Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production

Active sites identification in metal-free carbon materials is crucial for developing practical electrocatalysts, but resolving precise configuration of active site remains a challenge because of the elusive dynamic structural evolution process during reactions. Here, we reveal the dynamic active sit...

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Bibliographic Details
Published in:Nature communications 2023-10, Vol.14 (1), p.6275-6275, Article 6275
Main Authors: Wu, Qilong, Zou, Haiyuan, Mao, Xin, He, Jinghan, Shi, Yanmei, Chen, Shuangming, Yan, Xuecheng, Wu, Liyun, Lang, Chengguang, Zhang, Bin, Song, Li, Wang, Xin, Du, Aijun, Li, Qin, Jia, Yi, Chen, Jun, Yao, Xiangdong
Format: Article
Language:English
Subjects:
147/137
639/301/299/886
639/638/77/886
Carbon
Carbonyl compounds
Carbonyls
Configurations
Defects
Density
Electrocatalysts
Electrochemistry
Evolution
Graphene
Humanities and Social Sciences
Hydrogen peroxide
Intermediates
multidisciplinary
Oxygen
Performance evaluation
Science
Science (multidisciplinary)
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Summary:Active sites identification in metal-free carbon materials is crucial for developing practical electrocatalysts, but resolving precise configuration of active site remains a challenge because of the elusive dynamic structural evolution process during reactions. Here, we reveal the dynamic active site identification process of oxygen modified defective graphene. First, the defect density and types of oxygen groups were precisely manipulated on graphene, combined with electrocatalytic performance evaluation, revealing a previously overlooked positive correlation relationship between the defect density and the 2 e - oxygen reduction performance. An electrocatalytic-driven oxygen groups redistribution phenomenon was observed, which narrows the scope of potential configurations of the active site. The dynamic evolution processes are monitored via multiple in-situ technologies and theoretical spectra simulations, resolving the configuration of major active sites (carbonyl on pentagon defect) and key intermediates (*OOH), in-depth understanding the catalytic mechanism and providing a research paradigm for metal-free carbon materials. Active sites identification in metal-free carbon materials is crucial for developing practical electrocatalysts. Here the authors report a dynamic active site evolution phenomenon on oxygen modified defective graphene during electrochemical H2O2 production.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-023-41947-7