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Title: Stress-Dependent Chemo-Mechanical Performance of Amorphous Si Anodes for Li-Ion Batteries upon Lithiation

Abstract

Alloying-type anodes are significantly governed by their chemo-mechanical performance during the electrochemical cycling. The reaction-induced huge volumetric change of these anodes may cause material degradation and failure under mechanical constraints. Here, we investigate the stress-dependent lithiation behavior of amorphous Si (a-Si) anodes using molecular dynamics simulations. It is indicated that a-Si anodes can sustain higher hydrostatic stress than biaxial/uniaxial ones without the occurrence of mechanical failure. Thermodynamic and electrochemical calculations demonstrate that although the lithiation procedure also affects the thermodynamic stability of a-Si anodes, it is mainly dominated by the external mean stresses. Compressive stress is confirmed to destabilize a-Si anodes and further trigger their capacity fading. Compared with our atomistic simulations, previous continuum models underestimate the open-cell potentials of a-Si anodes, due to their ignored large volumetric deformation at higher stresses and Li concentrations. Finally, this computational study provides the intensive atomic-level understanding of the stress-dependent lithiation behavior of a-Si anodes.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4]
+ Show Author Affiliations
  1. Univ. of Queensland, St. Lucia, QLD (Australia)
  2. Beijing University of Posts and Telecommunications (China)
  3. Cornell Univ., Ithaca, NY (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1892386
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Energy Materials
Additional Journal Information:
Journal Volume: 4; Journal Issue: 12; Journal ID: ISSN 2574-0962
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Si anodes; chemo-mechanics; formation enthalpy; stress effect; electrochemical properties; lithiation

Citation Formats

Wang, Mingchao, Ye, Han, Zhai, Chenxi, and Yang, Guang. Stress-Dependent Chemo-Mechanical Performance of Amorphous Si Anodes for Li-Ion Batteries upon Lithiation. United States: N. p., 2021. Web. doi:10.1021/acsaem.1c03394.
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Wang, Mingchao, Ye, Han, Zhai, Chenxi, & Yang, Guang. Stress-Dependent Chemo-Mechanical Performance of Amorphous Si Anodes for Li-Ion Batteries upon Lithiation. United States. https://doi.org/10.1021/acsaem.1c03394
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Wang, Mingchao, Ye, Han, Zhai, Chenxi, and Yang, Guang. Mon . "Stress-Dependent Chemo-Mechanical Performance of Amorphous Si Anodes for Li-Ion Batteries upon Lithiation". United States. https://doi.org/10.1021/acsaem.1c03394. https://www.osti.gov/servlets/purl/1892386.
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@article{osti_1892386,
title = {Stress-Dependent Chemo-Mechanical Performance of Amorphous Si Anodes for Li-Ion Batteries upon Lithiation},
author = {Wang, Mingchao and Ye, Han and Zhai, Chenxi and Yang, Guang},
abstractNote = {Alloying-type anodes are significantly governed by their chemo-mechanical performance during the electrochemical cycling. The reaction-induced huge volumetric change of these anodes may cause material degradation and failure under mechanical constraints. Here, we investigate the stress-dependent lithiation behavior of amorphous Si (a-Si) anodes using molecular dynamics simulations. It is indicated that a-Si anodes can sustain higher hydrostatic stress than biaxial/uniaxial ones without the occurrence of mechanical failure. Thermodynamic and electrochemical calculations demonstrate that although the lithiation procedure also affects the thermodynamic stability of a-Si anodes, it is mainly dominated by the external mean stresses. Compressive stress is confirmed to destabilize a-Si anodes and further trigger their capacity fading. Compared with our atomistic simulations, previous continuum models underestimate the open-cell potentials of a-Si anodes, due to their ignored large volumetric deformation at higher stresses and Li concentrations. Finally, this computational study provides the intensive atomic-level understanding of the stress-dependent lithiation behavior of a-Si anodes.},
doi = {10.1021/acsaem.1c03394},
journal = {ACS Applied Energy Materials},
number = 12,
volume = 4,
place = {United States},
year = {Mon Dec 13 00:00:00 EST 2021},
month = {Mon Dec 13 00:00:00 EST 2021}
}
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https://doi.org/10.1021/acsaem.1c03394
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Works referenced in this record:

