Prussian blue analogues for potassium-ion batteries: insights into the electrochemical mechanisms,Journal of Materials Chemistry A

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Prussian blue analogues for potassium-ion batteries: insights into the electrochemical mechanisms
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-01-18 , DOI: 10.1039/d2ta08439b
Phuong Nam Le Pham _{1,

2} , Romain Wernert _{1,

3,

4} , Maëlle Cahu ₁ , Moulay Tahar Sougrati _{1,

2,

4} , Giuliana Aquilanti ₅ , Patrik Johansson _{2,

6} , Laure Monconduit _{1,

2,

4} , Lorenzo Stievano _{1,

2,

4}

Affiliation

A comprehensive description of the electrochemical mechanisms of the Prussian Blue Analogue (PBA) K_1.67Mn_0.65Fe_0.35[Fe(CN)₆]_0.92·0.45H₂O is obtained by combining several complementary ex situ and operando physico-chemical characterisation techniques. This particular PBA, which shows very good electrochemical performance as a cathode material in potassium-ion batteries (PIBs), undergoes three successive redox reactions during the (de-)potassiation that are hereby identified by ex situ ⁵⁷Fe Mössbauer spectroscopy and operando Mn and Fe K-edge X-ray absorption spectroscopy. These reactions come along with notable modifications of the crystal structure, which are followed in real time by operando X-ray diffraction. The correlation of these results, interpreted with the support of chemometric methods, also reveals the limitations of this PBA, probably related to the deactivation of the Mn undergoing extensive reversible Jahn–Teller distortion during cycling as well as possible dissolution in the electrolyte. These results underline that optimisation of the chemical composition of PBAs is a crucial step towards the preparation of reliable and stable PBA-based cathodes for PIBs.

中文翻译：

用于钾离子电池的普鲁士蓝类似物：对电化学机制的洞察

普鲁士蓝类似物 (PBA) K _1.67 Mn _0.65 Fe _0.35 [Fe(CN) ₆ ] _0.92 ·0.45H ₂ O 的电化学机制的全面描述是通过结合几种互补的非原位和操作物理化学表征技术获得的。这种特殊的 PBA 作为钾离子电池 (PIB) 的阴极材料显示出非常好的电化学性能，在（去）钾化过程中经历了三个连续的氧化还原反应，特此通过非原位 ⁵⁷ Fe Mössbauer 光谱和操作数确定Mn 和 Fe K 边 X 射线吸收光谱。这些反应伴随着晶体结构的显着改变，通过原位X 射线衍射实时跟踪。这些结果的相关性，在化学计量学方法的支持下解释，也揭示了这种 PBA 的局限性，可能与 Mn 在循环过程中经历广泛的可逆 Jahn-Teller 畸变的失活以及可能在电解质中的溶解有关。这些结果强调，优化 PBA 的化学成分是为 PIB 制备可靠且稳定的 PBA 基正极的关键一步。

更新日期：2023-01-18

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