High damage tolerance of electrochemically lithiated silicon
Abstract
Mechanical degradation and resultant capacity fade in high-capacity electrode materials critically hinder their use in high-performance rechargeable batteries. Despite tremendous efforts devoted to the study of the electro–chemo–mechanical behaviours of high-capacity electrode materials, their fracture properties and mechanisms remain largely unknown. In this paper, we report a nanomechanical study on the damage tolerance of electrochemically lithiated silicon. Our in situ transmission electron microscopy experiments reveal a striking contrast of brittle fracture in pristine silicon versus ductile tensile deformation in fully lithiated silicon. Quantitative fracture toughness measurements by nanoindentation show a rapid brittle-to-ductile transition of fracture as the lithium-to-silicon molar ratio is increased to above 1.5. Molecular dynamics simulations elucidate the mechanistic underpinnings of the brittle-to-ductile transition governed by atomic bonding and lithiation-induced toughening. Finally, our results reveal the high damage tolerance in amorphous lithium-rich silicon alloys and have important implications for the development of durable rechargeable batteries.
- Authors:
-
- Georgia Inst. of Technology, Atlanta, GA (United States). Woodruff School of Mechanical Engineering
- Univ. of Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Materials Science
- Univ. of Illinois, Urbana, IL (United States). Dept. of Aerospace Engineering
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Georgia Institute of Technology, Atlanta, GA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- Contributing Org.:
- Univ. of Illinois, Urbana, IL (United States); Univ. of Pittsburgh, PA (United States)
- OSTI Identifier:
- 1347348
- Alternate Identifier(s):
- OSTI ID: 1261096
- Report Number(s):
- SAND2015-5484J
Journal ID: ISSN 2041-1723; ncomms9417
- Grant/Contract Number:
- AC04-94AL85000; NSF-CMMI-1300458; NSF-CMMI-1300805; NSF-CMMI-1100205; NSF-DMR-1410936; NSF-CMMI-08010934
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 6; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE; chemical sciences; materials science; nanotechnology; batteries; mechanical properties
Citation Formats
Wang, Xueju, Fan, Feifei, Wang, Jiangwei, Wang, Haoran, Tao, Siyu, Yang, Avery, Liu, Yang, Beng Chew, Huck, Mao, Scott X., Zhu, Ting, and Xia, Shuman. High damage tolerance of electrochemically lithiated silicon. United States: N. p., 2015.
Web. doi:10.1038/ncomms9417.
Wang, Xueju, Fan, Feifei, Wang, Jiangwei, Wang, Haoran, Tao, Siyu, Yang, Avery, Liu, Yang, Beng Chew, Huck, Mao, Scott X., Zhu, Ting, & Xia, Shuman. High damage tolerance of electrochemically lithiated silicon. United States. https://doi.org/10.1038/ncomms9417
Wang, Xueju, Fan, Feifei, Wang, Jiangwei, Wang, Haoran, Tao, Siyu, Yang, Avery, Liu, Yang, Beng Chew, Huck, Mao, Scott X., Zhu, Ting, and Xia, Shuman. Thu .
"High damage tolerance of electrochemically lithiated silicon". United States. https://doi.org/10.1038/ncomms9417. https://www.osti.gov/servlets/purl/1347348.
