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231226s2023 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202209210
|2 doi
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|a pubmed24n1166.xml
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|a (DE-627)NLM349951527
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|a (NLM)36482825
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|a DE-627
|b ger
|c DE-627
|e rakwb
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|a eng
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|a Yu, Jia
|e verfasserin
|4 aut
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|a Breaking the Electronic Conductivity Bottleneck of Manganese Oxide Family for High-Power Fluorinated Graphite Composite Cathode by Ligand-Field High-Dimensional Constraining Strategy
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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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|a Date Completed 24.02.2023
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|a Date Revised 24.02.2023
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2022 Wiley-VCH GmbH.
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|a Primary lithium fluorinated graphite (Li/CFx ) batteries with superior energy density are an indispensable energy supply for multiple fields but suffer from sluggish reaction kinetics of the CFx cathode. Designing composite cathodes emerges as a solution to this problem. Despite the optimal composite component for CFx , the manganese oxide family represented by MnO2 is still faced with an intrinsic electronic conductivity bottleneck, which severely limits the power density of the composite cathode. Here, a cation-induced high-dimensional constraining strategy from the perspective of ligand-field stacking structure topological design, which breaks the molecular orbital hybridization of pristine semiconductive oxides to transform them into the high-conductivity metallic state while competitively maintaining structural stability, is proposed. Through first-principles phase diagram calculations, mixed-valent Mn5 O8 ( Mn 2 2 + Mn 3 4 + O 8 ${\rm{Mn}}_2^{2 + }{\rm{Mn}}_3^{4 + }{{\rm{O}}_8}$ ) is explored as an ideal high-dimensional constraining material with satisfied conductivity and large-scale production feasibility. Experiments demonstrate that the as-proposed CFx Mn5 O8 composite cathode achieves 2.36 times the power density (11399 W kg-1 ) of pristine CFx and a higher CFx conversion ratio (86%). Such a high-dimensional field-constraining strategy is rooted in the established four-quadrant electronic structure tuning framework, which fundamentally changes the orbital symmetry under the ligand field to overcome the common conductivity challenge of wide transition metal oxide materials
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|a Journal Article
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|a electronic conductivities
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|a fluorinated graphite
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|a high-dimensional constraining
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|a ligand-field stacking topology
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|a transition metal oxides
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|a Wang, Da
|e verfasserin
|4 aut
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|a Wang, Guoxin
|e verfasserin
|4 aut
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|a Cui, Yanhua
|e verfasserin
|4 aut
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|a Shi, Siqi
|e verfasserin
|4 aut
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 35(2023), 8 vom: 09. Feb., Seite e2209210
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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|g volume:35
|g year:2023
|g number:8
|g day:09
|g month:02
|g pages:e2209210
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|u http://dx.doi.org/10.1002/adma.202209210
|3 Volltext
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|d 35
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