Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production
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Date
2023
Authors
Wu, Q.
Zou, H.
Mao, X.
He, J.
Shi, Y.
Chen, S.
Yan, X.
Wu, L.
Lang, C.
Zhang, B.
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Journal article
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Nature Communications, 2023; 14(1):6275-1-6275-11
Statement of Responsibility
Qilong Wu, Haiyuan Zou, XinMao, JinghanHe, Yanmei Shi, Shuangming Chen, Xuecheng Yan, LiyunWu, Chengguang Lang, Bin Zhang, Li Song, XinWang, Aijun Du, Qin Li, Yi Jia, Jun Chen and Xiangdong Yao
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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.
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Published online: 07 October 2023
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© The Author(s) 2023. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/ licenses/by/4.0/.