@article{osti_1347348,
title = {High damage tolerance of electrochemically lithiated silicon},
author = {Wang, Xueju and Fan, Feifei and Wang, Jiangwei and Wang, Haoran and Tao, Siyu and Yang, Avery and Liu, Yang and Beng Chew, Huck and Mao, Scott X. and Zhu, Ting and Xia, Shuman},
abstractNote = {Mechanical degradation and resultant capacity fade in high-capacity electrode materials critically hinder their use in high-performance rechargeable batteries. Despite tremendous efforts devoted to the study of the electro–chemo–mechanical behaviours of high-capacity electrode materials, their fracture properties and mechanisms remain largely unknown. In this paper, we report a nanomechanical study on the damage tolerance of electrochemically lithiated silicon. Our in situ transmission electron microscopy experiments reveal a striking contrast of brittle fracture in pristine silicon versus ductile tensile deformation in fully lithiated silicon. Quantitative fracture toughness measurements by nanoindentation show a rapid brittle-to-ductile transition of fracture as the lithium-to-silicon molar ratio is increased to above 1.5. Molecular dynamics simulations elucidate the mechanistic underpinnings of the brittle-to-ductile transition governed by atomic bonding and lithiation-induced toughening. Finally, our results reveal the high damage tolerance in amorphous lithium-rich silicon alloys and have important implications for the development of durable rechargeable batteries.},
doi = {10.1038/ncomms9417},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Thu Sep 24 00:00:00 EDT 2015},
month = {Thu Sep 24 00:00:00 EDT 2015}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 142 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Issues and challenges facing rechargeable lithium batteries
journal, November 2001
- Tarascon, J.-M.; Armand, M.
- Nature, Vol. 414, Issue 6861, p. 359-367
Electrical Energy Storage for the Grid: A Battery of Choices
journal, November 2011
- Dunn, B.; Kamath, H.; Tarascon, J. -M.
- Science, Vol. 334, Issue 6058
Challenges for Rechargeable Li Batteries
journal, February 2010
- Goodenough, John B.; Kim, Youngsik
- Chemistry of Materials, Vol. 22, Issue 3, p. 587-603
High-performance lithium-ion anodes using a hierarchical bottom-up approach
journal, March 2010
- Magasinski, A.; Dixon, P.; Hertzberg, B.
- Nature Materials, Vol. 9, Issue 4, p. 353-358
Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes
journal, September 2014
- Li, Yiyang; El Gabaly, Farid; Ferguson, Todd R.
- Nature Materials, Vol. 13, Issue 12
Decrepitation model for capacity loss during cycling of alloys in rechargeable electrochemical systems
journal, January 2000
- Huggins, R. A.; Nix, W. D.
- Ionics, Vol. 6, Issue 1-2, p. 57-63
Colossal Reversible Volume Changes in Lithium Alloys
journal, January 2001
- Beaulieu, L. Y.; Eberman, K. W.; Turner, R. L.
- Electrochemical and Solid-State Letters, Vol. 4, Issue 9
High-performance lithium battery anodes using silicon nanowires
journal, December 2007
- Chan, Candace K.; Peng, Hailin; Liu, Gao
- Nature Nanotechnology, Vol. 3, Issue 1, p. 31-35
Evolution of stress within a spherical insertion electrode particle under potentiostatic and galvanostatic operation
journal, May 2009
- Cheng, Yang-Tse; Verbrugge, Mark W.
- Journal of Power Sources, Vol. 190, Issue 2, p. 453-460
Fracture of electrodes in lithium-ion batteries caused by fast charging
journal, October 2010
- Zhao, Kejie; Pharr, Matt; Vlassak, Joost J.
- Journal of Applied Physics, Vol. 108, Issue 7
In situ measurements of stress evolution in silicon thin films during electrochemical lithiation and delithiation
journal, August 2010
- Sethuraman, Vijay A.; Chon, Michael J.; Shimshak, Maxwell
- Journal of Power Sources, Vol. 195, Issue 15
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
A High Capacity Nano-Si Composite Anode Material for Lithium Rechargeable Batteries
journal, January 1999
- Li, Hong; Huang, Xuejie; Chen, Liquan
- Electrochemical and Solid-State Letters, Vol. 2, Issue 11, p. 547-549
Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation
journal, August 2011
- Liu, Xiao Hua; Zheng, He; Zhong, Li
- Nano Letters, Vol. 11, Issue 8, p. 3312-3318
Real-Time Measurement of Stress and Damage Evolution during Initial Lithiation of Crystalline Silicon
journal, July 2011
- Chon, M. J.; Sethuraman, V. A.; McCormick, A.
