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

Abstract

Here, 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 catalyse C–C coupling for C2+ products, but still suffer from low selectivity in water. Here, we use density functional theory to determine the energetics of the initial C–C coupling steps on different Cu facets in CO2 reduction, and suggest that the Cu(100) and stepped (211) facets favour C2+ product formation over Cu(111). To demonstrate this, we report the tuning of facet exposure on Cu foil through the metal ion battery cycling method. Compared with the polished Cu foil, our 100-cycled Cu nanocube catalyst with exposed (100) facets presents a sixfold improvement in C2+ to C1 product ratio, with a highest C2+ Faradaic efficiency of over 60% and H2 below 20%, and a corresponding C2+ current of more than 40 mA cm–2.

Authors:
ORCiD logo [1];  [2];  [1];  [2];  [1];  [3];  [3]; ORCiD logo [1]
  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 Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (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. https://doi.org/10.1038/s41929-017-0009-x.
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
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.
@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 = {Here, 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 catalyse C–C coupling for C2+ products, but still suffer from low selectivity in water. Here, we use density functional theory to determine the energetics of the initial C–C coupling steps on different Cu facets in CO2 reduction, and suggest that the Cu(100) and stepped (211) facets favour C2+ product formation over Cu(111). To demonstrate this, we report the tuning of facet exposure on Cu foil through the metal ion battery cycling method. Compared with the polished Cu foil, our 100-cycled Cu nanocube catalyst with exposed (100) facets presents a sixfold improvement in C2+ to C1 product ratio, with a highest C2+ Faradaic efficiency of over 60% and H2 below 20%, and a corresponding C2+ current of more than 40 mA cm–2.},
doi = {10.1038/s41929-017-0009-x},
journal = {Nature Catalysis},
number = 2,
volume = 1,
place = {United States},
year = {2018},
month = {1}
}

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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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    • Meng, Nannan; Liu, Cuibo; Liu, Yang
    • Angewandte Chemie International Edition, Vol. 58, Issue 52
    • 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


    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


    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


    Isolated Ni single atoms in graphene nanosheets for high-performance CO 2 reduction
    journal, January 2018

    • Jiang, Kun; Siahrostami, Samira; Zheng, Tingting
    • Energy & Environmental Science, Vol. 11, Issue 4
    • DOI: 10.1039/c7ee03245e

    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

    CO 2 reduction on gas-diffusion electrodes and why catalytic performance must be assessed at commercially-relevant conditions
    journal, January 2019

    • Burdyny, Thomas; Smith, Wilson A.
    • Energy & Environmental Science, Vol. 12, Issue 5
    • DOI: 10.1039/c8ee03134g

    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

    Zn-Doped Cu(100) facet with efficient catalytic ability for the CO 2 electroreduction to ethylene
    journal, January 2019

    • Zhang, Yuefeng; Zhao, Yong; Wang, Caiyun
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 38
    • DOI: 10.1039/c9cp03692j

    Highly efficient electroconversion of carbon dioxide into hydrocarbons by cathodized copper–organic frameworks
    journal, January 2019

    • Yang, Fan; Chen, Aling; Deng, Pei Lin
    • Chemical Science, Vol. 10, Issue 34
    • DOI: 10.1039/c9sc02605c

    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

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


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.