Sn‐Driven Grain Boundary Elimination for Single‐Crystalline Ni‐Rich Cathodes with Superior High‐Voltage Stability in Lithium‐Ion Batteries

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Abstract
Single‐crystalline Ni‐rich cathodes are regarded as promising candidates for high‐energy‐density lithium‐ion batteries (LIBs), providing superior mechanical and structural stability compared to polycrystalline counterparts. In this work, we present a low‐temperature grain‐boundary‐elimination approach to synthesize single‐crystalline LiNi 0.9 Co 0.08 Al 0.02 O 2 (SC‐NCA) through Sn‐assisted modification. Beyond enabling low‐temperature synthesis, the integrated Sn serves a dual‐protective function. Bulk Sn doping robustly pins lattice oxygen and mitigates harmful irreversible phase transitions, preserving structural integrity. Simultaneously, the residual formation of a highly conductive Li 2 SnO 3 surface layer accelerates Li + diffusion kinetics and robustly passivates the cathode‐electrolyte interphase against parasitic degradation. Consequently, this dual‐site modified SC‐Sn‐NCA90 cathode exhibits exceptional electrochemical performance, delivering a remarkable capacity retention of 86.7% after 500 cycles at 1 C (2.8–4.5 V), vastly eclipsing the 40.8% retention of the polycrystalline benchmark. This work presents a low‐temperature strategy for synthesizing SC‐NCA combined with Sn doping, facilitating the development of Ni‐rich layered cathodes for high‐energy‐density LIBs.
Funding Information
  • National Natural Science Foundation of China (52200076)

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