ACS Nano | VOL. 16
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Imaging Phase Segregation in Nanoscale LixCoO2 Single Particles

Publication Date Sep 21, 2022

Abstract

LixCoO2 (LCO) is a common battery cathode material that has recently emerged as a promising material for other applications including electrocatalysis and as electrochemical random access memory (ECRAM). During charge-discharge cycling LCO exhibits phase transformations that are significantly complicated by electron correlation. While the bulk phase diagram for an ensemble of battery particles has been studied extensively, it remains unclear how these phases scale to nanometer dimensions and the effects of strain and diffusional anisotropy at the single-particle scale. Understanding these effects is critical to modeling battery performance and for predicting the scalability and performance of electrocatalysts and ECRAM. Here we investigate isolated, epitaxial LiCoO2 islands grown by pulsed laser deposition. After electrochemical cycling of the islands, conductive atomic force microscopy (c-AFM) is used to image the spatial distribution of conductive and insulating phases. Above 20 nm island thicknesses, we observe a kinetically arrested state in which the phase boundary is perpendicular to the Li-planes; we propose a model and present image analysis results that show smaller LCO islands have a higher conductive fraction than larger area islands, and the overall conductive fraction is consistent with the lithiation state. Thinner islands (14 nm), with a larger surface to volume ratio, are found to exhibit a striping pattern, which suggests surface energy can dominate below a critical dimension. When increasing force is applie...

Concepts

Photoemission Electron Microscopy Images Conductive Atomic Force Microscopy Performance Of Electrocatalysts Lithiation State Thinner Islands Nanometer Dimensions Pulsed Laser Deposition Diffusional Anisotropy Effects Of Strain Critical Dimension

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No potential conflict of interest was reported by the authors. The conception and design of the study, acquisition of data, analysis and interpretatio...

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