FeOHSO4@C Cathode with Low Strain and High Pseudocapacitance for Advanced Potassium-Ion Batteries.

Dai-Huo Liu, Cheng Yun,Bao Li,Dongmei Dai,Fang Xu, Yunli Li,Ao Wang, Chunyan Xu, Zhenjiang Li, Mengqin Song,Zhuangzhuang Zhang,Junpo Guo

Chemistry（2025）

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Abstract

Iron-based polyanionic cathode materials in potassium-ion batteries (KIBs) have appealed to an increasing number of interest due to these advantages of low cost, environmental friendliness and excellent structural stability. However, these inherent drawbacks of inferior electronic conductivity and terrible nanostructural stability hinder its practical application. Here, we report a novel low-strain iron-based polyanion-type cathode material FeOHSO4@C for KIBs. In this work, the surface of FeOHSO4 nanoparticles is well carbon encapsulated, carbon coating layer with large surface area and excellent electrical conductivity is ≈2.5 nm in thick, which can not only inhibit the aggregation and growth between FeOHSO4@C nanoparticles during charging and discharging, but also provide a 3D electronic conductive framework that activates electrochemical reactivity. As a result, the FeOHSO4@C cathode exhibits outstanding potassium storage capacity (capacity retention of 80.95% over 200 cycles at 20 mA g-1) attributed to a low-strain mechanism for K+ uptake/removal, high pseudocapacitance, as well as 3D electronic conductive framework. Operando XRD and ex situ XPS analyses revealed a single-phase reaction route of orthorhombic FeOHSO4@C during cycling.

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【要点】：本研究报道了一种低应变铁基聚阴离子型正极材料FeOHSO4@C，具有高伪电容和优异的电化学性能，用于高级钾离子电池。

【方法】：通过在FeOHSO4纳米粒子表面进行碳包覆，形成约2.5纳米厚的碳涂层，该涂层具有大表面积和优秀的电导性，有效抑制了FeOHSO4@C纳米粒子在充放电过程中的聚集和生长，并提供了一个3D电子导电路径以激活电化学活性。

【实验】：在20 mA g^-1的电流密度下，FeOHSO4@C正极在200个循环中容量保持率为80.95%，实验中使用了 operando XRD和ex situ XPS技术分析，证实了FeOHSO4@C在循环过程中的单相反应路径。