Spatially and Temporally Resolved Dynamic Response of Co-Based Composite Interface during the Oxygen Evolution Reaction | |
Zhong, Xia1,2,3; Xu, Jingyao1; Chen, Junnan2,3; Wang, Xiyang4; Zhu, Qian1; Zeng, Hui1; Zhang, Yaowen1; Pu, Yinghui2,3; Hou, Xiangyan1; Wu, Xiaofeng1; Niu, Yiming2,3; Zhang, Wei5,6; Wu, Yimin A.4; Wang, Ying7; Zhang, Bingsen2,3; Huang, Keke1; Feng, Shouhua1 | |
通讯作者 | Wang, Ying(ywang_2012@ciac.ac.cn) ; Zhang, Bingsen(bszhang@imr.ac.cn) ; Huang, Keke(kkhuang@jlu.edu.cn) ; Feng, Shouhua(shfeng@jlu.edu.cn) |
2024-03-06 | |
发表期刊 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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ISSN | 0002-7863 |
卷号 | 146期号:11页码:7467-7479 |
摘要 | Interfacial interaction dictates the overall catalytic performance and catalytic behavior rules of the composite catalyst. However, understanding of interfacial active sites at the microscopic scale is still limited. Importantly, identifying the dynamic action mechanism of the "real" active site at the interface necessitates nanoscale, high spatial-time-resolved complementary-operando techniques. In this work, a Co3O4 homojunction with a well-defined interface effect is developed as a model system to explore the spatial-correlation dynamic response of the interface toward oxygen evolution reaction. Quasi in situ scanning transmission electron microscopy-electron energy-loss spectroscopy with high spatial resolution visually confirms the size characteristics of the interface effect in the spatial dimension, showing that the activation of active sites originates from strong interfacial electron interactions at a scale of 3 nm. Multiple time-resolved operando spectroscopy techniques explicitly capture dynamic changes in the adsorption behavior for key reaction intermediates. Combined with density functional theory calculations, we reveal that the dynamic adjustment of multiple adsorption configurations of intermediates by highly activated active sites at the interface facilitates the O-O coupling and *OOH deprotonation processes. The dual dynamic regulation mechanism accelerates the kinetics of oxygen evolution and serves as a pivotal factor in promoting the oxygen evolution activity of the composite structure. The resulting composite catalyst (Co-B@Co3O4/Co3O4 NSs) exhibits an approximately 70-fold turnover frequency and 20-fold mass activity than the monomer structure (Co3O4 NSs) and leads to significant activity (eta(10) similar to 257 mV). The visual complementary analysis of multimodal operando/in situ techniques provides us with a powerful platform to advance our fundamental understanding of interfacial structure-activity relationships in composite structured catalysts. |
资助者 | National Key Research and Development Program of China ; National Natural Science Foundation of China ; Jilin Province Science and Technology Development Plan ; National Key R&D Program of China |
DOI | 10.1021/jacs.3c12820 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | National Key Research and Development Program of China[22090044] ; National Key Research and Development Program of China[21831003] ; National Key Research and Development Program of China[22373097] ; National Key Research and Development Program of China[22171102] ; National Natural Science Foundation of China[20200802003GH] ; National Natural Science Foundation of China[20200801005GH] ; National Natural Science Foundation of China[20210509035RQ] ; Jilin Province Science and Technology Development Plan[2021YFF0500502] ; National Key R&D Program of China |
WOS研究方向 | Chemistry |
WOS类目 | Chemistry, Multidisciplinary |
WOS记录号 | WOS:001180644900001 |
出版者 | AMER CHEMICAL SOC |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/184706 |
专题 | 中国科学院金属研究所 |
通讯作者 | Wang, Ying; Zhang, Bingsen; Huang, Keke; Feng, Shouhua |
作者单位 | 1.Jilin Univ, Preparat Chem Coll Chem, State Key Lab Inorgan Synth, Changchun 130012, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 4.Univ Waterloo, Waterloo Inst Nanotechnol, Dept Mech & Mechatron Engn, Waterloo, ON N2L 3G1, Canada 5.Jilin Univ, Electron Microscopy Ctr, Changchun 130012, Peoples R China 6.Jilin Univ, Jilin Prov Int Cooperat Key Lab High Efficiency Cl, Changchun 130012, Peoples R China 7.Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Jilin, Peoples R China |
推荐引用方式 GB/T 7714 | Zhong, Xia,Xu, Jingyao,Chen, Junnan,et al. Spatially and Temporally Resolved Dynamic Response of Co-Based Composite Interface during the Oxygen Evolution Reaction[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146(11):7467-7479. |
APA | Zhong, Xia.,Xu, Jingyao.,Chen, Junnan.,Wang, Xiyang.,Zhu, Qian.,...&Feng, Shouhua.(2024).Spatially and Temporally Resolved Dynamic Response of Co-Based Composite Interface during the Oxygen Evolution Reaction.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(11),7467-7479. |
MLA | Zhong, Xia,et al."Spatially and Temporally Resolved Dynamic Response of Co-Based Composite Interface during the Oxygen Evolution Reaction".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.11(2024):7467-7479. |
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