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|a 10.1002/adma.202305945
|2 doi
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|a pubmed24n1198.xml
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|a (DE-627)NLM359512968
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|a (NLM)37450565
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|a DE-627
|b ger
|c DE-627
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|a eng
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|a Yuan, Long-Ji
|e verfasserin
|4 aut
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|a d-Orbital Electron Delocalization Realized by Axial Fe4 C Atomic Clusters Delivers High-Performance Fe-N-C Catalysts for Oxygen Reduction Reaction
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|c 2023
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
|b c
|2 rdamedia
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|a ƒa Online-Ressource
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|2 rdacarrier
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|a Date Revised 20.10.2023
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2023 Wiley-VCH GmbH.
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|a Fe-N-C catalyst for oxygen reduction reaction (ORR) has been considered as the most promising nonprecious metal catalyst due to its comparable catalytic performance to Pt in proton exchange membrane fuel cells (PEMFCs). The active centers of Fe-pyrrolic N4 have been proven to be extremely active for ORR. However, forming a stable Fe-pyrrolic N4 structure is a huge challenge. Here, a Cyan-Fe-N-C catalyst with Fe-pyrrolic N4 as the intrinsic active center is constructed with the help of axial Fe4 C atomic clusters, which shows a half-wave potential of up to 0.836 V (vs. RHE) in the acid environment. More remarkably, it delivers a high power density of 870 and 478 mW cm-2 at 1.0 bar in H2 -O2 and H2 -Air fuel cells, respectively. According to theoretical calculation and in situ spectroscopy, the axial Fe4 C can provide strong electronic perturbation to Fe-N4 active centers, leading to the d-orbital electron delocalization of Fe and forming the Fe-pyrrolic N4 bond with high charge distribution, which stabilizes the Fe-pyrrolic N4 structure and optimizes the OH* adsorption during the catalytic process. This work proposes a new strategy to adjust the electronic structure of single-atom catalysts based on the strong interaction between single atoms and atomic clusters
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|a Journal Article
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|a Fe-N-C
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|a atomic clusters
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|a electron delocalization
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|a interaction mechanism
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|a oxygen reduction reaction
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| 700 |
1 |
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|a Liu, Bo
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Shen, Li-Xiao
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Dai, Yun-Kun
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Li, Qi
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Liu, Chang
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Gong, Wei
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Sui, Xu-Lei
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Wang, Zhen-Bo
|e verfasserin
|4 aut
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| 773 |
0 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 35(2023), 39 vom: 11. Sept., Seite e2305945
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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| 773 |
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|g volume:35
|g year:2023
|g number:39
|g day:11
|g month:09
|g pages:e2305945
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|u http://dx.doi.org/10.1002/adma.202305945
|3 Volltext
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|d 35
|j 2023
|e 39
|b 11
|c 09
|h e2305945
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