Structural Engineering of Prussian Blue Analogues Enabling All-Climate and Ultralong Cycling Sodium-Ion Batteries
Jian Peng, Weibo Hua, Zhuo Yang, Jiayang Li, Jinsong Wang, Jinsong Wang, Yaru Liang, Lingfei Zhao, Wei‐Hong Lai, Xingqiao Wu, Zhenxiang Cheng, Germanas Peleckis, Sylvio Indris, Jiazhao Wang, Jiazhao Wang, Huan Liu, Shi Xue Dou, Shulei Chou
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.