The mechanics of large-volume-change transformations in high-capacity battery materials
journal, December 2016

Failure mechanisms of 2D silicon film anodes: in situ observations and simulations on crack evolution
journal, January 2018

  • Yang, Le; Chen, Hao-Sen; Jiang, Hanqing
  • Chemical Communications, Vol. 54, Issue 32
  • DOI: 10.1039/c7cc09708e

A finite deformation stress-dependent chemical potential and its applications to lithium ion batteries
journal, July 2012

  • Cui, Zhiwei; Gao, Feng; Qu, Jianmin
  • Journal of the Mechanics and Physics of Solids, Vol. 60, Issue 7
  • DOI: 10.1016/j.jmps.2012.03.008

Intrinsic stress mitigation via elastic softening during two-step electrochemical lithiation of amorphous silicon
journal, June 2016

A nonlinear theory of thermochemical equilibrium of solids under stress
journal, January 1978

Cyclic plasticity and shakedown in high-capacity electrodes of lithium-ion batteries
journal, April 2013

  • Brassart, Laurence; Zhao, Kejie; Suo, Zhigang
  • International Journal of Solids and Structures, Vol. 50, Issue 7-8
  • DOI: 10.1016/j.ijsolstr.2012.12.019

Lithium concentration dependent structure and mechanics of amorphous silicon
journal, June 2016

  • Sitinamaluwa, H. S.; Wang, M. C.; Will, G.
  • Journal of Applied Physics, Vol. 119, Issue 24
  • DOI: 10.1063/1.4954683

In situ atomic-scale imaging of electrochemical lithiation in silicon
journal, October 2012

  • Liu, Xiao Hua; Wang, Jiang Wei; Huang, Shan
  • Nature Nanotechnology, Vol. 7, Issue 11
  • DOI: 10.1038/nnano.2012.170

Two-phase versus two-stage versus multi-phase lithiation kinetics in silicon
journal, September 2013

  • Cui, Zhiwei; Gao, Feng; Qu, Jianmin
  • Applied Physics Letters, Vol. 103, Issue 14
  • DOI: 10.1063/1.4824064

Large Plastic Deformation in High-Capacity Lithium-Ion Batteries Caused by Charge and Discharge: Large Plastic Deformation in Lithium-Ion Batteries
journal, March 2011

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Effects of stress on lithium transport in amorphous silicon electrodes for lithium-ion batteries
journal, April 2015

Lattice-distorted lithiation behavior of a square phase Janus MoSSe monolayer for electrode applications
journal, January 2021

  • Tang, Xin; Ye, Han; Liu, Wenjun
  • Nanoscale Advances, Vol. 3, Issue 10
  • DOI: 10.1039/d1na00112d

A linear theory of thermochemical equilibrium of solids under stress
journal, August 1973

25th Anniversary Article: Understanding the Lithiation of Silicon and Other Alloying Anodes for Lithium-Ion Batteries
journal, August 2013

  • McDowell, Matthew T.; Lee, Seok Woo; Nix, William D.
  • Advanced Materials, Vol. 25, Issue 36
  • DOI: 10.1002/adma.201301795

Atomistic Mechanisms of Phase Boundary Evolution during Initial Lithiation of Crystalline Silicon
journal, July 2014

  • Kim, Sang-Pil; Datta, Dibakar; Shenoy, Vivek B.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 31
  • DOI: 10.1021/jp502523t

Operando Nanoindentation: A New Platform to Measure the Mechanical Properties of Electrodes during Electrochemical Reactions
journal, January 2017

