Fracture of crystalline silicon nanopillars during electrochemical lithium insertion

Handle URI:
http://hdl.handle.net/10754/598364
Title:
Fracture of crystalline silicon nanopillars during electrochemical lithium insertion
Authors:
Lee, S. W.; McDowell, M. T.; Berla, L. A.; Nix, W. D.; Cui, Y.
Abstract:
From surface hardening of steels to doping of semiconductors, atom insertion in solids plays an important role in modifying chemical, physical, and electronic properties of materials for a variety of applications. High densities of atomic insertion in a solid can result in dramatic structural transformations and associated changes in mechanical behavior: This is particularly evident during electrochemical cycling of novel battery electrodes, such as alloying anodes, conversion oxides, and sulfur and oxygen cathodes. Silicon, which undergoes 400% volume expansion when alloying with lithium, is an extreme case and represents an excellent model system for study. Here, we show that fracture locations are highly anisotropic for lithiation of crystalline Si nanopillars and that fracture is strongly correlated with previously discovered anisotropic expansion. Contrary to earlier theoretical models based on diffusion-induced stresses where fracture is predicted to occur in the core of the pillars during lithiation, the observed cracks are present only in the amorphous lithiated shell. We also show that the critical fracture size is between about 240 and 360 nm and that it depends on the electrochemical reaction rate.
Citation:
Lee SW, McDowell MT, Berla LA, Nix WD, Cui Y (2012) Fracture of crystalline silicon nanopillars during electrochemical lithium insertion. Proceedings of the National Academy of Sciences 109: 4080–4085. Available: http://dx.doi.org/10.1073/pnas.1201088109.
Publisher:
Proceedings of the National Academy of Sciences
Journal:
Proceedings of the National Academy of Sciences
KAUST Grant Number:
KUS-l1-001-12; KUK-F1-038-02
Issue Date:
27-Feb-2012
DOI:
10.1073/pnas.1201088109
PubMed ID:
22371565
PubMed Central ID:
PMC3306693
Type:
Article
ISSN:
0027-8424; 1091-6490
Sponsors:
A portion of this work is supported by the US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Contract DE-AC02-76SF00515 through the Stanford Linear Accelerator Center National Accelerator Laboratory, Laboratory Directed Research and Development project and Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US DOE under Contract DE-AC02-05CH11231, Subcontract 6951379 under the Batteries for Advanced Transportation Technologies Program. Y.C. acknowledges support from the King Abdullah University of Science and Technology (KAUST) Investigator Award (KUS-l1-001-12). S. W. L. acknowledges support from KAUST (KUK-F1-038-02). M. T. M. acknowledges support from the Chevron Stanford Graduate Fellowship, the National Defense Science and Engineering Graduate Fellowship, and the National Science Foundation Graduate Fellowship. L. A. B. acknowledges support from the National Science Foundation Graduate Research Fellowship and, together with W.D.N., gratefully acknowledges support from the Office of Science, Office of Basic Energy Sciences, of the US DOE under Contract DE-FG02-04-ER46163.
Appears in Collections:
Publications Acknowledging KAUST Support

Full metadata record

DC FieldValue Language
dc.contributor.authorLee, S. W.en
dc.contributor.authorMcDowell, M. T.en
dc.contributor.authorBerla, L. A.en
dc.contributor.authorNix, W. D.en
dc.contributor.authorCui, Y.en
dc.date.accessioned2016-02-25T13:19:27Zen
dc.date.available2016-02-25T13:19:27Zen
dc.date.issued2012-02-27en
dc.identifier.citationLee SW, McDowell MT, Berla LA, Nix WD, Cui Y (2012) Fracture of crystalline silicon nanopillars during electrochemical lithium insertion. Proceedings of the National Academy of Sciences 109: 4080–4085. Available: http://dx.doi.org/10.1073/pnas.1201088109.en
dc.identifier.issn0027-8424en
dc.identifier.issn1091-6490en
dc.identifier.pmid22371565en
dc.identifier.doi10.1073/pnas.1201088109en
dc.identifier.urihttp://hdl.handle.net/10754/598364en
dc.description.abstractFrom surface hardening of steels to doping of semiconductors, atom insertion in solids plays an important role in modifying chemical, physical, and electronic properties of materials for a variety of applications. High densities of atomic insertion in a solid can result in dramatic structural transformations and associated changes in mechanical behavior: This is particularly evident during electrochemical cycling of novel battery electrodes, such as alloying anodes, conversion oxides, and sulfur and oxygen cathodes. Silicon, which undergoes 400% volume expansion when alloying with lithium, is an extreme case and represents an excellent model system for study. Here, we show that fracture locations are highly anisotropic for lithiation of crystalline Si nanopillars and that fracture is strongly correlated with previously discovered anisotropic expansion. Contrary to earlier theoretical models based on diffusion-induced stresses where fracture is predicted to occur in the core of the pillars during lithiation, the observed cracks are present only in the amorphous lithiated shell. We also show that the critical fracture size is between about 240 and 360 nm and that it depends on the electrochemical reaction rate.en
dc.description.sponsorshipA portion of this work is supported by the US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Contract DE-AC02-76SF00515 through the Stanford Linear Accelerator Center National Accelerator Laboratory, Laboratory Directed Research and Development project and Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US DOE under Contract DE-AC02-05CH11231, Subcontract 6951379 under the Batteries for Advanced Transportation Technologies Program. Y.C. acknowledges support from the King Abdullah University of Science and Technology (KAUST) Investigator Award (KUS-l1-001-12). S. W. L. acknowledges support from KAUST (KUK-F1-038-02). M. T. M. acknowledges support from the Chevron Stanford Graduate Fellowship, the National Defense Science and Engineering Graduate Fellowship, and the National Science Foundation Graduate Fellowship. L. A. B. acknowledges support from the National Science Foundation Graduate Research Fellowship and, together with W.D.N., gratefully acknowledges support from the Office of Science, Office of Basic Energy Sciences, of the US DOE under Contract DE-FG02-04-ER46163.en
dc.publisherProceedings of the National Academy of Sciencesen
dc.subjectAnisotropyen
dc.subjectLithium ion batteryen
dc.subjectPlasticityen
dc.subjectSilicon anodeen
dc.titleFracture of crystalline silicon nanopillars during electrochemical lithium insertionen
dc.typeArticleen
dc.identifier.journalProceedings of the National Academy of Sciencesen
dc.identifier.pmcidPMC3306693en
dc.contributor.institutionStanford University, Palo Alto, United Statesen
dc.contributor.institutionStanford Linear Accelerator Center, Menlo Park, United Statesen
kaust.grant.numberKUS-l1-001-12en
kaust.grant.numberKUK-F1-038-02en

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