Prussian blue analogue Co3[Co(CN)6]2 anode for lithium-ion batteries: Operando magnetometry insights into lithium storage

普鲁士蓝 锂(药物) 阳极 磁强计 离子 材料科学 无机化学 化学 电化学 电极 有机化学 磁场 物理化学 物理 内分泌学 医学 量子力学
作者
Fujie Li,Yan Liu,Zhenghua Lv,Liyan Chen,Guihuan Chen,Qiang Li
标识
DOI:10.1016/j.scenem.2025.100013
摘要

Prussian blue analogues (PBAs) have attracted considerable attention as electrode materials due to their open framework structures and tunable compositions. In this study, a well-defined PBA material, Co 3 [Co(CN) 6 ] 2 , was synthesized via a co-precipitation method and systematically evaluated as an anode for lithium-ion batteries. The material delivers a high reversible capacity of 537.4 mAh g -1 at a current density of 0.1 A g -1 , and maintains 116.2 mAh g -1 even at 5 A g -1 , demonstrating excellent rate performance and electrochemical stability. Remarkably, it retains 64.6% of its initial capacity after 1000 cycles, highlighting its outstanding long-term cyclability. To gain insight into the lithium storage mechanism, operando magnetization measurement combined with ex situ X-ray photoelectron spectroscopy were employed, revealing the redox and spin-state transitions of cobalt ions during the electrochemical process. Furthermore, a full cell constructed with Co 3 [Co(CN) 6 ] 2 as the anode and LiFePO 4 as the cathode exhibited stable electrochemical performance, confirming its potential for practical applications. This work not only introduces a promising PBA-based anode material, but also underscores the utility of operando magnetization measurement as a powerful tool for probing charge storage mechanisms. • Developed a straightforward co-precipitation route to synthesize Prussian blue analogue Co 3 [Co(CN) 6 ] 2 featuring a three-dimensional open-framework. • Demonstrated high reversible capacity and excellent rate capability across a broad range of current densities. • Exhibited robust long-term cycling stability with minimal capacity fade over extended cycles. • Leveraged operando magnetometry to elucidate cobalt redox and spin-state dynamics during lithium storage.

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