High damage tolerance of electrochemically lithiated silicon

Wang, Xueju; Fan, Feifei; Wang, Jiangwei; Wang, Haoran; Tao, Siyu; Yang, Avery; Liu, Yang; Beng Chew, Huck; Mao, Scott X.; Zhu, Ting; Xia, Shuman

doi:10.1038/ncomms9417

High damage tolerance of electrochemically lithiated silicon

Journal Article · Thu Sep 24 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms9417· OSTI ID:1261096

Wang, Xueju ^[1]; Fan, Feifei ^[1]; Wang, Jiangwei ^[2]; Wang, Haoran ^[3]; Tao, Siyu ^[1]; Yang, Avery ^[1]; Liu, Yang ^[4]; Beng Chew, Huck ^[3]; Mao, Scott X. ^[2]; Zhu, Ting ^[1]; Xia, Shuman ^[1]

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

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.

View Accepted Manuscript (DOE)

Research Organization:: Georgia Inst. of Technology, Atlanta, GA (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: National Science Foundation (NSF) (United States); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Contributing Organization:: Univ. of Illinois, Urbana, IL (United States); Univ. of Pittsburgh, PA (United States)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1261096

Alternate ID(s):: OSTI ID: 1347348

Report Number(s):: SAND2015--5484J; ncomms9417

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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