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Construction of Co-4 Atomic Clusters to Enable Fe-N-4 Motifs with Highly Active and Durable Oxygen Reduction Performance
Han, Ali1,2; Sun, Wenming3; Wan, Xin4; Cai, Dandan5; Wang, Xijun6; Li, Feng7; Shui, Jianglan4; Wang, Dingsheng2
通讯作者Wang, Dingsheng(wangdingsheng@mail.tsinghua.edu.cn)
2023-06-14
发表期刊ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN1433-7851
页码11
摘要Fe-N-C catalysts with single-atom Fe-N-4 configurations are highly needed owing to the high activity for oxygen reduction reaction (ORR). However, the limited intrinsic activity and dissatisfactory durability have significantly restrained the practical application of proton-exchange membrane fuel cells (PEMFCs). Here, we demonstrate that constructing adjacent metal atomic clusters (ACs) is effective in boosting the ORR performance and stability of Fe-N-4 catalysts. The integration of Fe-N-4 configurations with highly uniform Co-4 ACs on the N-doped carbon substrate (Co-4@/Fe-1@NC) is realized through a "pre-constrained" strategy using Co-4 molecular clusters and Fe(acac)(3) implanted carbon precursors. The as-developed Co-4@/Fe-1@NC catalyst exhibits excellent ORR activity with a half-wave potential (E-1/2) of 0.835 V vs. RHE in acidic media and a high peak power density of 840 mW cm(-2) in a H-2-O-2 fuel cell test. First-principles calculations further clarify the ORR catalytic mechanism on the identified Fe-N-4 that modified with Co-4 ACs. This work provides a viable strategy for precisely establishing atomically dispersed polymetallic centers catalysts for efficient energy-related catalysis.
关键词Atomic Clusters Fuel Cell Oxygen Reduction Reaction Single-Atom Catalysts
资助者National Key R&D Program of China ; National Natural Science Foundation of China ; Natural Science Foundation of Liaoning Province-Outstanding Youth Foundation
DOI10.1002/anie.202303185
收录类别SCI
语种英语
资助项目National Key R&D Program of China[2018YFA0702003] ; National Key R&D Program of China[2021YFA1501500] ; National Natural Science Foundation of China[22202214] ; National Natural Science Foundation of China[21890383] ; National Natural Science Foundation of China[22171157] ; National Natural Science Foundation of China[21875097] ; National Natural Science Foundation of China[22068008] ; Natural Science Foundation of Liaoning Province-Outstanding Youth Foundation[2022-YQ-02]
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
WOS记录号WOS:001006359000001
出版者WILEY-V C H VERLAG GMBH
引用统计
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/178265
专题中国科学院金属研究所
通讯作者Wang, Dingsheng
作者单位1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Peoples R China
2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
3.Capital Normal Univ, Dept Chem, Beijing Key Lab Opt Mat & Photon Devices, Beijing 100048, Peoples R China
4.Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China
5.Sun Yat Sen Univ, Sch Chem Engn & Technol, Zhuhai 519082, Peoples R China
6.Northwestern Univ, Dept Chem & Biol Engn, 2145 Sheridan Rd, Evanston, IL 60208 USA
7.Fudan Univ, Lab Adv Mat, Shanghai Key Lab Mol Catalysis & Innovat Mat, 220 Handan, Shanghai 200433, Peoples R China
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GB/T 7714
Han, Ali,Sun, Wenming,Wan, Xin,et al. Construction of Co-4 Atomic Clusters to Enable Fe-N-4 Motifs with Highly Active and Durable Oxygen Reduction Performance[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023:11.
APA Han, Ali.,Sun, Wenming.,Wan, Xin.,Cai, Dandan.,Wang, Xijun.,...&Wang, Dingsheng.(2023).Construction of Co-4 Atomic Clusters to Enable Fe-N-4 Motifs with Highly Active and Durable Oxygen Reduction Performance.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,11.
MLA Han, Ali,et al."Construction of Co-4 Atomic Clusters to Enable Fe-N-4 Motifs with Highly Active and Durable Oxygen Reduction Performance".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2023):11.
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