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Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries.

Abstract：

:Interfacial issues commonly exist in solid-state batteries, and the microstructural complexity combines with the chemical heterogeneity to govern the local interfacial chemistry. The conventional wisdom suggests that "point-to-point" ion diffusion at the interface determines the ion transport kinetics. Here, we show that solid-solid ion transport kinetics are not only impacted by the physical interfacial contact but are also closely associated with the interior local environments within polycrystalline particles. In spite of the initial discrete interfacial contact, solid-state batteries may still display homogeneous lithium-ion transportation owing to the chemical potential force to achieve an ionic-electronic equilibrium. Nevertheless, once the interior local environment within secondary particle is disrupted upon cycling, it triggers charge distribution from homogeneity to heterogeneity and leads to fast capacity fading. Our work highlights the importance of interior local environment within polycrystalline particles for electrochemical reactions in solid-state batteries and provides crucial insights into underlying mechanism in interfacial transport.

journal_name

Nat Commun

journal_title

Nature communications

authors

Lou S,Liu Q,Zhang F,Liu Q,Yu Z,Mu T,Zhao Y,Borovilas J,Chen Y,Ge M,Xiao X,Lee WK,Yin G,Yang Y,Sun X,Wang J

doi

10.1038/s41467-020-19528-9

subject

Has Abstract

pub_date

2020-11-11 00:00:00

pages

5700

issue

1

issn

2041-1723

pii

10.1038/s41467-020-19528-9

journal_volume

11

pub_type

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