Origin and hysteresis of lithium compositional spatiodynamics within battery primary particles

Jongwoo Lim, Yiyang Li, Daan Hein Alsem, Hongyun So, Sang Chul Lee, Peng Bai, Daniel A. Cogswell, Xuzhao Liu, Norman Jin, Young Sang Yu, Norman J. Salmon, David A. Shapiro, Martin Z. Bazant, Tolek Tyliszczak, William C. Chueh

Research output: Contribution to journalArticlepeer-review

378 Scopus citations

Abstract

The kinetics and uniformity of ion insertion reactions at the solid-liquid interface govern the rate capability and lifetime, respectively, of electrochemical devices such as Li-ion batteries. Using an operando x-ray microscopy platform that maps the dynamics of the Li composition and insertion rate in LixFePO4, we found that nanoscale spatial variations in rate and in composition control the lithiation pathway at the subparticle length scale. Specifically, spatial variations in the insertion rate constant lead to the formation of nonuniform domains, and the composition dependence of the rate constant amplifies nonuniformities during delithiation but suppresses them during lithiation, and moreover stabilizes the solid solution during lithiation. This coupling of lithium composition and surface reaction rates controls the kinetics and uniformity during electrochemical ion insertion.
Original languageEnglish (US)
Pages (from-to)566-571
Number of pages6
JournalScience
Volume353
Issue number6299
DOIs
StatePublished - Aug 5 2016
Externally publishedYes

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