Phase Reconstruction‐Assisted Electron‐Li + Reservoirs Enable High‐Performance Li‐S Battery Operation Across Wide Temperature Range

作者：Yongqian He, Duanfeng Xiong, Yixin Luo, Wanqi Zhang, Sisi Liu, Yongjie Ye, Mengqing Wang, Ying Chen, Hong Liu, Jian Wang, Hongzhen Lin, Jincang Su, Xianyou Wang, Hongbo Shu, Manfang Chen · 发表于：Advanced Functional Materials · 年份：2024 · DOI：10.1002/adfm.202410899 · 被引用次数：36 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Advanced Battery Technologies Research

Abstract Lithium‐sulfur batteries (LSBs) are known as high energy density, but their performance deteriorates sharply under high/low‐temperature surroundings, due to the sluggish kinetics of sulfur redox conversion and Li + transport. Herein, a catalytic strategy of phase reconstruction with abundant “electron‐Li + ” reservoirs has been proposed to simultaneously regulate electron and Li + exchange. As a demo, the 1T‐phase lithiation molybdenum disulfide grown on hollow carbon nitride (1T‐Li x MoS 2 /HC 3 N 4 ) is achieved via in situ electrochemical modulation, where the 1T‐Li x MoS 2 serves as an auxiliary “Li + source” for facilitating Li + transport and the HC 3 N 4 acts as an electron donor for electronic supplier. From the theoretical calculations, experimental and post‐modern analyses, the relationship between the catalytic behaviors and mechanism of “electron‐Li + ” reservoirs in accelerating the rate‐determining kinetics of sulfur species are deeply understood. Consequently, the cells with 1T‐Li x MoS 2 /HC 3 N 4 /PP functional separator demonstrate excellent long‐term electrochemical performance and stabilize the areal capacity of 6 mAh cm −2 under 5.0 mg cm −2 . Even exposed to robust surroundings from high (60 °C) to low (0 °C) temperatures, the optimized cells exhibit high‐capacity retention of 76.2% and 90.4% after 100 cycles, respectively, pointing out the potential application of catalysts with phase reconstruction‐assisted “electron‐Li + ” reservoirs in LSBs.