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

Wu，Qilong1,2,3; Zou，Haiyuan4; Mao，Xin5; He，Jinghan1; Shi，Yanmei6; Chen，Shuangming7; Yan，Xuecheng3; Wu，Liyun1; Lang，Chengguang3,8; Zhang，Bin6; Song，Li7; Wang，Xin9,10; Du，Aijun5; Li，Qin3; Jia，Yi9,10; Chen，Jun2; Yao，Xiangdong1,8

2023-12-01

10.1038/s41467-023-41947-7

Nature Communications   影响因子和分区

2041-1723

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.

SCI

英语

NI论文

其他

2-s2.0-85173665483

Scopus

1.State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,College of Chemistry,Jilin University,Changchun,130012,China
2.Intelligent Polymer Research Institute,Australian Institute for Innovative Materials,Innovation Campus,University of Wollongong,Squires Way,North Wollongong,2500,Australia
3.School of Environmental engineering and Built Environment,Griffith University,Brisbane,Nathan Campus,4111,Australia
4.Guangdong Provincial Key Laboratory of Energy Materials for Electric Power,Southern University of Science and Technology,Shenzhen,518055,China
5.School of Chemistry and Physics and Centre for Materials Science,Queensland University of Technology,Gardens Point Campus,Brisbane,4001,Australia
6.School of Science,Institute of Molecular Plus,Tianjin University,Tianjin,300072,China
7.Hefei National Laboratory for Physical Sciences at the Microscale,iChEM (Collaborative Innovation Center of Chemistry for Energy Materials),School of Chemistry and Materials Science,and National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei,Anhui,230026,China
8.School of Advanced Energy,Sun Yat-Sen University (Shenzhen),Shenzhen,Guangdong,518107,China
9.Petroleum and Chemical Industry Key Laboratory of Organic Electrochemical Synthesis,College of Chemical Engineering,and Zhejiang Moganshan Carbon Neutral Innovation Institute,Zhejiang University of Technology,Hangzhou,18 Chaowang Road, Gongshu District,310032,China
10.Zhejiang Carbon Neutral Innovation Institute,Moganshan Institute ZJUT,Kangqian District,Deqing,313200,China

Wu，Qilong,Zou，Haiyuan,Mao，Xin,et al. Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production[J]. Nature Communications,2023,14(1).

Wu，Qilong.,Zou，Haiyuan.,Mao，Xin.,He，Jinghan.,Shi，Yanmei.,...&Yao，Xiangdong.(2023).Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production.Nature Communications,14(1).

Wu，Qilong,et al."Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production".Nature Communications 14.1(2023).