skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Electron-Rich Driven Electrochemical Solid-State Amorphization in Li-Si Alloys

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.

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1094948
Report Number(s):
PNNL-SA-97210
47714
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Nano Letters, 13(9):4511-4516
Additional Journal Information:
Journal Name: Nano Letters, 13(9):4511-4516
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Wang, Zhiguo, Gu, Meng, Zhou, Yungang, Zu, Xiaotao, Connell, Justin G., Xiao, Jie, Perea, Daniel E., Lauhon, Lincoln J., Bang, Junhyeok, Zhang, Shengbai, Wang, Chong M., and Gao, Fei. Electron-Rich Driven Electrochemical Solid-State Amorphization in Li-Si Alloys. United States: N. p., 2013. Web. doi:10.1021/nl402429a.
Wang, Zhiguo, Gu, Meng, Zhou, Yungang, Zu, Xiaotao, Connell, Justin G., Xiao, Jie, Perea, Daniel E., Lauhon, Lincoln J., Bang, Junhyeok, Zhang, Shengbai, Wang, Chong M., & Gao, Fei. Electron-Rich Driven Electrochemical Solid-State Amorphization in Li-Si Alloys. United States. https://doi.org/10.1021/nl402429a
Wang, Zhiguo, Gu, Meng, Zhou, Yungang, Zu, Xiaotao, Connell, Justin G., Xiao, Jie, Perea, Daniel E., Lauhon, Lincoln J., Bang, Junhyeok, Zhang, Shengbai, Wang, Chong M., and Gao, Fei. 2013. "Electron-Rich Driven Electrochemical Solid-State Amorphization in Li-Si Alloys". United States. https://doi.org/10.1021/nl402429a.
@article{osti_1094948,
title = {Electron-Rich Driven Electrochemical Solid-State Amorphization in Li-Si Alloys},
author = {Wang, Zhiguo and Gu, Meng and Zhou, Yungang and Zu, Xiaotao and Connell, Justin G. and Xiao, Jie and Perea, Daniel E. and Lauhon, Lincoln J. and Bang, Junhyeok and Zhang, Shengbai and Wang, Chong M. and Gao, Fei},
abstractNote = {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.},
doi = {10.1021/nl402429a},
url = {https://www.osti.gov/biblio/1094948}, journal = {Nano Letters, 13(9):4511-4516},
number = ,
volume = ,
place = {United States},
year = {Wed Aug 14 00:00:00 EDT 2013},
month = {Wed Aug 14 00:00:00 EDT 2013}
}