Nitrogenized 2D Covalent Organic Framework Decorated Ni‐Rich Single Crystal Cathode to Ameliorate the Electrochemical Performance of Lithium Batteries

Abstract Organic cathode materials for lithium‐ion batteries (LIBs) have elicited interest due to their wide‐ranging structures and finely regulated molecular levels. However, designing a cathode material with a high specific capacity, high rate‐performance, and long‐cycle life remains highly challenging. Herein, a nitrogenized 2D covalent organic framework (COF) with maximal active and minimal inactive groups is described and created by utilizing a coating material for single crystal LiNi 0.78 Mn 0.12 Co 0.1 O 2 (SCNMC) cathodes for LIBs. The composite cathode delivers a high reversible capacity of 160.5 mAh g −1 at 1 C with a retention rate of 87.5% after 200 cycles. The cycled SCNMC@COF particles show no lattice gliding and micro‐cracks, demonstrating that the SC shape may considerably reduce anisotropic micro‐strain. This efficient, repeatable, and customizable method for producing SCNMC cathodes shall hasten their commercialization. The solid framework further ensures outstanding capacity retention and rate performance. According to density functional theory calculations, optimizing the loading of redox‐active groups in a stable network structure is an efficient technique for designing a stable structure and improving the cycling life of SCNCM cathode material.