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

Tao, L (Tao, Li)[ 1 ] ; Qiao, M (Qiao, Man)[ 2 ] ; Jin, R (Jin, Rong)[ 3 ] ; Li, Y (Li, Yan)[ 2 ] ; Xiao, ZH (Xiao, Zhaohui)[ 1 ] ; Wang, YQ (Wang, Yuqing)[ 1 ] ; Zhang, NN (Zhang, Nana)[ 1 ] ; Xie, C (Xie, Chao)[ 1 ] ; He, QG (He, Qinggang)[ 4 ] ; Jiang, DC (Jiang, Dechen)[ 3 ] ; Yu, G (Yu, Gang)[ 1 ]* ; Li, YF (Li, Yafei)*（李亞飛）; Wang, SY (Wang, Shuangyin)[ 1 ]*

[ 1 ] Hunan Univ, Coll Chem & Chem Engn, Prov Hunan Key Lab Graphene Mat & Devices, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China

[ 2 ] Nanjing Normal Univ, Sch Chem & Mat Sci, Nanjing 210023, Jiangsu, Peoples R China

[ 3 ] Nanjing Univ, Sch Chem & Chem Engn, Nanjing 210093, Jiangsu, Peoples R China

[ 4 ] Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION，201901,58(4),1019-1024

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 sp(2)-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.

文章鏈接：

https://onlinelibrary.wiley.com/doi/full/10.1002/anie.201810207

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