Constructing Robust Electrode/Electrolyte Interphases for Highly Stable Lithium–Sulfurized Polyacrylonitrile Batteries

作者：Siyuan Shao, Jinze Hou, Youxuan Ni, Chunyan Zhu, Shuang Wu, Xinyi Liu, Can Wang, Kai Zhang, Zhenhua Yan, Yong Lü, Jun Chen · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202503214 · 被引用次数：15 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Polyoxometalates: Synthesis and Applications

Abstract Lithium–sulfurized polyacrylonitrile (SPAN) batteries show great promise for energy storage, but are plagued by poor cycling stability, which can be attributed to unfavorable electrode/electrolyte interphases for both anode and cathode. Here we design and achieve the anion‐moderate solvation structure based interconnected clusters in electrolyte by regulating the interactions of solvent with Li + and diluent to construct robust anode/electrolyte and cathode/electrolyte interphases simultaneously for high‐performance Li–SPAN batteries. The optimal electrolyte endows Li plating/stripping with a high Coulombic efficiency of 99.47% at 1 mA cm −2 in Li||Cu cells. The Li–SPAN batteries show excellent cycling stability with a high capacity retention of 94.21% after 1215 cycles. Moreover, the assembled pouch‐type Li–SPAN battery under limited electrolyte condition (2.40 g Ah −1 ) achieves a capacity of 3.75 Ah, corresponding to a high energy density of 180 Wh kg −1 based on the total mass of the battery. This work provides a good electrolyte design principle to construct robust anode/electrolyte and cathode/electrolyte interphases for batteries.