Cited by 201CO2 Reduction Techniques and CatalystsCatalysts for Methane ReformingElectrocatalysts for Energy Conversion

Selective Heterogeneous CO2 Electroreduction to Methanol

Back, Seoin, Kim, Heejin, Jung, Yousung·2015·ACS Catalysis

Abstract

Catalytic electroreduction of carbon dioxide to useful chemical feedstocks is an environmentally and technologically important process, yet the low energy efficiency and difficulty in controlling product selectivity are great challenges. The reason for part of the latter is that there are presently no catalyst design principles to selectively control CO 2 electroreduction toward a desired product. In this work, as a first attempt, we suggest combining a few criteria (CO binding energy, OH binding energy, and H binding energy) that can be collectively used as activity- and selectivity-determining descriptors to preferentially produce methanol over methane from CO 2 electroreduction. We then apply these concepts to near-surface alloys (NSAs) to propose efficient and selective CO 2 electrochemical reduction catalysts to produce methanol. The W/Au alloy is identified as a promising candidate to have increased catalyst efficiency (decreased CO 2 reduction overpotential and increased overpotential for unwanted hydrogen evolution) as well as improved product selectivity toward methanol, in comparison to conventional Cu catalyst.

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Crossref · 10.1021/cs501600x

Cites

52 of 52 references verified0 citation errors · 0 not checkable

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  • A strong correlation between binding energies of various reaction intermediates on transition metals and a lack of ability to independently control them poses a significant intrinsic limitation in developing suitable catalysts for large-scale commercialization of the CO2 reduction reaction.

    “general understanding at present is that a strong correlation between binding energies of various reaction intermediates on transition metals and a lack of ability to independently control them poses a significant intrinsic limitation in developing suitable catalysts for large-scale commercialization of the CO2 reduction reaction.”
  • The predicted theoretical limiting potential for CH3OH production using Pt@dv-Gr is significantly less negative than any catalysts that produce CH4 or CH3OH in the literature, whether synthesized (-0.5 to -1.0 V) or predicted (-0.3 to -1.0 V).

    “In particular, as in the free energy diagram shown in Fig. 4 in detail, the predicted theoretical limiting potential (U L) for CH3OH production using Pt@dv-Gr is significantly less negative than any catalysts that produce CH4 or CH3OH in the literature, synthesized (–0.5 to –1.0 V)35,37,38 or predicted (–0.3 V to –1.0 V).4,6,39,40”
  • The theoretical limiting potentials for CH4 production on Ni (211), Pt (211) and Cu (211) surfaces are -0.7 to -0.8 V vs. RHE.

    “For example, the theoretical limiting potentials for CH4 production on Ni (211), Pt (211) and Cu (211) surfaces are –0.7 to –0.8 V vs. RHE.4”
  • The experimental product selectivity is significantly different for Ni, Pt and Cu, even though their theoretical limiting potentials for the CO2 reduction reaction are similar.

    “It is thus noteworthy that the experimental product selectivity is significantly different for Ni, Pt and Cu, even though their theoretical limiting potentials for the CO2 reduction reaction are similar.”

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Authors
Back, S., Kim, H., & Jung, Y.
Affiliations
Korea Advanced Institute of Science and Technology (KR)
Corresponding author
Jung, Yousung
Venue
ACS Catalysis
Published
2015-01-09
Volume
5
Issue
2
Pages
965-971
ISSN
2155-5435 (ISSN-L)
OpenAlex
W2559810192
Cited by
201
References
53
Citations by year
2026: 9 · 2025: 13 · 2024: 16 · 2023: 19 · 2022: 13 · 2021: 22 · 2020: 23 · 2019: 15 · 2018: 23 · 2017: 24 · 2016: 13 · 2015: 11
FWCI
5.28
Type
journal article
Language
en
Open access
closed
Locations
ACS Catalysis (publishedVersion)
Funders
  • National Research Foundation of Korea (NRF-2014H1A2A1016055)
  • Korea Carbon Capture & Sequestration R&D Center
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, methanol synthesis, heterogeneous electrocatalysis, product selectivity, CO binding energy, hydrogen evolution suppression

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