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One-Step Calcination Synthesis of Bulk-Doped Surface-Modified Ni-Rich Cathodes with Superlattice for Long-Cycling Li-Ion Batteries
Authors:Yongjiang Sun  Changhong Wang  Wenjin Huang  Genfu Zhao  Lingyan Duan  Qing Liu  Shimin Wang  Adam Fraser  Hong Guo  Xueliang Sun
Institution:1. International Joint Research Center for Advanced Energy Materials of Yunnan Province, Electron Microscope Center of Yunnan University, School of Materials and Energy, Yunnan University, 650091 Kunming, China

These authors contributed equally to this work.;2. Department of Mechanical and Materials Engineering, University of Western Ontario, 1151 Richmond St., N6A3K7 London, Ontario, Canada;3. International Joint Research Center for Advanced Energy Materials of Yunnan Province, Electron Microscope Center of Yunnan University, School of Materials and Energy, Yunnan University, 650091 Kunming, China

Abstract:Nickel-rich (Ni≥90 %) layered cathodes are critical materials for achieving higher-energy-density and lower-cost next-generation Li-ion batteries (LIBs). However, their bulk and interface structural instabilities significantly impair their electrochemical performance, thus hindering their widespread adoption in commercial LIBs. Exploiting Ti and Mo diffusion chemistry, we report one-step calcination to synthesize bulk-to-surface modified LiNi0.9Co0.09Mo0.01O2 (NCMo90) featuring a 5 nm Li2TiO3 coating on the surface, a Mo-rich Li+/Ni2+ superlattice at the sub-surface, and Ti-doping in the bulk. Such a multi-functional structure effectively maintains its structural integrity upon cycling. As a result, such NCMo90 exhibits a high initial capacity of 221 mAh g?1 at 0.1 C, excellent rate performance (184 mAh g?1 at 5 C), and high capacity retention of 94.0 % after 500 cycles. This work opens a new avenue to developing industry-applicable Ni-rich cathodes for next-generation LIBs.
Keywords:Bulk-to-Surface Modification  Li-Ion Batteries  Ni-Rich Cathodes  One-Step Synthesis  Ordered Superlattice
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