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

Qilong Wu, Haiyuan Zou, Xin Mao, Jinghan He, Yanmei Shi, Shuangming Chen, Xuecheng Yan, Liyun Wu, Chengguang Lang, Bin Zhang, Li Song, Xin Wang, Aijun Du, Qin Li, Yi Jia (), Jun Chen () and Xiangdong Yao ()
Additional contact information
Qilong Wu: Jilin University
Haiyuan Zou: Southern University of Science and Technology
Xin Mao: Queensland University of Technology, Gardens Point Campus
Jinghan He: Jilin University
Yanmei Shi: Tianjin University
Shuangming Chen: University of Science and Technology of China
Xuecheng Yan: Griffith University, Nathan Campus
Liyun Wu: Jilin University
Chengguang Lang: Griffith University, Nathan Campus
Bin Zhang: Tianjin University
Li Song: University of Science and Technology of China
Xin Wang: Zhejiang University of Technology
Aijun Du: Queensland University of Technology, Gardens Point Campus
Qin Li: Griffith University, Nathan Campus
Yi Jia: Zhejiang University of Technology
Jun Chen: University of Wollongong, Squires Way
Xiangdong Yao: Jilin University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-41947-7

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