  • de Vasconcelos, Luize Scalco; Xu, Rong; Zhao, Kejie
  • Journal of The Electrochemical Society, Vol. 164, Issue 14
  • DOI: 10.1149/2.1411714jes

Interface-reaction controlled diffusion in binary solids with applications to lithiation of silicon in lithium-ion batteries
journal, February 2013

  • Cui, Zhiwei; Gao, Feng; Qu, Jianmin
  • Journal of the Mechanics and Physics of Solids, Vol. 61, Issue 2
  • DOI: 10.1016/j.jmps.2012.11.001

Stable cycling of double-walled silicon nanotube battery anodes through solid–electrolyte interphase control
journal, March 2012

  • Wu, Hui; Chan, Gerentt; Choi, Jang Wook
  • Nature Nanotechnology, Vol. 7, Issue 5
  • DOI: 10.1038/nnano.2012.35

Two-Phase Electrochemical Lithiation in Amorphous Silicon
journal, January 2013

  • Wang, Jiang Wei; He, Yu; Fan, Feifei
  • Nano Letters, Vol. 13, Issue 2
  • DOI: 10.1021/nl304379k

Failure modes of hollow core–shell structural active materials during the lithiation–delithiation process
journal, September 2015

In Situ Measurements of Stress-Potential Coupling in Lithiated Silicon
journal, January 2010

  • Sethuraman, V. A.; Srinivasan, V.; Bower, A. F.
  • Journal of The Electrochemical Society, Vol. 157, Issue 11
  • DOI: 10.1149/1.3489378

Studying the Kinetics of Crystalline Silicon Nanoparticle Lithiation with In Situ Transmission Electron Microscopy
journal, September 2012

  • McDowell, Matthew T.; Ryu, Ill; Lee, Seok Woo
  • Advanced Materials, Vol. 24, Issue 45
  • DOI: 10.1002/adma.201202744

Modeling the delamination of amorphous-silicon thin film anode for lithium-ion battery
journal, January 2014

Concurrent Reaction and Plasticity during Initial Lithiation of Crystalline Silicon in Lithium-Ion Batteries
journal, January 2012

  • Zhao, Kejie; Pharr, Matt; Wan, Qiang
  • Journal of The Electrochemical Society, Vol. 159, Issue 3
  • DOI: 10.1149/2.020203jes

In Situ TEM of Two-Phase Lithiation of Amorphous Silicon Nanospheres
journal, January 2013

  • McDowell, Matthew T.; Lee, Seok Woo; Harris, Justin T.
  • Nano Letters, Vol. 13, Issue 2
  • DOI: 10.1021/nl3044508

Effect of plasticity on voltage decay studied by a stress coupled phase field reaction model
journal, January 2021

Measurements of the Fracture Energy of Lithiated Silicon Electrodes of Li-Ion Batteries
journal, October 2013

  • Pharr, Matt; Suo, Zhigang; Vlassak, Joost J.
  • Nano Letters, Vol. 13, Issue 11
  • DOI: 10.1021/nl403197m

Reactive Flow in Silicon Electrodes Assisted by the Insertion of Lithium
journal, July 2012

  • Zhao, Kejie; Tritsaris, Georgios A.; Pharr, Matt
  • Nano Letters, Vol. 12, Issue 8
  • DOI: 10.1021/nl302261w

In situ measurement of lithiation-induced stress in silicon nanoparticles using micro-Raman spectroscopy
journal, April 2016

The Mixing Mechanism during Lithiation of Si Negative Electrode in Li-Ion Batteries: An Ab Initio Molecular Dynamics Study
journal, December 2011

  • Johari, Priya; Qi, Yue; Shenoy, Vivek B.
  • Nano Letters, Vol. 11, Issue 12
  • DOI: 10.1021/nl203302d

Lithiation-Assisted Strengthening Effect and Reactive Flow in Bulk and Nanoconfined Sulfur Cathodes of Lithium–Sulfur Batteries
journal, July 2017

