Cited by 702CO2 Reduction Techniques and CatalystsElectrocatalysts for Energy ConversionCatalysts for Methane Reforming

Electric Field Effects in Electrochemical CO 2 Reduction

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Chen, Leanne D., Urushihara, Makoto, Chan, Karen, Nørskov, Jens K.·2016·ACS Catalysis

Abstract

Electrochemical reduction of CO 2 has the potential to reduce greenhouse gas emissions while providing energy storage and producing chemical feedstocks. A mechanistic understanding of the process is crucial to the discovery of efficient catalysts, and an atomistic description of the electrochemical interface is a major challenge due to its complexity. Here, we examine the CO 2 → CO electrocatalytic pathway on Ag(111) using density functional theory (DFT) calculations and an explicit model of the electrochemical interface. We show that the electric field from solvated cations in the double layer and their corresponding image charges on the metal surface significantly stabilizes key intermediates—*CO 2 and *COOH. At the field-stabilized sites, the formation of *CO is rate-determining. We present a microkinetic model that incorporates field effects and electrochemical barriers from ab initio calculations. The computed polarization curves show reasonable agreement with experiment without fitting any parameters.

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Cited by

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Authors
Chen, L. D., Urushihara, M., Chan, K., & Nørskov, J. K.
Affiliations
  • SLAC National Accelerator Laboratory (US)
  • Mitsubishi Materials (Japan) (JP)
Corresponding author
Nørskov, Jens K.
Venue
ACS Catalysis
Published
2016-09-26
Volume
6
Issue
10
Pages
7133-7139
ISSN
2155-5435 (ISSN-L)
OpenAlex
W2522135447
Cited by
702
References
62
Citations by year
2026: 85 · 2025: 115 · 2024: 104 · 2023: 80 · 2022: 75 · 2021: 66 · 2020: 56 · 2019: 49 · 2018: 45 · 2017: 25 · 2016: 2
FWCI
10.93
Type
journal article
Language
en
Open access
Locations
  • ACS Catalysis (publishedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
Funders
  • Basic Energy Sciences
  • Office of Science (DE-SC0004993)
  • Natural Sciences and Engineering Research Council of Canada
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
Keywords
electrochemical CO2 reduction, electric field effects, Ag(111), electric double layer, image charges, intermediate stabilization, microkinetic model, polarization curves, electrochemical interfaces

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