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Bottom-Up Construction of Active Sites in a Cu-N-4-C Catalyst for Highly Efficient Oxygen Reduction Reaction
Li, Wei1,2; Min, Chungang2; Tan, Feng1,2; Li, Zhanping3; Zhang, Bingsen4; Si, Rui5; Xu, Mingli6; Liu, Weiping1; Zhou, Liexing2; Wei, Qingmao1,2; Zhang, Yuzhen1,2; Yang, Xikun1,2
通讯作者Yang, Xikun(yxk630@hotmail.com)
2019-03-01
发表期刊ACS NANO
ISSN1936-0851
卷号13期号:3页码:3177-3187
摘要Bottom-up construction of efficient active sites in transition metal-nitrogen-carbon (M-N-C) catalysts for oxygen reduction reaction (ORR) from single molecular building blocks remains one of the most difficult challenges. Herein, we report a bottom-up approach to produce a highly active Cu-N-4-C catalyst with well-defined Cu-N-4 coordination sites derived from a small molecular copper complex containing Cu-N-4 moieties. The Cu-N-4 moieties were found to be covalently integrated into graphene sheets to create the Cu-N-4 active sites for ORR. Furthermore, the activity was boosted by tuning the structure of active sites. We find that the high ORR activity of the Cu-N-4-C catalyst is related to the Cu-N-4 center linked to edges of the graphene sheets, where the electronic structure of the Cu center has the right symmetry for the degenerate pi* orbital of the O-2 molecule. These findings point out the direction for the synthesis of the M-N-C catalysts at the molecular level.
关键词bottom-up fabrication single molecular building blocks ORR Cu-N-4 active sites orbital symmetry
资助者National Natural Science Foundation of China
DOI10.1021/acsnano.8b08692
收录类别SCI
语种英语
资助项目National Natural Science Foundation of China[21363012] ; National Natural Science Foundation of China[51374117] ; National Natural Science Foundation of China[11764026] ; National Natural Science Foundation of China[51764030]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号WOS:000462950500045
出版者AMER CHEMICAL SOC
引用统计
被引频次:107[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/132576
专题中国科学院金属研究所
通讯作者Yang, Xikun
作者单位1.Kunming Univ Sci & Technol, Fac Mat Sci & Engn, Kunming 650093, Yunnan, Peoples R China
2.Kunming Univ Sci & Technol, Res Ctr Anal & Measurement, Kunming 650093, Yunnan, Peoples R China
3.Tsinghua Univ, Anal Ctr, Beijing 100080, Peoples R China
4.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China
5.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
6.Kunming Univ Sci & Technol, Fac Met & Energy Engn, Kunming 650093, Yunnan, Peoples R China
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GB/T 7714
Li, Wei,Min, Chungang,Tan, Feng,et al. Bottom-Up Construction of Active Sites in a Cu-N-4-C Catalyst for Highly Efficient Oxygen Reduction Reaction[J]. ACS NANO,2019,13(3):3177-3187.
APA Li, Wei.,Min, Chungang.,Tan, Feng.,Li, Zhanping.,Zhang, Bingsen.,...&Yang, Xikun.(2019).Bottom-Up Construction of Active Sites in a Cu-N-4-C Catalyst for Highly Efficient Oxygen Reduction Reaction.ACS NANO,13(3),3177-3187.
MLA Li, Wei,et al."Bottom-Up Construction of Active Sites in a Cu-N-4-C Catalyst for Highly Efficient Oxygen Reduction Reaction".ACS NANO 13.3(2019):3177-3187.
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