Space Charge, Modulating the Catalytic Activity of Single-Atom Metal Catalysts

Potential-induced electrode charging is a prerequisite to initiate electrochemical reactions at the electrode-electrolyte interface. The 'interface space charge' could dramatically alter the reaction environment and the charge density of the active site, both of which potentially affect the electrochemical activity. However, our understanding of the electrocatalytic role of space charge has been limited. Here, we separately modulate the amount of space charge (characterized by the areal density, σ) with maintaining the electrochemical potential for the oxygen reduction reaction (ORR) at the same level, by exploiting the unique structural feature of MeNC. We reveal that changes in σ control the ORR activity, which is computationally explained by the inductive polarization of the charge density at the active sites, affecting their turnover rates. To guide catalyst design including the space charge effect, we develop a new descriptor, explaining the activity trend in various metal centers and pH conditions using a single volcano. These findings offer fresh insights into the role of space charge in electrocatalysis, providing a new framework for optimizing catalyst design and performance.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-04-14
DOI
https://doi.org/10.1021/jacs.4c17413
Citations
6
Primary Topic
Electrocatalysts for Energy Conversion
Type
article
Field-Weighted Citation Impact
2.18

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article

Space Charge, Modulating the Catalytic Activity of Single-Atom Metal Catalysts

Hyung‐Suk Oh, Geunsu Bae, Seung‐Jae Shin, Frédéric Jaouen et al.
6 citations
Journal of the American Chemical Society
Electrocatalysts for Energy Conversion
2.18
article

Space Charge, Modulating the Catalytic Activity of Single-Atom Metal Catalysts

Hyung‐Suk Oh, Geunsu Bae, Seung‐Jae Shin, Frédéric Jaouen, Junsic Cho, Man Ho Han, Hansol Choi, Chang Hyuck Choi, Kug‐Seung Lee, Moulay Tahar Sougrati, Hyungjun Kim
article en
6 citations

Abstract

Potential-induced electrode charging is a prerequisite to initiate electrochemical reactions at the electrode-electrolyte interface. The 'interface space charge' could dramatically alter the reaction environment and the charge density of the active site, both of which potentially affect the electrochemical activity. However, our understanding of the electrocatalytic role of space charge has been limited. Here, we separately modulate the amount of space charge (characterized by the areal density, σ) with maintaining the electrochemical potential for the oxygen reduction reaction (ORR) at the same level, by exploiting the unique structural feature of MeNC. We reveal that changes in σ control the ORR activity, which is computationally explained by the inductive polarization of the charge density at the active sites, affecting their turnover rates. To guide catalyst design including the space charge effect, we develop a new descriptor, explaining the activity trend in various metal centers and pH conditions using a single volcano. These findings offer fresh insights into the role of space charge in electrocatalysis, providing a new framework for optimizing catalyst design and performance.

Journal of the American Chemical SocietyVol. 147(16)
École Nationale Supérieure de Chimie de Montpellier (FR), Pohang University of Science and Technology (KR), Centre National de la Recherche Scientifique (FR), Korea Advanced Institute of Science and Technology (KR), Yonsei University (KR), Université de Montpellier (FR), Institut Charles Gerhardt Montpellier (FR), Advanced Institute of Convergence Technology (KR), Clean Energy (United States) (US), Nano Carbon (Poland) (PL), Ulsan National Institute of Science and Technology (KR), Korea Institute of Science and Technology (KR), Sungkyunkwan University (KR)
National Research Foundation of Korea, Samsung Science and Technology Foundation
Openalex Percentile: Top 13%
Electrocatalysts for Energy Conversion
2.18
DOIOpen Access PDFOpenAlex
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