Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper

Li, Christina W.; Ciston, Jim; Kanan, Matthew W.

doi:10.1038/nature13249

Cited by 1,728CO2 Reduction Techniques and CatalystsCatalysts for Methane ReformingElectrocatalysts for Energy Conversion

Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper

Li, Christina W., Ciston, Jim, Kanan, Matthew W.·2014·Nature

DOI 10.1038/nature13249

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Abstract

The electrochemical conversion of CO2 and H2O into liquid fuel is ideal for high-density renewable energy storage and could provide an incentive for CO2 capture. However, efficient electrocatalysts for reducing CO2 and its derivatives into a desirable fuel are not available at present. Although many catalysts can reduce CO2 to carbon monoxide (CO), liquid fuel synthesis requires that CO is reduced further, using H2O as a H(+) source. Copper (Cu) is the only known material with an appreciable CO electroreduction activity, but in bulk form its efficiency and selectivity for liquid fuel are far too low for practical use. In particular, H2O reduction to H2 outcompetes CO reduction on Cu electrodes unless extreme overpotentials are applied, at which point gaseous hydrocarbons are the major CO reduction products. Here we show that nanocrystalline Cu prepared from Cu2O ('oxide-derived Cu') produces multi-carbon oxygenates (ethanol, acetate and n-propanol) with up to 57% Faraday efficiency at modest potentials (-0.25 volts to -0.5 volts versus the reversible hydrogen electrode) in CO-saturated alkaline H2O. By comparison, when prepared by traditional vapour condensation, Cu nanoparticles with an average crystallite size similar to that of oxide-derived copper produce nearly exclusive H2 (96% Faraday efficiency) under identical conditions. Our results demonstrate the ability to change the intrinsic catalytic properties of Cu for this notoriously difficult reaction by growing interconnected nanocrystallites from the constrained environment of an oxide lattice. The selectivity for oxygenates, with ethanol as the major product, demonstrates the feasibility of a two-step conversion of CO2 to liquid fuel that could be powered by renewable electricity.

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Only <1% of the original 18O content remained after only ∼10 min of reaction at -1.0 V vs RHE, indicating that residual oxides are unstable in OD Cu catalysts.
“Only <1 % of the original 18 O content remained after only ∼10 min of reaction at -1.0 V vs RHE, indicating that residual oxides are unstable in OD Cu catalysts.”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [105]

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Authors: Li, C. W., Ciston, J., & Kanan, M. W.
Affiliations: Stanford University (US)
Lawrence Berkeley National Laboratory (US)
Corresponding author: Kanan, Matthew W.
ORCID: Li, Christina W.
Ciston, Jim
Kanan, Matthew W.
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2014-04
Volume: 508
Issue: 7497
Pages: 504-507
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/nature13249
OpenAlex: W1991003106
Cited by: 1,728
References: 32
Citations by year: 2026: 86 · 2025: 122 · 2024: 153 · 2023: 174 · 2022: 158 · 2021: 182 · 2020: 183 · 2019: 190 · 2018: 151 · 2017: 135 · 2016: 93 · 2015: 76 · 2014: 23
FWCI: 35.86
Type: journal article
Language: en
Open access: closed
Licence: www.springer.com/tdm (tdm)
Locations: Nature (publishedVersion)
PubMed (publishedVersion)
RePEc: Research Papers in Economics (submittedVersion)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Keywords: electrochemical CO2 reduction, liquid fuel synthesis, oxide-derived copper, nanocrystalline copper, copper oxide, ethanol production, acetate, 1-propanol, hydrogen evolution suppression, Faradaic efficiency, renewable energy storage, CO2 capture, alkaline water electrolysis

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Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper

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