• Login
    • Submit
    View Item 
    •   Repository Home
    • UT Electronic Theses and Dissertations
    • UT Electronic Theses and Dissertations
    • View Item
    • Repository Home
    • UT Electronic Theses and Dissertations
    • UT Electronic Theses and Dissertations
    • View Item
    JavaScript is disabled for your browser. Some features of this site may not work without it.

    First principles study of silicon-based nanomaterials for lithium ion battery anodes

    Icon
    View/Open
    CHOU-DISSERTATION-2014.pdf (18.76Mb)
    Date
    2014-05
    Author
    Chou, Chia-Yun Ph. D.
    Share
     Facebook
     Twitter
     LinkedIn
    Metadata
    Show full item record
    Abstract
    Silicon (Si)-based materials have recently emerged as a promising candidate for anodes in lithium-ion batteries because they exhibit much higher energy-storage capacities than the conventional graphite anode. However, the practical use of Si is hampered by its poor cycleability; during lithiation, Si forms alloys with Li and undergoes significant structural and volume changes, which can cause severe cracking/pulverization and consequent capacity fading arising from the loss of electrical contacts. To overcome these drawbacks, many innovative approaches have been explored with encouraging results; however, many fundamental aspects of the lithiation behavior remain ambiguous. Hence, the focus of this work is to develop a better understanding of the lithiation process at the atomistic scale using quantum mechanical calculations. In addition, based on the improved understanding, we attempt to address the fundamental mechanisms behind the successful approaches to enhance the anode performance. To lay a foundation for the investigation of alloy-type anodes, in Chapter 3, we first examine how lithiation occurs in Si and the formation of crystalline and amorphous LixSi alloys (0 ≤ x ≤ 4); followed by assessing the lithiation-induced changes in the energetics, atomic structure, electronic and mechanical properties, and Li diffusivity. The same approach is then extended to analyze the lithiation behavior of germanium (Ge) and tin (Sn) for developing a generalized understanding on the Group IV alloy-type anodes. Along this comparative study, we notice a few distinguishing features pertain only to Si (or Ge), such as the facile Li diffusion in Ge and facet-dependent lithiation in Si, which are discussed in Chapter 4. Beyond the fundamental research, we also look into factors that may contribute to the improved anode performance, including (i) finetuning of the oxidation effects in Si-rich oxides, [alpha] -SiO [subscript 1/3] (Chapter 5), (ii) maximizing the surface effects through nano-engineered structures (Chapters 6 & 7), and finally (iii) the role of interface in Si-graphene (carbon) composites (Chapter 8).
    Department
    Materials Science and Engineering
    Subject
    Silicon
    Anode
    Lithium ion battery
    Density functional theory
    URI
    http://hdl.handle.net/2152/30499
    Collections
    • UT Electronic Theses and Dissertations
    University of Texas at Austin Libraries
    • facebook
    • twitter
    • instagram
    • youtube
    • CONTACT US
    • MAPS & DIRECTIONS
    • JOB OPPORTUNITIES
    • UT Austin Home
    • Emergency Information
    • Site Policies
    • Web Accessibility Policy
    • Web Privacy Policy
    • Adobe Reader
    Subscribe to our NewsletterGive to the Libraries

    © The University of Texas at Austin

    Browse

    Entire RepositoryCommunities & CollectionsDate IssuedAuthorsTitlesSubjectsDepartmentThis CollectionDate IssuedAuthorsTitlesSubjectsDepartment

    My Account

    Login

    Information

    AboutContactPoliciesGetting StartedGlossaryHelpFAQs

    Statistics

    View Usage Statistics
    University of Texas at Austin Libraries
    • facebook
    • twitter
    • instagram
    • youtube
    • CONTACT US
    • MAPS & DIRECTIONS
    • JOB OPPORTUNITIES
    • UT Austin Home
    • Emergency Information
    • Site Policies
    • Web Accessibility Policy
    • Web Privacy Policy
    • Adobe Reader
    Subscribe to our NewsletterGive to the Libraries

    © The University of Texas at Austin