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
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ISSN | 1936-0851 |
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 |
DOI | 10.1021/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 | |
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 |
推荐引用方式 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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