Bridging the Surface Charge and Catalytic Activity of a Defective Carbon Electrocatalyst

Electrocatalysis is dominated by reaction at the solid–liquid–gas interface; surface properties of electrocatalysts determine the electrochemical behavior. The surface charge of active sites on catalysts modulate adsorption and desorption of intermediates. However, there is no direct evidence to bri...

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Published inAngewandte Chemie International Edition Vol. 58; no. 4; pp. 1019 - 1024
Main Authors Tao, Li, Qiao, Man, Jin, Rong, Li, Yan, Xiao, Zhaohui, Wang, Yuqing, Zhang, Nana, Xie, Chao, He, Qinggang, Jiang, Dechen, Yu, Gang, Li, Yafei, Wang, Shuangyin
Format Journal Article
LanguageEnglish
Published Germany Wiley Subscription Services, Inc 21.01.2019
EditionInternational ed. in English
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Summary:Electrocatalysis is dominated by reaction at the solid–liquid–gas interface; surface properties of electrocatalysts determine the electrochemical behavior. The surface charge of active sites on catalysts modulate adsorption and desorption of intermediates. However, there is no direct evidence to bridge surface charge and catalytic activity of active sites. Defects (active sites) were created on a HOPG (highly oriented pyrolytic graphite) surface that broke the intrinsic sp2‐hybridization of graphite by plasma, inducing localization of surface charge onto defective active sites, as shown by scanning ion conductance microscopy (SICM) and Kelvin probe force microscopy (KPFM). An electrochemical test revealed enhanced intrinsic activity by the localized surface charge. DFT calculations confirmed the relationship between surface charge and catalytic activity. This work correlates surface charge and catalytic activity, providing insights into electrocatalytic behavior and guiding the design of advanced electrocatalysts. Highly oriented pyrolytic graphite (HOPG) was employed as a model to analyze the promotion of surface charge for electrocatalytic reactions. Via plasma irradiation, numerous defects are generated, which would induce charge re‐distribution on the surface of HOPG. A direct relationship between surface charge and the electrocatalytic activity is proposed.
Bibliography:These authors contributed equally to this work.
ObjectType-Article-1
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content type line 23
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201810207