Stabilizing High‐Capacity Layered Cathode Materials via Nanocluster Cross‐Linked Polymer

ABSTRACT Ni‐rich layered oxides and Li‐rich layered oxides are technologically important high‐capacity cathode materials for constructing high‐energy‐density batteries. However, their practical application is severely limited by interfacial instability and structural degradation during cycling. Herein, an organic‐inorganic hybrid polymer (PHM‐T) composed of titanium‐oxo clusters (TOCs) cross‐linked polyurethane is proposed to stabilize high‐capacity layered oxides. Rationally designing the soft and hard domains of polyurethane endows PHM‐T with high mechanical strength, excellent electrolyte tolerance, and strong cathode affinity. When employed as a surface coating layer, PHM‐T acts as an artificial cathode electrolyte interphase and dramatically improves the structural and compositional stabilities of both Ni‐rich layered oxides and Li‐rich layered oxides. With the suppressed lattice distortion and transition‐metal dissolution, the PHM‐T coated LiNi 0.8 Mn 0.1 Co 0.1 O 2 achieves enhanced rate capability (149.8 mAh g −1 at 10 C) and cycling stability (78% capacity retention after 200 cycles at 1 C). More impressively, the TOC cross‐linked polymer can serve directly as a reinforced binder, enabling one‐step surface modification and electrode fabrication without the pre‐coating process, offering a convenient and industrially Binder engineering, Cathode‐electrolyte interphase, Layered cathode materials, Nanocluster cross‐linked polymer, interfacial engineeringcompatible “two‐in‐one” interfacial‐engineering route to develop high‐performance batteries.