- Physical Review Letters, Vol. 107, Issue 4
Size-Dependent Fracture of Silicon Nanoparticles During Lithiation
journal, January 2012
- Liu, Xiao Hua; Zhong, Li; Huang, Shan
- ACS Nano, Vol. 6, Issue 2
Two-Phase Electrochemical Lithiation in Amorphous Silicon
journal, January 2013
- Wang, Jiang Wei; He, Yu; Fan, Feifei
- Nano Letters, Vol. 13, Issue 2
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
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
“Electrochemical Shock” of Intercalation Electrodes: A Fracture Mechanics Analysis
journal, January 2010
- Woodford, William H.; Chiang, Yet-Ming; Carter, W. Craig
- Journal of The Electrochemical Society, Vol. 157, Issue 10
Method to deduce the critical size for interfacial delamination of patterned electrode structures and application to lithiation of thin-film silicon islands
journal, May 2012
- Haftbaradaran, Hamed; Xiao, Xingcheng; Verbrugge, Mark W.
- Journal of Power Sources, Vol. 206
Atomic-Scale Mechanisms of Sliding along an Interdiffused Li–Si–Cu Interface
journal, February 2015
- Wang, Haoran; Hou, Binyue; Wang, Xueju
- Nano Letters, Vol. 15, Issue 3
Mechanical properties of amorphous Li x Si alloys: a reactive force field study
journal, October 2013
- Fan, Feifei; Huang, Shan; Yang, Hui
- Modelling and Simulation in Materials Science and Engineering, Vol. 21, Issue 7
Elastic softening of amorphous and crystalline Li–Si Phases with increasing Li concentration: A first-principles study
journal, October 2010
- Shenoy, V. B.; Johari, P.; Qi, Y.
- Journal of Power Sources, Vol. 195, Issue 19
Ex-situ depth-sensing indentation measurements of electrochemically produced Si–Li alloy films
journal, August 2011
- Hertzberg, Benjamin; Benson, Jim; Yushin, Gleb
- Electrochemistry Communications, Vol. 13, Issue 8
Mechanical behavior of electrochemically lithiated silicon
journal, January 2015
- Berla, Lucas A.; Lee, Seok Woo; Cui, Yi
- Journal of Power Sources, Vol. 273
In situ tensile and creep testing of lithiated silicon nanowires
journal, December 2013
- Boles, Steven T.; Thompson, Carl V.; Kraft, Oliver
- Applied Physics Letters, Vol. 103, Issue 26
Variation of stress with charging rate due to strain-rate sensitivity of silicon electrodes of Li-ion batteries
journal, December 2014
- Pharr, Matt; Suo, Zhigang; Vlassak, Joost J.
- Journal of Power Sources, Vol. 270
Quantitative Fracture Strength and Plasticity Measurements of Lithiated Silicon Nanowires by In Situ TEM Tensile Experiments
journal, October 2012
- Kushima, Akihiro; Huang, Jian Yu; Li, Ju
- ACS Nano, Vol. 6, Issue 11
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
In Situ Observation of the Electrochemical Lithiation of a Single SnO2 Nanowire Electrode
journal, December 2010
- Huang, J. Y.; Zhong, L.; Wang, C. M.
- Science, Vol. 330, Issue 6010, p. 1515-1520
Stress generation during lithiation of high-capacity electrode particles in lithium ion batteries
journal, July 2013
- Huang, S.; Fan, F.; Li, J.
- Acta Materialia, Vol. 61, Issue 12
Strength and sharp contact fracture of silicon
journal, February 2006
- Cook, R. F.
- Journal of Materials Science, Vol. 41, Issue 3
The Tension of Metallic Films Deposited by Electrolysis
journal, May 1909
- Stoney, G. G.
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 82, Issue 553
On Plastic Deformation and Fracture in Si Films during Electrochemical Lithiation/Delithiation Cycling
journal, January 2013
- Nadimpalli, Siva P. V.; Sethuraman, Vijay A.; Bucci, Giovanna
- Journal of The Electrochemical Society, Vol. 160, Issue 10
Surface effects on the structure and lithium behavior in lithiated silicon: A first principles study
journal, June 2013
- Chou, Chia-Yun; Hwang, Gyeong S.
