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231227s2024 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202310052
|2 doi
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|a pubmed24n1353.xml
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|a eng
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|a Zhao, Zhiqiang
|e verfasserin
|4 aut
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|a Enhanced Electron Delocalization within Coherent Nano-Heterocrystal Ensembles for Optimizing Polysulfide Conversion in High-Energy-Density Li-S Batteries
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|c 2024
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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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|a Date Revised 28.03.2024
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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 Commercialization of high energy density Lithium-Sulfur (Li-S) batteries is impeded by challenges such as polysulfide shuttling, sluggish reaction kinetics, and limited Li+ transport. Herein, a jigsaw-inspired catalyst design strategy that involves in situ assembly of coherent nano-heterocrystal ensembles (CNEs) to stabilize high-activity crystal facets, enhance electron delocalization, and reduce associated energy barriers is proposed. On the catalyst surface, the stabilized high-activity facets induce polysulfide aggregation. Simultaneously, the surrounded surface facets with enhanced activity promote Li2S deposition and Li+ diffusion, synergistically facilitating continuous and efficient sulfur redox. Experimental and DFT computations results reveal that the dual-component hetero-facet design alters the coordination of Nb atoms, enabling the redistribution of 3D orbital electrons at the Nb center and promoting d-p hybridization with sulfur. The CNE, based on energy level gradient and lattice matching, endows maximum electron transfer to catalysts and establishes smooth pathways for ion diffusion. Encouragingly, the NbN-NbC-based pouch battery delivers a Weight energy density of 357 Wh kg-1, thereby demonstrating the practical application value of CNEs. This work unveils a novel paradigm for designing high-performance catalysts, which has the potential to shape future research on electrocatalysts for energy storage applications
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|a Journal Article
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|a catalytic conversion
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|a coherent nano‐heterocrystal
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|a electron delocalization
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|a lithium‐sulfur battery
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| 650 |
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|a polysulfide adsorption
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1 |
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|a Pan, Yukun
|e verfasserin
|4 aut
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|a Yi, Shan
|e verfasserin
|4 aut
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1 |
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|a Su, Zhe
|e verfasserin
|4 aut
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|a Chen, Hongli
|e verfasserin
|4 aut
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|a Huang, Yanan
|e verfasserin
|4 aut
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| 700 |
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|a Niu, Bo
|e verfasserin
|4 aut
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| 700 |
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|a Long, Donghui
|e verfasserin
|4 aut
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| 700 |
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|a Zhang, Yayun
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 36(2024), 13 vom: 28. März, Seite e2310052
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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|g volume:36
|g year:2024
|g number:13
|g day:28
|g month:03
|g pages:e2310052
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|u http://dx.doi.org/10.1002/adma.202310052
|3 Volltext
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