Selective Heterogeneous CO2 Electroreduction to Methanol
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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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.”
From Single-atom catalysts for CO <sub>2</sub> electroreduction with significant activity and selectivity improvements (2017) · cites this paper as [4]
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”
From Single-atom catalysts for CO <sub>2</sub> electroreduction with significant activity and selectivity improvements (2017) · cites this paper as [4]
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”
From Single-atom catalysts for CO <sub>2</sub> electroreduction with significant activity and selectivity improvements (2017) · cites this paper as [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.”
From Single-atom catalysts for CO <sub>2</sub> electroreduction with significant activity and selectivity improvements (2017) · cites this paper as [4]
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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
- Publisher
- American Chemical Society (ACS)
- 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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