- Surface Science, Vol. 612
Robustness of amorphous silicon during the initial lithiation/delithiation cycle
journal, July 2014
- Berla, Lucas A.; Lee, Seok Woo; Ryu, Ill
- Journal of Power Sources, Vol. 258
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
Tough Germanium Nanoparticles under Electrochemical Cycling
journal, March 2013
- Liang, Wentao; Yang, Hui; Fan, Feifei
- ACS Nano, Vol. 7, Issue 4
Increased cycling efficiency and rate capability of copper-coated silicon anodes in lithium-ion batteries
journal, January 2011
- Sethuraman, Vijay A.; Kowolik, Kristin; Srinivasan, Venkat
- Journal of Power Sources, Vol. 196, Issue 1
High-performance lithium battery anodes using silicon nanowires
book, October 2010
- Chan, Candace K.; Peng, Hailin; Liu, Gao
- Materials for Sustainable Energy: A Collection of Peer-Reviewed Research and Review Articles from Nature Publishing Group, p. 187-191
Increased Cycling Efficiency and Rate Capability of Copper-coated Silicon Anodes in Lithium-ion Batteries
text, January 2011
- Sethuraman, Vijay A.; Kowolik, Kristin; Srinivasan, Venkat
- arXiv
In Situ Measurements of Stress Evolution in Silicon Thin Films During Electrochemical Lithiation and Delithiation
text, January 2011
- Sethuraman, Vijay A.; Chon, Michael J.; Shimshak, Maxwell
- arXiv
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
Variation of stress with charging rate due to strain-rate sensitivity of silicon electrodes of Li-ion batteries
journal, December 2014
- Pharr, Matt; Suo, Zhigang; Vlassak, Joost J.
- Journal of Power Sources, Vol. 270
Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation
journal, August 2011
- Liu, Xiao Hua; Zheng, He; Zhong, Li
- Nano Letters, Vol. 11, Issue 8, p. 3312-3318
Two-Phase Electrochemical Lithiation in Amorphous Silicon
journal, January 2013
- Wang, Jiang Wei; He, Yu; Fan, Feifei
- Nano Letters, Vol. 13, Issue 2
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
Atomic-Scale Mechanisms of Sliding along an Interdiffused Li–Si–Cu Interface
journal, February 2015
- Wang, Haoran; Hou, Binyue; Wang, Xueju
- Nano Letters, Vol. 15, Issue 3
Quantitative Fracture Strength and Plasticity Measurements of Lithiated Silicon Nanowires by In Situ TEM Tensile Experiments
journal, October 2012
- Kushima, Akihiro; Huang, Jian Yu; Li, Ju
- ACS Nano, Vol. 6, Issue 11
Tough Germanium Nanoparticles under Electrochemical Cycling
journal, March 2013
- Liang, Wentao; Yang, Hui; Fan, Feifei
- ACS Nano, Vol. 7, Issue 4
The Tension of Metallic Films Deposited by Electrolysis
journal, May 1909
- Stoney, G. G.
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 82, Issue 553
Electrical Energy Storage for the Grid: A Battery of Choices
journal, November 2011
- Dunn, B.; Kamath, H.; Tarascon, J. -M.
