A MOF-Mediated Strategy for In Situ Niobium Doping and Synthesis of High-Performance Single-Crystal Ni-Rich Cathodes

The development of single-crystal Ni-rich layered cathode materials (SC-NCMs) is regarded as an effective strategy to address the mechanical failure issues commonly associated with polycrystalline counterparts. However, the industrial production of SC-NCM faces challenges such as lengthy processing steps, high manufacturing costs, and inconsistent product quality. In this study, we innovatively propose a metal/organic framework (MOF)-mediated one-step synthesis strategy to achieve controllable structural preparation and in situ Nb5+ doping in SC-NCM. Using a Ni–Co–Mn-based MOF as both precursor and self-template, we precisely regulated the thermal treatment pathway to guide the nucleation and oriented growth of high-density SC-NCM particles. Simultaneously, Nb5+ was pre-anchored within the MOF framework, enabling atomic-level homogeneous doping into the transition metal layers during crystal growth. Exceptional electrochemical performance is revealed in the in situ Nb-doped SC-NCM, with an initial discharge capacity reaching 176 mAh/g at a 1C rate and a remarkable capacity retention of 86.36% maintained after 200 cycles. This study paves a versatile and innovative pathway for the design of high-stability, high-energy-density cathode materials via a MOF-mediated synthesis strategy, enabling precise manipulation of both morphology and chemical composition.