高性能铁基普鲁士蓝阴极材料通过Cu掺杂增强低自旋铁的活性,ACS Applied Materials & Interfaces

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高性能铁基普鲁士蓝阴极材料通过Cu掺杂增强低自旋铁的活性
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-01-24 , DOI: 10.1021/acsami.1c23793
Zhao-Yao Chen _{1,

2} , Xin-Yuan Fu ₁ , Lu-Lu Zhang ₁ , Bo Yan ₁ , Xue-Lin Yang ₁

Affiliation

铁基普鲁士蓝（FeHCF）理论容量高，铁矿石资源丰富，在钠离子（Na ⁺ ）电池规模化生产中具有巨大的应用潜力。然而，Fe(CN) ₆空位和结晶水严重影响电化学性能。在此，通过共沉淀法直接制备了Cu掺杂的FeHCF（Cu-FeHCF）正极材料。Cu掺杂后，单斜晶结构和准立方形态得以保留，但电化学性能显着提高。除少量Fe(CN) ₆空位和低结晶水，改善的性能还与低自旋Fe的电化学活性增强和Cu对晶体结构的稳定作用有关。此外，Cu掺杂也在一定程度上控制了副反应。结果，Cu 掺杂后，在 100 mA g ^{-1时初始放电容量从 107.9 提高到 127.4 mA hg}^-1，尤其是低自旋 Fe 贡献的容量从 30.0、21.7 和 16.7 mA hg ^-1提高前三个循环分别为48.8、45.4 和 43.7 mA hg ^{–1 。}即使在 2 A g ^–1下，Cu-FeHCF 仍具有 82.3 mA hg ^{–1的有希望的初始容量}超过 500 个循环，每个循环只有 0.047% 的容量衰减率。因此，Cu-FeHCF在Na ⁺储能电池领域显示出极好的应用潜力。

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High-Performance Fe-Based Prussian Blue Cathode Material for Enhancing the Activity of Low-Spin Fe by Cu Doping

Iron-based Prussian blue (FeHCF) has great application potential in the large-scale production of sodium-ion (Na⁺) batteries because of its high theoretical capacity and abundant Fe ore resources. However, the Fe(CN)₆ vacancies and crystal water seriously affect the electrochemical performance. Herein, a Cu-doped FeHCF (Cu–FeHCF) cathode material is successfully prepared directly by a coprecipitation method. After Cu doping, the monoclinic structure and the quasi-cubic morphology are retained, but the electrochemical performance is significantly improved. In addition to few Fe(CN)₆ vacancies and low crystal water, the improved performance is also related to the enhanced electrochemical activity of low-spin Fe and the stabilizing effect of Cu on the crystal structure. Moreover, Cu doping also controls the side reaction to a certain extent. As a result, after Cu doping, the initial discharge capacity is enhanced from 107.9 to 127.4 mA h g^–1 at 100 mA g^–1, especially the capacities contributed by low-spin Fe increase from 30.0, 21.7, and 16.7 mA h g^–1 to 48.8, 45.4, and 43.7 mA h g^–1 for the first three cycles, respectively. Even at 2 A g^–1, Cu–FeHCF still has a promising initial capacity of 82.3 mA h g^–1 and only a 0.047% capacity decay rate for each cycle over 500 cycles. Therefore, Cu–FeHCF shows excellent application potential in the field of Na⁺ energy storage batteries.

更新日期：2022-02-02

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