Voltage Hysteresis of Silicon Nanoparticles: Chemo-Mechanical Particle-SEI Model

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Main Authors: Köbbing, Lukas, Latz, Arnulf, Horstmann, Birger
Format: Preprint
Published: 2023
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author Köbbing, Lukas
Latz, Arnulf
Horstmann, Birger
author_facet Köbbing, Lukas
Latz, Arnulf
Horstmann, Birger
contents Silicon is a promising anode material for next-generation lithium-ion batteries. However, the volume change and the voltage hysteresis during lithiation and delithiation are two substantial drawbacks to their lifetime and performance. We investigate the reason for the voltage hysteresis in amorphous silicon nanoparticles covered by a solid-electrolyte interphase (SEI). Concentration gradients inside the nanoscale silicon can not produce the massive stresses necessary to cause the reported voltage hysteresis. Our chemo-mechanical model shows that plastic deformation of the stiff, inorganic SEI during lithiation and delithiation reproduces the observed silicon open-circuit voltage hysteresis. Additionally, the viscous behavior of the SEI explains the difference between the voltage hysteresis observed at low currents and after relaxation. We conclude that the visco-elastoplastic behavior of the SEI is the origin of the voltage hysteresis in silicon nanoparticle anodes. Thus, consideration of the SEI mechanics is crucial for further improvements.
format Preprint
id arxiv_https___arxiv_org_abs_2305_17533
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Voltage Hysteresis of Silicon Nanoparticles: Chemo-Mechanical Particle-SEI Model
Köbbing, Lukas
Latz, Arnulf
Horstmann, Birger
Chemical Physics
Applied Physics
Silicon is a promising anode material for next-generation lithium-ion batteries. However, the volume change and the voltage hysteresis during lithiation and delithiation are two substantial drawbacks to their lifetime and performance. We investigate the reason for the voltage hysteresis in amorphous silicon nanoparticles covered by a solid-electrolyte interphase (SEI). Concentration gradients inside the nanoscale silicon can not produce the massive stresses necessary to cause the reported voltage hysteresis. Our chemo-mechanical model shows that plastic deformation of the stiff, inorganic SEI during lithiation and delithiation reproduces the observed silicon open-circuit voltage hysteresis. Additionally, the viscous behavior of the SEI explains the difference between the voltage hysteresis observed at low currents and after relaxation. We conclude that the visco-elastoplastic behavior of the SEI is the origin of the voltage hysteresis in silicon nanoparticle anodes. Thus, consideration of the SEI mechanics is crucial for further improvements.
title Voltage Hysteresis of Silicon Nanoparticles: Chemo-Mechanical Particle-SEI Model
topic Chemical Physics
Applied Physics
url https://arxiv.org/abs/2305.17533