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- Title
Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production.
- 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
- Abstract
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.
- Subjects
CARBON-based materials; HYDROGEN peroxide; HYDROGEN production; ELECTROCATALYSTS; OXYGEN reduction; HYDROGEN evolution reactions
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-41947-7