Invoking Interfacial Engineering Boosts Structural Stability Empowering Exceptional Cyclability of Ni‐Rich Cathode

作者：Youqi Chu, Yongbiao Mu, Huicun Gu, Yan Hu, Xianbin Wei, Lingfeng Zou, Can Yu, Xiaoqian Xu, Shaowei Kang, Kang Li, Meisheng Han, Qing Zhang, Lin Zeng · 发表于：Advanced Materials · 年份：2024 · DOI：10.1002/adma.202405628 · 被引用次数：44 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Supercapacitor Materials and Fabrication

Abstract The cycling stability of LiNi 0.8 Co 0.1 Mn 0.1 O 2 under high voltages is hindered by the occurrence of hybrid anion‐ and cation‐redox processes, leading to oxygen escape and uncontrolled phase collapse. In this study, an interfacial engineering strategy involving a straightforward mechanical ball milling and low‐temperature calcination, employing a Se‐doped and FeSe 2 &Fe 2 O 3 ‐modified approach is proposed to design a stable Ni‐rich cathode. Se 2− are selectively adsorbed within oxygen vacancies to form O ─ TM ─ Se bond, effectively stabilizing lattice oxygen, and preventing structural distortion. Simultaneously, the Se‐NCM811//FeSe 2 //Fe 2 O 3 self‐assembled electric field is activated, improving interfacial charge transfer and coupling. Furthermore, FeSe 2 accelerates Li + diffusion and reacts with oxygen to form Fe 2 O 3 and SeO 2 . The Fe 2 O 3 coating mitigates hydrofluoric acid erosion and acts as an electrostatic shield layer, limiting the outward migration of oxygen anions. Impressively, the modified materials exhibit significantly improved electrochemical performance, with a capacity retention of 79.7% after 500 cycles at 1C under 4.5 V. Furthermore, it provides an extraordinary capacity retention of 94.6% in 3–4.25 V after 550 cycles in pouch‐type full battery. This dual‐modification approach demonstrates its feasibility and opens new perspective for the development of stable lithium‐ion batteries operating at high voltages.