Electron-rich driven electrochemical solid-state amorphization in Li-Si alloys

Zhiguo Wang*, Meng Gu, Yungang Zhou, Xiaotao Zu, Justin G. Connell, Jie Xiao, Daniel Perea, Lincoln J. Lauhon, Junhyeok Bang, Shengbai Zhang, Chongmin Wang, Fei Gao

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

37 Scopus citations

Abstract

The physical and chemical behaviors of materials used in energy storage devices, such as lithium-ion batteries (LIBs), are mainly controlled by an electrochemical process, which normally involves insertion/extraction of ions into/from a host lattice with a concurrent flow of electrons to compensate charge balance. The fundamental physics and chemistry governing the behavior of materials in response to the ions insertion/extraction is not known. Herein, a combination of in situ lithiation experiments and large-scale ab initio molecular dynamics simulations are performed to explore the mechanisms of the electrochemically driven solid-state amorphization in Li-Si systems. We find that local electron-rich condition governs the electrochemically driven solid-state amorphization of Li-Si alloys. This discovery provides the fundamental explanation of why lithium insertion in semiconductor and insulators leads to amorphization, whereas in metals, it leads to a crystalline alloy. The present work correlates electrochemically driven reactions with ion insertion, electron transfer, lattice stability, and phase equilibrium.

Original languageEnglish (US)
Pages (from-to)4511-4516
Number of pages6
JournalNano letters
Volume13
Issue number9
DOIs
StatePublished - Sep 11 2013

Keywords

  • Li-Si alloys
  • ab initio molecular dynamics simulations
  • electrochemical solid-state amorphization
  • electron rich
  • in situ TEM

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

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