A novel method for surface modification of LiNi0.5Mn1.5O4 (LNMO) was proposed, in which a hybrid layer combined by Li1.3Al0.3Ti1.7(PO4)3 (LATP) and carbon (C) composite on LNMO material were connected by lithium iodide. Structure and morphology analyses illustrated that a higher contact area of active substances was achieved by the LATP/C composite layer without changing the original crystal structure of LNMO. XPS analysis proved that I− promoted the reduction of trace Mn4+, resulting in a higher ion conductivity. Galvanostatic charge–discharge tests exhibited the capacity of the LNMO with 5% LATP/C improved with 35.83% at 25 °C and 95.77% at 50 °C, respectively, compared with the bare after 100 cycles, implying the modification of high-temperature deterioration. EIS results demonstrated that one order of magnitude of improvement of the lithium-ion diffusion coefficient of LATP/C-LNMO was achieved (3.04 × 10−11 S cm−1). In conclusion, the effective low-temperature modification strategy improved the ionic and electronic conductivities of the cathode and suppressed the side reactions of high-temperature treatment.

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A mixed ionic (Li1.3Al0.3Ti1.7(PO4)3: LATP) and electronic conductor (porous carbon: C) hybrid layer can effectively enhance the electrochemical performance of cathode materials. In this work, a sustainable low-temperature synthesis strategy (≤ 200℃) combining ball milling and solvent-recrystallization of lithium iodide is proposed to prepare the LATP/C coated LiNi1/3Co1/3Mn1/3O2 (LNCMO) material. The characterizations of structures and morphology reveal that LATP and porous carbon powder are mixed into the ethanol dissolved lithium iodide by a simple ball milling process, then the lithium iodide is recrystallized to serve as a binder when ethanol is vaporized at a low temperature to coat uniform thickness and homogeneously distributed LATP/C on the surface of LNCMO cathode. The charge-discharge results illustrate that the cycling performance and rate discharge capability of the active materials coated with LATP/C are significantly superior to the bare LNCMO. AC impedance analysis confirms that lower charge transfer resistance and higher Li+ ion diffusion coefficient are achieved in cathode materials. This work successfully exploited a novel low-temperature cathode coating method based on lithium iodide solvent-recrystallization and obtained results comparable to high-temperature processes without suffering from side reaction problems.

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