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Low-Spin Fe³⁺ Evoked by Multiple Defects with Optimal Intermediate Adsorption Attaining Unparalleled Performance in Water Oxidation 期刊论文 WOS高被引论文

编号：

F60246783F22FBC26A54699DE9A1A3D8
作者：

Wang, Yihao#^[1]Li, Shanqing(李善青)#^[2]Hou, Xu#^[3]Cui, Tingting*^[1]Zhuang, Zechao^[4];Zhao, Yunhe^[1];Wang, Haozhi^[5];Wei, Wei^[6];Xu, Ming^[1];Fu, Qiang*^[7]Chen, Chunxia*^[1]Wang, Dingsheng*^[4]
语种：

英文
期刊：

ADVANCED MATERIALS ISSN：0935-9648 2024 年 36 卷 52 期 ; DEC
收录：
关键词：

defect engineering layered double hydroxides low-spin Fe3+ spin state regulation water oxidation
摘要：

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, t(2g)(5)e(g)(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, t(2g)(3)e(g)(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.
推荐引用方式
GB/T 7714：

Wang Yihao,Li Shanqing,Hou Xu, et al. Low-Spin Fe³⁺ Evoked by Multiple Defects with Optimal Intermediate Adsorption Attaining Unparalleled Performance in Water Oxidation [J].ADVANCED MATERIALS,2024,36(52).
APA：

Wang Yihao,Li Shanqing,Hou Xu,Cui Tingting,&Wang Dingsheng.(2024).Low-Spin Fe³⁺ Evoked by Multiple Defects with Optimal Intermediate Adsorption Attaining Unparalleled Performance in Water Oxidation .ADVANCED MATERIALS,36(52).
MLA：

Wang Yihao, et al. "Low-Spin Fe³⁺ Evoked by Multiple Defects with Optimal Intermediate Adsorption Attaining Unparalleled Performance in Water Oxidation" .ADVANCED MATERIALS 36,52(2024).
入库时间：

12/10/2024 9:01:26 PM
更新时间：

8/24/2025 9:06:29 PM

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Low-Spin Fe3+ Evoked by Multiple Defects with Optimal Intermediate Adsorption Attaining Unparalleled Performance in Water Oxidation 期刊论文 WOS高被引论文

Low-Spin Fe³⁺ Evoked by Multiple Defects with Optimal Intermediate Adsorption Attaining Unparalleled Performance in Water Oxidation 期刊论文 WOS高被引论文