Nanoscale Mechanics of the Solid Electrolyte Interphase on Lithiated-Silicon Electrodes

Haoran Wang; Huck Beng Chew

doi:10.1021/acsami.7b07626

Nanoscale Mechanics of the Solid Electrolyte Interphase on Lithiated-Silicon Electrodes

Haoran Wang, Huck Beng Chew

Aerospace Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

The ∼300% volume changes of lithiated silicon electrodes (Li_xSi) during electrochemical cycling lead to cracking of the solid electrolyte interface (SEI). Here, we report how strain is transferred from Li_xSi to two primary inorganic SEI components: LiF and Li₂O. Our first principle calculations show that LiF, effectively bonded on Li_xSi at x > 1, enables the entire interface structure to deform plastically by forming delocalized stable voids. In contrast, Li₂O tightly bonded to Li_xSi is stiffer, and deforms rigidly across all x. Our results explain the significantly improved ductility of SEI with higher LiF versus Li₂O content observed experimentally.

Original language	English (US)
Pages (from-to)	25662-25667
Number of pages	6
Journal	ACS Applied Materials and Interfaces
Volume	9
Issue number	31
DOIs	https://doi.org/10.1021/acsami.7b07626
State	Published - Aug 9 2017

Keywords

density functional theory
lithium-ion batteries
mechanical deformation
silicon electrodes
solid electrolyte interphase

ASJC Scopus subject areas

Materials Science(all)

Online availability

10.1021/acsami.7b07626

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abstract = "The ∼300% volume changes of lithiated silicon electrodes (LixSi) during electrochemical cycling lead to cracking of the solid electrolyte interface (SEI). Here, we report how strain is transferred from LixSi to two primary inorganic SEI components: LiF and Li2O. Our first principle calculations show that LiF, effectively bonded on LixSi at x > 1, enables the entire interface structure to deform plastically by forming delocalized stable voids. In contrast, Li2O tightly bonded to LixSi is stiffer, and deforms rigidly across all x. Our results explain the significantly improved ductility of SEI with higher LiF versus Li2O content observed experimentally.",

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AB - The ∼300% volume changes of lithiated silicon electrodes (LixSi) during electrochemical cycling lead to cracking of the solid electrolyte interface (SEI). Here, we report how strain is transferred from LixSi to two primary inorganic SEI components: LiF and Li2O. Our first principle calculations show that LiF, effectively bonded on LixSi at x > 1, enables the entire interface structure to deform plastically by forming delocalized stable voids. In contrast, Li2O tightly bonded to LixSi is stiffer, and deforms rigidly across all x. Our results explain the significantly improved ductility of SEI with higher LiF versus Li2O content observed experimentally.

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KW - lithium-ion batteries

KW - mechanical deformation

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KW - solid electrolyte interphase

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Nanoscale Mechanics of the Solid Electrolyte Interphase on Lithiated-Silicon Electrodes

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