定向形成的普鲁士蓝纳米花作为钠离子电池的高性能阴极,ACS Sustainable Chemistry & Engineering

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定向形成的普鲁士蓝纳米花作为钠离子电池的高性能阴极
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-10-21 , DOI: 10.1021/acssuschemeng.0c05466
Daxian Zuo ₁ , Cuiping Wang ₁ , Jiajia Han ₁ , Junwei Wu ₂ , Huajun Qiu ₂ , Qian Zhang ₂ , Yong Lu ₁ , Yongjin Lin ₁ , Xingjun Liu ₃

Affiliation

最近，具有独特形态的普鲁士蓝（PB）阴极的合理设计和制造已被认为是改善钠离子电池（SIB）电化学性能的一种有前途的方法。但是，迄今为止，PB的形状控制制备仍具有挑战性。在本文中，我们首次展示了一种定向的自组装策略，可以通过三维（3D）花状结构合成PB，通过实验实现对花大小的控制。通过密度泛函理论（DFT）计算，研究了花朵结构的形成机理。发现所得的PB纳米花的表现是由于其优越的固有特性，可以提供低的Fe（CN）₆空位和较大的比表面积。此外，特殊的花状PB具有出色的速率能力（在1600 mA g ^–1时为113 mAh g ^–1）和出色的循环稳定性（在800 mA g ^–1下400次循环后，容量保持率接近80％）。增强的性能归因于纳米级的花状结构，可以提供稳健的结构完整性，扩大电极与电解质之间的接触面积，并改善Na ⁺离子的表观扩散系数。此外，花朵结构在经历多个充放电循环后可以保留其母体结构，从而进一步确认了结构稳定性。

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Oriented Formation of a Prussian Blue Nanoflower as a High Performance Cathode for Sodium Ion Batteries

Recently, the rational design and fabrication of Prussian blue (PB) cathodes with a unique morphology has been regarded as a promising way to improve the electrochemical properties for sodium ion batteries (SIBs). However, the shape-controlled preparation of PB still remains challenging up to now. Herein, we demonstrate an oriented self-assembly strategy to synthesize PB with three-dimensional (3D) flowerlike structures for the first time, experimentally realizing control of the flower size. And the formation mechanism of the flower structure is investigated through density function theory (DFT) calculations. It is found that the resulting PB nanoflowers perform because of superior inherent properties, which can afford low Fe(CN)₆ vacancies and large specific surface areas. In addition, the special flowerlike PB exhibits superior rate capability (113 mAh g^–1 at 1600 mA g^–1) and excellent cyclic stability (close to 80% capacity retention after 400 cycles at 800 mA g^–1). The enhanced performance can be attributed to the flowerlike structure at the nanoscale, which can provide robust structural integrity, enlarge the contact area between electrode and electrolyte, and improve the apparent diffusion coefficient of Na⁺ ions. In addition, the flower structures can retain their parent structure when undergoing multiple charge–discharge cycles, further confirming the structural stability.

更新日期：2020-11-02

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