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Origin and hysteresis of lithium compositional spatiodynamics within battery primary particles

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

in Batteries / Cycles / Electric batteries / Electrochemistry / Electrodes / Insertion / Iron / Kinetics / Lithium / Nanostructure / Rate constants / Reaction kinetics / Solid solutions / Spectrometry / Variability

2016

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Origin and hysteresis of lithium compositional spatiodynamics within battery primary particles

2016

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Origin and hysteresis of lithium compositional spatiodynamics within battery primary particles

2016

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Journal Article

Origin and hysteresis of lithium compositional spatiodynamics within battery primary particles

Tyliszczak, Tolek,

Shapiro, David A.,

Jin, Norman,

Lee, Sang Chul,

Bai, Peng,

So, Hongyun,

Cogswell, Daniel A.,

Bazant, Martin Z.,

Yu, Young-sang,

Alsem, Daan Hein,

Chueh, William C.,

Lim, Jongwoo,

Li, Yiyang,

Salmon, Norman J.,

Liu, Xuzhao

2016

Overview

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.

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Publisher

American Association for the Advancement of Science,The American Association for the Advancement of Science

Subject

/ Cycles

/ Iron