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241116s2024 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202412598
|2 doi
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|a pubmed24n1644.xml
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|a (DE-627)NLM380298643
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|a (NLM)39543434
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|a eng
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|a Wang, Yihao
|e verfasserin
|4 aut
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|a Low-Spin Fe3+ Evoked by Multiple Defects with Optimal Intermediate Adsorption Attaining Unparalleled Performance in Water Oxidation
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|c 2024
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|a Text
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|a ƒaComputermedien
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|2 rdamedia
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|a ƒa Online-Ressource
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|a Date Revised 28.12.2024
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2024 Wiley‐VCH GmbH.
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|a Electrocatalytic water splitting is long constrained by the sluggish kinetics of anodic oxygen evolution reaction (OER), and rational spin-state manipulation holds great promise to break through this bottleneck. Low-spin Fe3+ (LS, t2g 5eg 0) species are identified as highly active sites for OER in theory, whereas it is still a formidable challenge to construct experimentally. Herein, a new strategy is demonstrated for the effective construction of LS Fe3+ in NiFe-layered double hydroxide (NiFe-LDH) by introducing multiple defects, which induce coordination unsaturation over Fe sites and thus enlarge their d orbital splitting energy. The as-obtained catalyst exhibits extraordinary OER performance with an ultra-low overpotential of 244 mV at the industrially required current density of 500 mA cm-2, which is 110 mV lower than that of the conventional NiFe-LDH with high-spin Fe3+ (HS, t2g 3eg 2) and superior to most previously reported NiFe-based catalysts. Comprehensive experimental and theoretical studies reveal that LS Fe3+ configuration effectively reduces the adsorption strength of the O* intermediate compared with that of the HS case, thereby altering the rate-determining step from (O* → OOH*) to (OH* → O*) of OER and lowering its reaction energy barrier. This work paves a new avenue for developing efficient spin-dependent electrocatalysts for OER and beyond
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|a Journal Article
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|a defect engineering
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|a layered double hydroxides
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|a low‐spin Fe3+
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|a spin state regulation
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|a water oxidation
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|a Li, Shanqing
|e verfasserin
|4 aut
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|a Hou, Xu
|e verfasserin
|4 aut
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|a Cui, Tingting
|e verfasserin
|4 aut
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|a Zhuang, Zechao
|e verfasserin
|4 aut
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|a Zhao, Yunhe
|e verfasserin
|4 aut
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|a Wang, Haozhi
|e verfasserin
|4 aut
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|a Wei, Wei
|e verfasserin
|4 aut
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|a Xu, Ming
|e verfasserin
|4 aut
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|a Fu, Qiang
|e verfasserin
|4 aut
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|a Chen, Chunxia
|e verfasserin
|4 aut
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| 700 |
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|a Wang, Dingsheng
|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), 52 vom: 02. Dez., Seite e2412598
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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|g volume:36
|g year:2024
|g number:52
|g day:02
|g month:12
|g pages:e2412598
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|u http://dx.doi.org/10.1002/adma.202412598
|3 Volltext
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