- Science, Vol. 334, Issue 6058
Increased Cycling Efficiency and Rate Capability of Copper-coated Silicon Anodes in Lithium-ion Batteries
text, January 2011
- Sethuraman, Vijay A.; Kowolik, Kristin; Srinivasan, Venkat
- arXiv
Works referencing / citing this record:
Review of Recent Development of In Situ/Operando Characterization Techniques for Lithium Battery Research
journal, May 2019
- Liu, Dongqing; Shadike, Zulipiya; Lin, Ruoqian
- Advanced Materials, Vol. 31, Issue 28
“Self-Peel-Off” Transfer Produces Ultrathin Polyvinylidene-Fluoride-Based Flexible Nanodevices
journal, February 2017
- Tai, Yanlong; Lubineau, Gilles
- Advanced Science, Vol. 4, Issue 4
Dynamics of the Morphological Degradation of Si‐Based Anodes for Li‐Ion Batteries Characterized by In Situ Synchrotron X‐Ray Tomography
journal, March 2019
- Vanpeene, Victor; Villanova, Julie; King, Andrew
- Advanced Energy Materials, Vol. 9, Issue 18
In Situ TEM Investigation of ZnO Nanowires during Sodiation and Lithiation Cycling
journal, August 2017
- Asayesh-Ardakani, Hasti; Yao, Wentao; Yuan, Yifei
- Small Methods, Vol. 1, Issue 9
Theoretical analysis of the mechanical behavior in Li–ion battery cylindrical electrodes with phase transformation
journal, December 2019
- Weng, Li; Xu, Chengjun; Chen, Bingbing
- Acta Mechanica, Vol. 231, Issue 3
Characterization of Stress-Diffusion Coupling in Lithiated Germanium by Nanoindentation
journal, February 2018
- Papakyriakou, M.; Wang, X.; Xia, S.
- Experimental Mechanics, Vol. 58, Issue 4
In Situ Transmission Electron Microscopy Studies of Electrochemical Reaction Mechanisms in Rechargeable Batteries
journal, June 2019
- Wu, Xiaoyu; Li, Songmei; Yang, Bin
- Electrochemical Energy Reviews, Vol. 2, Issue 3
Strong stress-composition coupling in lithium alloy nanoparticles
journal, July 2019
- Seo, Hyeon Kook; Park, Jae Yeol; Chang, Joon Ha
- Nature Communications, Vol. 10, Issue 1
Ultrahigh energy storage and ultrafast ion diffusion in borophene-based anodes for rechargeable metal ion batteries
journal, January 2017
- Rao, Dewei; Zhang, Lingyan; Meng, Zhaoshun
- Journal of Materials Chemistry A, Vol. 5, Issue 5
Harnessing the concurrent reaction dynamics in active Si and Ge to achieve high performance lithium-ion batteries
journal, January 2018
- Zhang, Qiaobao; Chen, Huixin; Luo, Langli
- Energy & Environmental Science, Vol. 11, Issue 3
A facile method to fabricate a porous Si/C composite with excellent cycling stability for use as the anode in a lithium ion battery
journal, January 2019
- Zhang, Xiaosong; Zhou, Le; Zhang, Yi
- Chemical Communications, Vol. 55, Issue 89
Two-dimensional porous silicon nanosheets as anode materials for high performance lithium-ion batteries
journal, January 2019
- Tang, Jingjing; Yin, Qifang; Wang, Qian
- Nanoscale, Vol. 11, Issue 22
A phase-field study of the effect of local deformation velocity on lithiation-induced stress in wire-like structures
journal, February 2019
- Zhang, Kai; Li, Yong; Wang, Feng
- Journal of Physics D: Applied Physics, Vol. 52, Issue 14
In Situ Measurement of the Effect of Stress on the Chemical Diffusion Coefficient of Li in High-Energy-Density Electrodes
journal, January 2018
- Tripuraneni, Rajasekhar; Rakshit, Subhajit; Nadimpalli, Siva P. V.
- Journal of The Electrochemical Society, Vol. 165, Issue 10
Review—Promises and Challenges of In Situ Transmission Electron Microscopy Electrochemical Techniques in the Studies of Lithium Ion Batteries
journal, January 2017
- Xie, Zhi-Hui; Jiang, Zimin; Zhang, Xueyuan
- Journal of The Electrochemical Society, Vol. 164, Issue 9
“Self-Peel-Off” Transfer Produces Ultrathin Polyvinylidene-Fluoride-Based Flexible Nanodevices
journal, February 2017
- Tai, Yanlong; Lubineau, Gilles
- Advanced Science, Vol. 4, Issue 4
Strong stress-composition coupling in lithium alloy nanoparticles
journal, July 2019
- Seo, Hyeon Kook; Park, Jae Yeol; Chang, Joon Ha
- Nature Communications, Vol. 10, Issue 1