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Title: Mechanical Properties and Chemical Reactivity of Li xSiO y Thin Films

Abstract

Silicon (Si) is a commonly studied candidate material for next-generation anodes in Li-ion batteries. A native oxide SiO 2 on Si is often inevitable. However, it is not clear if this layer has a positive or negative effect on the battery performance. This understanding is complicated by the lack of knowledge about the physical properties of the SiO 2 lithiation products and by the convolution of chemical and electrochemical effects during the anode lithiation process. In this study, Li xSiO y thin films as model materials for lithiated SiO 2 were deposited by magnetron sputtering at ambient temperature, with the goal of (1) decoupling chemical reactivity from electrochemical reactivity and (2) evaluating the physical and electrochemical properties of Li xSiO y. X-ray photoemission spectroscopy analysis of the deposited thin films demonstrate that a composition close to previous experimental reports of lithiated native SiO 2 can be achieved through sputtering. Our density functional theory calculations also confirm that the possible phases formed by lithiating SiO 2 are very close to the measured film compositions. Scanning probe microscopy measurements show that the mechanical properties of the film are strongly dependent on lithium concentration, with a ductile behavior at a higher Li contentmore » and a brittle behavior at a lower Li content. The chemical reactivity of the thin films was investigated by measuring the AC impedance evolution, suggesting that Li xSiO y continuously reacts with the electrolyte, in part because of the high electronic conductivity of the film determined from solid-state impedance measurements. The electrochemical cycling data of the sputter-deposited Li xSiO y/Si films also suggest that Li xSiO y is not beneficial in stabilizing the Si anode surface during battery operation, despite its favorable mechanical properties.« less

Authors:
ORCiD logo [1];  [2];  [1];  [3]; ORCiD logo [1];  [1]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [5];  [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Colorado School of Mines, Golden, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Colorado School of Mines, Golden, CO (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1480917
Report Number(s):
NREL/JA-5K00-72507
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 44; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 25 ENERGY STORAGE; chemical reactivity; lithium ion batteries; LixSiOy; mechanical properties; solid electrolyte interphases

Citation Formats

Xu, Yun, Stetson, Caleb, Wood, Kevin, Sivonxay, Eric, Jiang, Chunsheng, Teeter, Glenn, Pylypenko, Svitlana, Han, Sang-Don, Persson, Kristin A., Burrell, Anthony, and Zakutayev, Andriy. Mechanical Properties and Chemical Reactivity of LixSiOy Thin Films. United States: N. p., 2018. Web. doi:10.1021/acsami.8b10895.
Xu, Yun, Stetson, Caleb, Wood, Kevin, Sivonxay, Eric, Jiang, Chunsheng, Teeter, Glenn, Pylypenko, Svitlana, Han, Sang-Don, Persson, Kristin A., Burrell, Anthony, & Zakutayev, Andriy. Mechanical Properties and Chemical Reactivity of LixSiOy Thin Films. United States. doi:10.1021/acsami.8b10895.
Xu, Yun, Stetson, Caleb, Wood, Kevin, Sivonxay, Eric, Jiang, Chunsheng, Teeter, Glenn, Pylypenko, Svitlana, Han, Sang-Don, Persson, Kristin A., Burrell, Anthony, and Zakutayev, Andriy. Mon . "Mechanical Properties and Chemical Reactivity of LixSiOy Thin Films". United States. doi:10.1021/acsami.8b10895.
@article{osti_1480917,
title = {Mechanical Properties and Chemical Reactivity of LixSiOy Thin Films},
author = {Xu, Yun and Stetson, Caleb and Wood, Kevin and Sivonxay, Eric and Jiang, Chunsheng and Teeter, Glenn and Pylypenko, Svitlana and Han, Sang-Don and Persson, Kristin A. and Burrell, Anthony and Zakutayev, Andriy},
abstractNote = {Silicon (Si) is a commonly studied candidate material for next-generation anodes in Li-ion batteries. A native oxide SiO2 on Si is often inevitable. However, it is not clear if this layer has a positive or negative effect on the battery performance. This understanding is complicated by the lack of knowledge about the physical properties of the SiO2 lithiation products and by the convolution of chemical and electrochemical effects during the anode lithiation process. In this study, LixSiOy thin films as model materials for lithiated SiO2 were deposited by magnetron sputtering at ambient temperature, with the goal of (1) decoupling chemical reactivity from electrochemical reactivity and (2) evaluating the physical and electrochemical properties of LixSiOy. X-ray photoemission spectroscopy analysis of the deposited thin films demonstrate that a composition close to previous experimental reports of lithiated native SiO2 can be achieved through sputtering. Our density functional theory calculations also confirm that the possible phases formed by lithiating SiO2 are very close to the measured film compositions. Scanning probe microscopy measurements show that the mechanical properties of the film are strongly dependent on lithium concentration, with a ductile behavior at a higher Li content and a brittle behavior at a lower Li content. The chemical reactivity of the thin films was investigated by measuring the AC impedance evolution, suggesting that LixSiOy continuously reacts with the electrolyte, in part because of the high electronic conductivity of the film determined from solid-state impedance measurements. The electrochemical cycling data of the sputter-deposited LixSiOy/Si films also suggest that LixSiOy is not beneficial in stabilizing the Si anode surface during battery operation, despite its favorable mechanical properties.},
doi = {10.1021/acsami.8b10895},
journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 44,
volume = 10,
place = {United States},
year = {2018},
month = {10}
}

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