Abstract：
The development of cost-efficient, long-lifespan, and all-climate sodium-ion batteries is of great importance for advancing large-scale energy storage but is plagued by the lack of suitable cathode materials. Here, we report low-cost Na-rich Mn-based Prussian blue analogues with superior rate capability and ultralong cycling stability over 10,000 cycles via structural optimization with electrochemically inert Ni atoms. Their thermal stability, all-climate properties, and potential in full cells are investigated in detail. Multiple in situ characterizations reveal that the outstanding performances benefit from their highly reversible three-phase transformations and trimetal (Mn-Ni-Fe) synergistic effects. In addition, a high sodium diffusion coefficient and a low volume distortion of 2.3% are observed through in situ transmission electron microscopy and first-principles calculations. Our results provide insights into the structural engineering of Prussian blue analogues for advanced sodium-ion batteries in large-scale energy storage applications.
摘要：
成本效益的发展，长寿命，全气候钠离子电池对于推进大规模储能至关重要，但因缺乏合适的正极材料而困扰。这里,我们报告了低成本的富含Na的Mn基普鲁士蓝类似物，通过电化学惰性Ni原子的结构优化，具有超过10,000次循环的优异倍率能力和超长循环稳定性。它们的热稳定性，全气候属性，详细研究了全细胞的潜力。多个原位表征表明，出色的性能得益于其高度可逆的三相转变和三金属（Mn-Ni-Fe）协同作用。此外,通过原位透射电子显微镜和第一性原理计算观察到高的钠扩散系数和2.3％的低体积畸变。我们的结果为大型储能应用中高级钠离子电池的普鲁士蓝类似物的结构工程提供了见解。