  • Wang, Mingchao; Yu, Jingui; Lin, Shangchao
  • The Journal of Physical Chemistry C, Vol. 121, Issue 31
  • DOI: 10.1021/acs.jpcc.7b05446

Stress-modulated driving force for lithiation reaction in hollow nano-anodes
journal, February 2015

Atomistic amorphous/crystalline interface modelling for superlattices and core/shell nanowires
journal, January 2014

  • France-Lanord, Arthur; Blandre, Etienne; Albaret, Tristan
  • Journal of Physics: Condensed Matter, Vol. 26, Issue 5
  • DOI: 10.1088/0953-8984/26/5/055011

The Effect of Stress on Battery-Electrode Capacity
journal, January 2017

  • Bucci, Giovanna; Swamy, Tushar; Bishop, Sean
  • Journal of The Electrochemical Society, Vol. 164, Issue 4
  • DOI: 10.1149/2.0371704jes

Interfacial Properties of the a-Si∕Cu:Active–Inactive Thin-Film Anode System for Lithium-Ion Batteries
journal, January 2006

  • Maranchi, J. P.; Hepp, A. F.; Evans, A. G.
  • Journal of The Electrochemical Society, Vol. 153, Issue 6
  • DOI: 10.1149/1.2184753

Atomistic Simulation Derived Insight on the Irreversible Structural Changes of Si Electrode during Fast and Slow Delithiation
journal, June 2017

Model for charge/discharge-rate-dependent plastic flow in amorphous battery materials
journal, September 2016

Fracture and debonding in lithium-ion batteries with electrodes of hollow core–shell nanostructures
journal, November 2012

Elastic softening of amorphous and crystalline Li–Si Phases with increasing Li concentration: A first-principles study
journal, October 2010

Reactive flow in solids
journal, January 2013

  • Brassart, Laurence; Suo, Zhigang
  • Journal of the Mechanics and Physics of Solids, Vol. 61, Issue 1
  • DOI: 10.1016/j.jmps.2012.09.007

Atomistic investigation into the mechanical behaviour of crystalline and amorphous TiO2 nanotubes
journal, January 2016

  • Xu, Yanan; Wang, Mingchao; Hu, Ning
  • RSC Advances, Vol. 6, Issue 33
  • DOI: 10.1039/c5ra27268h

Failure Prediction of High-Capacity Electrode Materials in Lithium-Ion Batteries
journal, January 2016

  • Wang, Chengpeng; Ma, Zengsheng; Wang, Yan
  • Journal of The Electrochemical Society, Vol. 163, Issue 7
  • DOI: 10.1149/2.0251607jes

Role of Stress Concentrations on the Electrochemical Response of a Li-Ion Battery Anode Particle
journal, January 2019

  • Ansari, Mohammad Ayub; Kumbhar, Pramod Yallappa; Swaminathan, Narasimhan
  • Journal of The Electrochemical Society, Vol. 166, Issue 12
  • DOI: 10.1149/2.0881912jes

Slower icosahedral cluster rejuvenation drives the brittle-to-ductile transition in nanoscale metallic glasses
journal, December 2017

Variation of stress with charging rate due to strain-rate sensitivity of silicon electrodes of Li-ion batteries
journal, December 2014

A First Molecular Dynamics Study for Modeling the Microstructure and Mechanical Behavior of Si Nanopillars during Lithiation
journal, April 2021

  • Shuang, Fei; Aifantis, Katerina E.
  • ACS Applied Materials & Interfaces, Vol. 13, Issue 18
  • DOI: 10.1021/acsami.1c02977

Hydrogen clustering in bcc metals: Atomic origin and strong stress anisotropy
journal, December 2020

Size-dependent fracture of Si nanowire battery anodes
journal, September 2011

  • Ryu, Ill; Choi, Jang Wook; Cui, Yi
  • Journal of the Mechanics and Physics of Solids, Vol. 59, Issue 9
  • DOI: 10.1016/j.jmps.2011.06.003
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