Peng Jian, Hua Weibo, Yang Zhuo, Li Jia-Yang, Wang Jinsong, Liang Yaru, Zhao Lingfei, Lai Weihong, Wu Xingqiao, Cheng Zhenxiang, Peleckis Germanas, Indris Sylvio, Wang Jia-Zhao, Liu Hua Kun, Dou Shi Xue, Chou Shulei
Institute of Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Zhejiang, Wenzhou 325035, China.
Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Innovation Campus, Squires Way, North Wollongong, NSW 2522, Australia.
ACS Nano. 2024 Jul 15. doi: 10.1021/acsnano.4c07021.
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.
开发具有成本效益、长寿命和全气候性能的钠离子电池对于推进大规模储能至关重要，但却因缺乏合适的阴极材料而受到困扰。在此，我们报告了一种低成本的富钠锰基普鲁士蓝类似物，通过用化学惰性的镍原子进行结构优化，其具有优异的倍率性能和超过10000次循环的超长循环稳定性。详细研究了它们的热稳定性、全气候性能以及在全电池中的潜力。多种原位表征表明，其出色的性能得益于高度可逆的三相转变和三金属（锰-镍-铁）协同效应。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钠扩散系数和2.3%的低体积畸变。我们的结果为大规模储能应用中用于先进钠离子电池的普鲁士蓝类似物的结构工程提供了见解。
