Molten Salt Synthesis of Multi-Faceted Pure-Phase Spinel LiNi0.5Mn1.5O4 Platelets

13 July 2023, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

The spinel LiNi0.5Mn1.5O4 is largely studied as a positive electrode material for lithium-ion batteries, but further optimization of its properties are required to enable its commercialization. The superior electrochemical performance of the disordered polymorph of LiNi0.5Mn1.5O4 is limited by its traditional method of synthesis. This solid-state route generates impurities that reduce specific capacity and results in the formation of octahedral particles with exposed {111} facets, thus limiting explo-ration of the effects of surface orientation. In this work, we report for the first time the preparation of a disordered impurity-free LiNi0.5Mn1.5O4 with platelet-like morphology via molten salt synthesis. We discovered that these platelets exhibit multi-ple surface orientations, including {111}, {112} and six other high-indexed facets, and deliver equivalent energy storage performance to their octahedral counterpart. Such ability to tune primary particle morphology and orientation will open the gate to investigate mechanisms at the individual particle level using spectroscopy and microscopy techniques.

Keywords

Li-ion Batteries
LiNi0.5Mn1.5O4
molten salt synthesis
surface orientation

Supplementary materials

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Supporting Information
Description
Description of samples preparation, material, and electro-chemical characterization methods; XPS analysis of sample 750°C, R=35 before and after extended washing in EtOH; ICP-OES anal-yses of all prepared samples; Raman spectra and their deconvolu-tion of prepared LNMO samples; Representation of the equivalence between layered hexagonal and cubic spinel structures; Representa-tions of Li+ ions diffusion pathways (BVEL) for eight different surface orientations observed on platelets of sample 750°C, R=35; Galvanostatic cycling curves of sample 750°C, R=35 before and after extended washing in EtOH; Self-discharge study on all pre-pared LNMO samples.
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