Embedding Covalency into Metal Catalysts for Efficient Electrochemical Conversion of CO2
Abstract
CO2 conversion is an essential technology to develop a sustainable carbon economy for the present and the future. Many studies have focused extensively on the electrochemical conversion of CO2 into various useful chemicals. However, there is not yet a solution of sufficiently high enough efficiency and stability to demonstrate practical applicability. In this work, we use first-principles-based high-throughput screening to propose silver-based catalysts for efficient electrochemical reduction of CO2 to CO while decreasing the overpotential by 0.4-0.5 V. We discovered the covalency-aided electrochemical reaction (CAER) mechanism in which p-block dopants have a major effect on the modulating reaction energetics by imposing partial covalency into the metal catalysts, thereby enhancing their catalytic activity well beyond modulations arising from d-block dopants. In particular, sulfur or arsenic doping can effectively minimize the overpotential with good structural and electrochemical stability. We expect this work to provide useful insights to guide the development of a feasible strategy to overcome the limitations of current technology for electrochemical CO2 conversion.
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High-throughput DFT simulations were used to screen Ag-based catalysts for efficient CO production.
“For instance, highthroughput DFT simulations were used to screen Ag-based catalysts for efficient CO production.[65]”
From Electrochemical CO <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [65]
p-block dopants modulate reaction energetics by imposing partial covalency into the Ag catalyst, thereby enhancing catalytic activity.
“It was found that p-block dopants modulate reaction energetics by imposing partial covalency into the Ag catalyst, thereby enhancing catalytic activity.”
From Electrochemical CO <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [65]
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Self-citation
- Authors
- Lim, H.-K., Shin, H., Goddard, W. A., Hwang, Y. J., Min, B. K., & Kim, H.
- Affiliations
- Korea Advanced Institute of Science and Technology (KR)
- California Institute of Technology (US)
- Korea Institute of Science and Technology (KR)
- Korea University (KR)
- Corresponding author
- Kim, Hyungjun
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-08-05
- Volume
- 136
- Issue
- 32
- Pages
- 11355-11361
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2160905458
- Cited by
- 222
- References
- 28
- Citations by year
- 2026: 5 · 2025: 12 · 2024: 13 · 2023: 21 · 2022: 21 · 2021: 28 · 2020: 20 · 2019: 25 · 2018: 19 · 2017: 19 · 2016: 25 · 2015: 12 · 2014: 2
- FWCI
- 6.36
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- CaltechAUTHORS (California Institute of Technology) (submittedVersion)
- Seoul National University Open Repository (Seoul National University) (submittedVersion)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Physical Sciences › Chemical Engineering › Process Chemistry and Technology › Carbon dioxide utilization in catalysis
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Keywords
- electrochemical CO2 reduction, CO2 to CO conversion, silver catalysts, sulfur doping, arsenic doping, overpotential reduction, high-throughput screening, reaction energetics, catalyst stability
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