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Title: Investigation of Solid Electrolyte Interphase Formed on Si Nanoparticle Composite Electrodes Using Hyperpolarized 129Xe Nuclear Magnetic Resonance Spectroscopy

Abstract

Solid electrolyte interphase (SEI) plays an important role in determining electrochemical performances of Li-ion batteries. The ideal SEI layer protects the electrolyte from being further reduced on the electrode surface and allows Li-ion diffusion in and out of electrodes without any consumption. However, degradation of the SEI layer over time, which contributes to the thickening of the SEI layer, is a leading pathway for gradual capacity fade. In this study, a hyperpolarized (HP) 129Xe nuclear magnetic resonance (NMR) technique was applied for the first time to probe changes in porosity and connectivity in Si nanoparticle composite electrodes as a result of the SEI formation. Nanopores are present in nanocomposite electrodes as a result of aggregation of the constituting nanoparticles. The connectivity among nanopores greatly affects the ion transport property of the electrode materials, which has a substantial influence on the overall energy output of Li-ion batteries. Here, information on thickness, uniformity of the SEI layer, and connectivity of the pores in the composite electrodes upon growing SEI was obtained from the analysis of temperature-dependent HP 129Xe NMR spectra. Such information is useful for gaining a better understanding of the degradation mechanism of SEI. This study demonstrates that HP 129Xe NMRmore » is a potentially unique tool in probing the porosity and connectivity changes in porous practical electrodes during electrochemical cycling.« less

Authors:
 [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Brown Univ., Providence, RI (United States)
Publication Date:
Research Org.:
Brown Univ., Providence, RI (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1534483
Grant/Contract Number:  
SC0007074; HRD-0548311
Resource Type:
Accepted Manuscript
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 31; Journal Issue: 5; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; energy & fuels; engineering; semiconducting nanostructured materials; layers; nanoparticles; electrodes; surface chemistry

Citation Formats

Mao, Yougang, Karan, Naba K., Song, Myeonghun, Hopson, Russell, Guduru, Pradeep R., and Wang, Li-Qiong. Investigation of Solid Electrolyte Interphase Formed on Si Nanoparticle Composite Electrodes Using Hyperpolarized 129Xe Nuclear Magnetic Resonance Spectroscopy. United States: N. p., 2017. Web. doi:10.1021/acs.energyfuels.7b00250.
Mao, Yougang, Karan, Naba K., Song, Myeonghun, Hopson, Russell, Guduru, Pradeep R., & Wang, Li-Qiong. Investigation of Solid Electrolyte Interphase Formed on Si Nanoparticle Composite Electrodes Using Hyperpolarized 129Xe Nuclear Magnetic Resonance Spectroscopy. United States. https://doi.org/10.1021/acs.energyfuels.7b00250
Mao, Yougang, Karan, Naba K., Song, Myeonghun, Hopson, Russell, Guduru, Pradeep R., and Wang, Li-Qiong. Mon . "Investigation of Solid Electrolyte Interphase Formed on Si Nanoparticle Composite Electrodes Using Hyperpolarized 129Xe Nuclear Magnetic Resonance Spectroscopy". United States. https://doi.org/10.1021/acs.energyfuels.7b00250. https://www.osti.gov/servlets/purl/1534483.
@article{osti_1534483,
title = {Investigation of Solid Electrolyte Interphase Formed on Si Nanoparticle Composite Electrodes Using Hyperpolarized 129Xe Nuclear Magnetic Resonance Spectroscopy},
author = {Mao, Yougang and Karan, Naba K. and Song, Myeonghun and Hopson, Russell and Guduru, Pradeep R. and Wang, Li-Qiong},
abstractNote = {Solid electrolyte interphase (SEI) plays an important role in determining electrochemical performances of Li-ion batteries. The ideal SEI layer protects the electrolyte from being further reduced on the electrode surface and allows Li-ion diffusion in and out of electrodes without any consumption. However, degradation of the SEI layer over time, which contributes to the thickening of the SEI layer, is a leading pathway for gradual capacity fade. In this study, a hyperpolarized (HP) 129Xe nuclear magnetic resonance (NMR) technique was applied for the first time to probe changes in porosity and connectivity in Si nanoparticle composite electrodes as a result of the SEI formation. Nanopores are present in nanocomposite electrodes as a result of aggregation of the constituting nanoparticles. The connectivity among nanopores greatly affects the ion transport property of the electrode materials, which has a substantial influence on the overall energy output of Li-ion batteries. Here, information on thickness, uniformity of the SEI layer, and connectivity of the pores in the composite electrodes upon growing SEI was obtained from the analysis of temperature-dependent HP 129Xe NMR spectra. Such information is useful for gaining a better understanding of the degradation mechanism of SEI. This study demonstrates that HP 129Xe NMR is a potentially unique tool in probing the porosity and connectivity changes in porous practical electrodes during electrochemical cycling.},
doi = {10.1021/acs.energyfuels.7b00250},
journal = {Energy and Fuels},
number = 5,
volume = 31,
place = {United States},
year = {Mon Apr 03 00:00:00 EDT 2017},
month = {Mon Apr 03 00:00:00 EDT 2017}
}

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Figures / Tables:

Table I Table I: ΔHads, δs and D values are listed based on the variable temperature chemical shift data

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.