Stabilizing Copper for CO2 Reduction in Low-Grade Electrolyte

  • Jingfu He
    Jingfu He
    Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada
    More by Jingfu He
  • Aoxue Huang
    Aoxue Huang
    Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada
    More by Aoxue Huang
  • Noah J. J. Johnson
    Noah J. J. Johnson
    Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada
  • Kevan E. Dettelbach
    Kevan E. Dettelbach
    Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada
  • David M. Weekes
    David M. Weekes
    Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada
  • Yang Cao
    Yang Cao
    Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada
    More by Yang Cao
  • , and 
  • Curtis P. Berlinguette*
    Curtis P. Berlinguette
    Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada
    Department of Chemical & Biological Engineering, The University of British Columbia, 2360 East Mall, Vancouver, British Columbia V6T 1Z3, Canada
    Stewart Blusson Quantum Matter Institute, The University of British Columbia, 2355 East Mall, Vancouver, British Columbia V6T 1Z4, Canada
    *E-mail: [email protected]
Cite this: Inorg. Chem. 2018, 57, 23, 14624–14631
Publication Date (Web):November 13, 2018
https://doi.org/10.1021/acs.inorgchem.8b02311
Copyright © 2018 American Chemical Society
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Abstract

We demonstrate herein a CO2 reduction electrocatalyst regeneration strategy based on the manipulation of the Cu(0)/Cu2+ equilibrium with high concentrations of ethylenediaminetetraacetic acid (EDTA). This strategy enables the sustained performance of copper catalysts in distilled and tap water electrolytes for over 12 h. The deposition of common electrolyte impurities such as iron, nickel, and zinc is blocked because EDTA can effectively bind the metal ions and negatively shift the electrode potential of M/Mn+. The Cu/Cu2+ redox couple is >600 mV more positive than the other metal ions and therefore participates in an equilibrium of dissolution and redeposition from and to the electrode in high concentrations of EDTA. These dynamic equilibria serve to further regenerate the surface copper catalyst to prevent the deactivation of catalytic sites. On the basis of this strategy, we show that >95% of initial hydrocarbon production activity can be maintained for 12 h in KHCO3 (99% purity) enriched distilled water and 6 h in KHCO3 (99% purity) enriched tap water.

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  • XRD patterns, SEM images, NMR spectra, and CO2 electrochemical reduction performances (PDF)

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This article is cited by 12 publications.

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