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Understanding the Effect of Local Short-Range Ordering on Lithium Diffusion in Li_1.3Nb_0.3Mn_0.4O₂ Single-Crystal Cathode

Publication Type

Journal Article

Date Published

09/2018

Authors

Kan, Wang Hay, Biao Deng, Yahong Xu, Alpesh Khushalcha Shukla, Tao Bo, Shuo Zhang, Jin Liu, Piero Pianetta, Bao-Tian Wang, Yijin Liu, Guoying Chen

DOI

10.1016/j.chempr.2018.05.008

Abstract

We report the observation of persistent chemical gradient on rock-salt Li1.3Nb0.3Mn0.4O2 single crystals transforming through a second-order reaction and reveal the dominating effect of local chemistry on Li diffusion within the percolated network. By using advanced 2D and 3D nanoscale X-ray spectro-microscopy on well-formed crystal samples, our study visualizes the mesoscale chemical distribution as a function of the state of charge at the subparticle level. We further reveal the presence of thermodynamically favorable short-range ordering of Nb-cation-only (Nb6) and Nb-cation-enriched (MnNb5) configurations, which promote non-equilibrium diffusion pathways and the expansive chemical heterogeneity observed on LixNb0.3Mn0.4O2 particles. The present study utilizes large single crystals to eliminate the influence of kinetic factors such as particle-size distribution, crystal facet, grain boundary, and strain, allowing us to clearly demonstrate the strong correlation between a material's structural defects and chemical propagation and its crucial impact on electrode performance and stability.

Journal

Chem

Volume

Year of Publication

2018

Issue

ISSN

24519294

Organization

Energy Storage and Distributed Resources Division, Energy Storage Group, Battery Group

Understanding the Effect of Local Short-Range Ordering on Lithium Diffusion in Li1.3Nb0.3Mn0.4O2 Single-Crystal Cathode