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Figures / Tables:

Figure 1 Figure 1: DFT simulations of C-C coupling on Cu facets. (a) Contour plot of the electric field in the vicinity of an ion and its image charge on a Cu(100) surface. (b) Binding free energies in vacuum for 2*CO and *OCCO as a function of electric field strength along themore » z-direction perpendicular to the slab (c) Free energy diagram at 0 V (RHE) for the energetics of the dimerization of *CO to form *OCCO and the subsequent surface hydrogenation (solid lines) and proton-electron transfer (dashed lines) to form *OCCHO in the presence of a solvent and cation-induced field (d) *OCCO configurations on the (100), (111) and (211) facets, where solvent molecules have been removed to show the adsorbate configurations« less
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    • DOI: 10.1002/anie.201913003

    Changing the Product Selectivity for Electrocatalysis of CO 2 Reduction Reaction on Plated Cu Electrodes
    journal, October 2019

    Selective Electroreduction of CO 2 to C2 Products over Cu 3 N‐Derived Cu Nanowires
    journal, March 2019

    Two‐Dimensional Electrocatalysts for Efficient Reduction of Carbon Dioxide
    journal, October 2019

    Structure‐Tunable Copper–Indium Catalysts for Highly Selective CO 2 Electroreduction to CO or HCOOH
    journal, August 2019

    Enhanced Ethanol Production from CO 2 Electroreduction at Micropores in Nitrogen‐Doped Mesoporous Carbon
    journal, December 2019

    Nanostructured Copper-Based Electrocatalysts for CO 2 Reduction
    journal, July 2018

    pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper
    journal, January 2019

    Selective electroreduction of carbon dioxide to methanol on copper selenide nanocatalysts
    journal, February 2019

    Plasmonic photosynthesis of C1–C3 hydrocarbons from carbon dioxide assisted by an ionic liquid
    journal, May 2019

    Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction
    journal, June 2019

    Carbon dioxide electroreduction to C2 products over copper-cuprous oxide derived from electrosynthesized copper complex
    journal, August 2019

    Efficient upgrading of CO to C3 fuel using asymmetric C-C coupling active sites
    journal, November 2019

    Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
    journal, September 2019

    • Birdja, Yuvraj Y.; Pérez-Gallent, Elena; Figueiredo, Marta C.
    • Nature Energy, Vol. 4, Issue 9
    • DOI: 10.1038/s41560-019-0450-y

    Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices
    journal, September 2019

    Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface
    journal, January 2020

    Efficient electrocatalytic CO2 reduction on a three-phase interface
    journal, July 2018

    High-rate electroreduction of carbon monoxide to multi-carbon products
    journal, August 2018

    Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide
    journal, October 2018

    Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper
    journal, February 2019

    Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products
    journal, March 2019

    Two-dimensional copper nanosheets for electrochemical reduction of carbon monoxide to acetate
    journal, April 2019

    Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces
    journal, December 2019

    Carbon monoxide electroreduction as an emerging platform for carbon utilization
    journal, December 2019

    Catalyst synthesis under CO2 electroreduction favours faceting and promotes renewable fuels electrosynthesis
    journal, December 2019

    Cu( ii )-nanoparticle-derived structures under CO 2 reduction conditions: a matter of shape
    journal, January 2019

    • Basiratnia, Amir; Rempel, Jacob; Li, Feng
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 11
    • DOI: 10.1039/c8cp07891b

    From CO 2 methanation to ambitious long-chain hydrocarbons: alternative fuels paving the path to sustainability
    journal, January 2019

    • Marques Mota, Filipe; Kim, Dong Ha
    • Chemical Society Reviews, Vol. 48, Issue 1
    • DOI: 10.1039/c8cs00527c

    Superaerophilic copper nanowires for efficient and switchable CO 2 electroreduction
    journal, January 2019

    • Zhang, Yusheng; Cai, Zhao; Zhao, Yuxin
    • Nanoscale Horizons, Vol. 4, Issue 2
    • DOI: 10.1039/c8nh00259b

    Enhanced CO 2 electroreduction via interaction of dangling S bonds and Co sites in cobalt phthalocyanine/ZnIn 2 S 4 hybrids
    journal, January 2019

    • Chen, Chunjun; Sun, Xiaofu; Yang, Dexin
    • Chemical Science, Vol. 10, Issue 6
    • DOI: 10.1039/c8sc03986k

    A CO 2 adsorption dominated carbon defect-based electrocatalyst for efficient carbon dioxide reduction
    journal, January 2020

    • Wu, Qilong; Gao, Jin; Feng, Jianrui
    • Journal of Materials Chemistry A, Vol. 8, Issue 3
    • DOI: 10.1039/c9ta11473d

    Current progress in electrocatalytic carbon dioxide reduction to fuels on heterogeneous catalysts
    journal, January 2020

    • Liu, Anmin; Gao, Mengfan; Ren, Xuefeng
    • Journal of Materials Chemistry A, Vol. 8, Issue 7
    • DOI: 10.1039/c9ta11966c

    Atomically dispersed asymmetric Cu–B pair on 2D carbon nitride synergistically boosts the conversion of CO into C 2 products
    journal, January 2020

    • He, Tianwei; Reuter, Karsten; Du, Aijun
    • Journal of Materials Chemistry A, Vol. 8, Issue 2
    • DOI: 10.1039/c9ta12090d

    Advances and challenges in electrochemical CO 2 reduction processes: an engineering and design perspective looking beyond new catalyst materials
    journal, January 2020

    • Garg, Sahil; Li, Mengran; Weber, Adam Z.
    • Journal of Materials Chemistry A, Vol. 8, Issue 4
    • DOI: 10.1039/c9ta13298h

    Current achievements and the future direction of electrochemical CO 2 reduction: A short review
    journal, June 2019

    Heterogeneous catalysts for catalytic CO2 conversion into value-added chemicals
    journal, March 2019

    Selective $CO_{2}$ Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte-Driven Nanostructuring
    text, January 2019

    • Gao, Dunfeng; Sinev, Ilya; Scholten, Fabian
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2020-00548

    pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper
    journal, January 2019

    Selective electroreduction of carbon dioxide to methanol on copper selenide nanocatalysts
    journal, February 2019

    Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction
    journal, June 2019

    Carbon dioxide electroreduction to C2 products over copper-cuprous oxide derived from electrosynthesized copper complex
    journal, August 2019

    Theoretical insights into selective electrochemical conversion of carbon dioxide
    journal, March 2019

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