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Title: Bending-induced Symmetry Breaking of Lithiation in Germanium Nanowires

Abstract

From signal transduction of living cells to oxidation and corrosion of metals, mechanical stress intimately couples with chemical reactions, regulating these biological and physiochemical processes. The coupled effect is particularly evident in electrochemical lithiation/delithiation cycling of high-capacity electrodes, such as silicon (Si), where on one hand lithiation-generated stress mediates lithiation kinetics, and on the other electrochemical reaction rate regulates stress generation and mechanical failure of the electrodes. Here we report for the first time the evidence on the controlled lithiation in germanium nanowires (GeNWs) through external bending. Contrary to the symmetric core-shell lithiation in free-standing GeNWs, we show bending GeNWs breaks the lithiation symmetry, speeding up lithaition at the tensile side while slowing down at the compressive side of the GeNWs. The bending-induced symmetry breaking of lithiation in GeNWs is further corroborated by chemomechanical modeling. In the light of the coupled effect between lithiation kinetics and mechanical stress in the electrochemical cycling, our findings shed light on strain/stress engineering of durable high-rate electrodes and energy harvesting through mechanical motion.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1170461
Report Number(s):
PNNL-SA-103596
48170
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nano Letters, 14(8):4622-4627
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Gu, Meng, Yang, Hui, Perea, Daniel E., Zhang, Jiguang, Zhang, Sulin, and Wang, Chong M. Bending-induced Symmetry Breaking of Lithiation in Germanium Nanowires. United States: N. p., 2014. Web. doi:10.1021/nl501680w.
Gu, Meng, Yang, Hui, Perea, Daniel E., Zhang, Jiguang, Zhang, Sulin, & Wang, Chong M. Bending-induced Symmetry Breaking of Lithiation in Germanium Nanowires. United States. doi:10.1021/nl501680w.
Gu, Meng, Yang, Hui, Perea, Daniel E., Zhang, Jiguang, Zhang, Sulin, and Wang, Chong M. Fri . "Bending-induced Symmetry Breaking of Lithiation in Germanium Nanowires". United States. doi:10.1021/nl501680w.
@article{osti_1170461,
title = {Bending-induced Symmetry Breaking of Lithiation in Germanium Nanowires},
author = {Gu, Meng and Yang, Hui and Perea, Daniel E. and Zhang, Jiguang and Zhang, Sulin and Wang, Chong M.},
abstractNote = {From signal transduction of living cells to oxidation and corrosion of metals, mechanical stress intimately couples with chemical reactions, regulating these biological and physiochemical processes. The coupled effect is particularly evident in electrochemical lithiation/delithiation cycling of high-capacity electrodes, such as silicon (Si), where on one hand lithiation-generated stress mediates lithiation kinetics, and on the other electrochemical reaction rate regulates stress generation and mechanical failure of the electrodes. Here we report for the first time the evidence on the controlled lithiation in germanium nanowires (GeNWs) through external bending. Contrary to the symmetric core-shell lithiation in free-standing GeNWs, we show bending GeNWs breaks the lithiation symmetry, speeding up lithaition at the tensile side while slowing down at the compressive side of the GeNWs. The bending-induced symmetry breaking of lithiation in GeNWs is further corroborated by chemomechanical modeling. In the light of the coupled effect between lithiation kinetics and mechanical stress in the electrochemical cycling, our findings shed light on strain/stress engineering of durable high-rate electrodes and energy harvesting through mechanical motion.},
doi = {10.1021/nl501680w},
journal = {Nano Letters, 14(8):4622-4627},
number = ,
volume = ,
place = {United States},
year = {Fri Aug 01 00:00:00 EDT 2014},
month = {Fri Aug 01 00:00:00 EDT 2014}
}