Abstract

Lithium nickel manganese cobalt oxide (NMC) cathodes are of great importance for the development of lithium ion batteries with high energy density. Currently, most commercially available NMC products are polycrystalline secondary particles, which are aggregated by anisotropic primary particles. Although the polycrystalline NMC particles have demonstrated large gravimetric capacity and good rate capabilities, the volumetric energy density, cycling stability as well as production adaptability are not satisfactory. Well-dispersed single-crystalline NMC is therefore proposed to be an alternative solution for further development of high-energy-density batteries. Various techniques have been explored to synthesize the single-crystalline NMC product, but the fundamental mechanisms behind these techniques are still fragmented and incoherent. In this manuscript, we start a journey from the fundamental crystal growth theory, compare the crystal growth of NMC among different techniques, and disclose the key factors governing the growth of single-crystalline NMC. We expect that the more generalized growth mechanism drawn from invaluable previous works could enhance the rational design and the synthesis of cathode materials with superior energy density.

Highlights

  • Lithium nickel manganese cobalt oxide (NMC) cathodes have been critical pillars of advanced lithium ion batteries at current state (Chen et al, 2019; Xu et al, 2019; Zhou et al, 2019; Kim et al, 2020; Li et al, 2020; Wang et al, 2020b; Wu et al, 2020; Zhang, 2020; Zheng et al, 2020)

  • The nucleation and the growth of single-crystalline NMC generally take place in a less-constrained environment, where several measures can be adopted in different stages to manipulate the morphology

  • Single-crystalline NMC811 particles grown in KCl exhibit an isotropic shape, whereas the octahedral shape with well-developed (003) and (11–1) facets is acquired in the NaCl flux

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Summary

INTRODUCTION

Lithium nickel manganese cobalt oxide (NMC) cathodes have been critical pillars of advanced lithium ion batteries at current state (Chen et al, 2019; Xu et al, 2019; Zhou et al, 2019; Kim et al, 2020; Li et al, 2020; Wang et al, 2020b; Wu et al, 2020; Zhang, 2020; Zheng et al, 2020). Several techniques, including solid-state sintering (Huang et al, 2011; Zhu et al, 2012; Lin et al, 2015; Wang et al, 2016; Jiang et al, 2017; Fan et al, 2020; Zhong et al, 2020), rheological reaction (Han et al, 2010), and molten flux growth (Kim, 2012; Kimijima et al, 2016a,b; Jiang et al, 2017), have been used to synthesize single-crystalline NMC cathode; equivalent electrochemical performances have been achieved in terms of capacity and rate capability compared with polycrystalline NMC. Well-dispersed singlecrystalline NMC111 particles of about 2–4 um were successfully obtained (Han et al, 2010)

Crystal Growth From Molten Salt Flux
MANIPULATION OF MORPHOLOGY
Control of Shape
Control of Facet
DISCUSSION AND PERSPECTIVE
AUTHOR CONTRIBUTIONS

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