Modulating the Coordination Environment of Single Fe Atoms with Enhanced Electrocatalytic Performance for Advanced Li─S Batteries

作者：Qinjun Shao, Yan Su, Min‐Hui Li, Xuejiao Chen, Zihan Jia, Jingting Hu, Dehui Deng, Jian Chen · 发表于：Advanced Functional Materials · 年份：2025 · DOI：10.1002/adfm.202501627 · 被引用次数：6 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Advanced battery technologies research

Abstract Involving electrocatalysts to increase the sluggish reduction reaction kinetics of soluble lithium polysulfides is evidenced effective in inhibiting the shuttle effect and enhancing the cycle stability of Li─S batteries. In this work, phosphorus‐coordinated single Fe atoms (FePC) are synthesized based on the coordination environment modulation strategy. Combining with experimental and theoretical methods, the well‐designed FePC with plane‐symmetric Fe─P 4 ─C configuration exhibits strengthened catalytic effect toward reversible conversion between LiPS and Li 2 S, that endows S@FePC cathodes with superior electrochemical performance. The prepared S@FePC coin cells achieve prolonged cyclic stability of over 1000 cycles at 1C with a high capacity retention of 77.8%. Even at high sulfur loading (5.7 mg cm −2 ) and low E/S ratio (6.2 µL mg S −1 ), the areal capacity reached 6.0 mAh cm −2 and 88.3% of it is retained after 100 cycles at 0.1 C. Moreover, the prepared 0.6 Ah S@FePC pouch cell exhibits higher capacity retention of 76.3% after 100 cycles at 0.1 C compared with S@FeNC. Meanwhile, the prepared 8Ah S@FePC pouch cell approaches a high specific energy of 401 Wh kg −1 at 0.1 C proving its practicability. The obtained outcomes may guide the future design and development of SACs with higher catalytic activity for practical Li─S batteries.