Gel-Confined Crystallization Unlocks Defect-Minimized Prussian Blue Cathode for High-Performance Sodium-Ion Batteries

IF 8.7 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-09-13 DOI:10.1021/acsmaterialslett.5c01093

Yonglin Lu, , , Yuheng Chen, , , Wanyi Yuan, , , Jingyi Chen, , , Xin Cao*, , , Yuwei Zhang*, , , Yawen Tang, , and , Ping Wu*,

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Abstract

Metal hexacyanoferrates (MHCFs) have emerged as promising cathodes for sodium-ion batteries. However, conventional wet-chemistry-derived MHCFs inevitably contain substantial Fe(CN)₆ vacancies and crystal water, resulting in an undesirable Na-storage performance. Herein, a gel-confined crystallization strategy is developed to prepare highly crystalline MHCFs. In a typical polypyrrole (PPy) gel, the cross-linked network effectively restricts the movement of internal ions through steric hindrance and attractive/repulsive interactions, leading to slow crystal growth and formation of highly crystalline MHCFs. Specifically, iron hexacyanoferrate (FeHCF), with only 1% Fe(CN)₆ vacancy and 2.0 wt% crystal water, has been formed in situ within a PPy gel via this gel-confined crystallization process. The highly crystalline FeHCF coupled with an interconnected PPy framework enables the hybrid cathode to exhibit enhanced activity of low-spin Fe sites, long cycling life, and good rate capability.

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凝胶限制结晶解锁缺陷最小化的高性能钠离子电池普鲁士蓝阴极

金属六氰高铁酸盐（MHCFs）已成为钠离子电池中很有前途的阴极。然而，传统的湿化学衍生mhcf不可避免地含有大量的Fe(CN)6空位和结晶水，导致不良的na存储性能。本文开发了一种凝胶约束结晶策略来制备高结晶mhcf。在典型的聚吡咯（PPy）凝胶中，交联网络通过空间位阻和吸引/排斥相互作用有效地限制了内部离子的运动，导致晶体生长缓慢和高结晶mhcf的形成。具体来说，通过这种凝胶约束结晶过程，在PPy凝胶中原位形成了六氰高铁（FeHCF），其Fe(CN)6空位仅为1%，结晶水为2.0 wt%。高度结晶的FeHCF与相互连接的PPy框架相结合，使得杂化阴极具有增强的低自旋Fe位活性，长循环寿命和良好的倍率能力。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.