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Title: Type I clathrates as novel silicon anodes: An electrochemical and structural investigation

Abstract

In this study, silicon clathrates contain cage-like structures that can encapsulate various guest atoms or molecules. Here we present an electrochemical evaluation of type I silicon clathrates based on Ba8AlySi46-y for the anode material in lithium-ion batteries. Post-cycling characterization with NMR and XRD show no discernible structural or volume changes even after electrochemical insertion of 44 Li into the clathrate structure. The observed properties are in stark contrast with lithiation of other silicon anodes, which become amorphous and suffer from larger volume changes. The lithiation/delithiation processes are proposed to occur in single phase reactions at approximately 0.2 and 0.4 V vs. Li/Li+, respectively, distinct from other diamond cubic or amorphous silicon anodes. Reversible capacities as high as 499 mAh g-1 at a 5 mA g-1 rate were observed for silicon clathrate with composition Ba8Al8.54Si37.46, corresponding to Li:Si of 1.18:1. The results show that silicon clathrates could be promising durable anodes for lithium-ion batteries.

Authors:
 [1];  [1];  [1];  [1];  [2];  [1];  [1];  [1];  [2];  [3];  [3];  [3];  [1]
+ Show Author Affiliations
  1. Arizona State Univ., Tempe, AZ (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Southwest Research Institute, San Antonio, TX (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1185934
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 2; Journal Issue: 6; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Li, Ying, Raghavan, Rahul, Wagner, Nicholas A., Davidowski, Stephen K., Baggetto, Loic, Zhao, Ran, Cheng, Qian, Yarger, Jeffery L., Veith, Gabriel M., Ellis-Terrell, Carol, Miller, Michael A., Chan, Kwai S., and Chan, Candace K. Type I clathrates as novel silicon anodes: An electrochemical and structural investigation. United States: N. p., 2015. Web. doi:10.1002/advs.201500057.
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Li, Ying, Raghavan, Rahul, Wagner, Nicholas A., Davidowski, Stephen K., Baggetto, Loic, Zhao, Ran, Cheng, Qian, Yarger, Jeffery L., Veith, Gabriel M., Ellis-Terrell, Carol, Miller, Michael A., Chan, Kwai S., & Chan, Candace K. Type I clathrates as novel silicon anodes: An electrochemical and structural investigation. United States. https://doi.org/10.1002/advs.201500057
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Li, Ying, Raghavan, Rahul, Wagner, Nicholas A., Davidowski, Stephen K., Baggetto, Loic, Zhao, Ran, Cheng, Qian, Yarger, Jeffery L., Veith, Gabriel M., Ellis-Terrell, Carol, Miller, Michael A., Chan, Kwai S., and Chan, Candace K. Tue . "Type I clathrates as novel silicon anodes: An electrochemical and structural investigation". United States. https://doi.org/10.1002/advs.201500057. https://www.osti.gov/servlets/purl/1185934.
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@article{osti_1185934,
title = {Type I clathrates as novel silicon anodes: An electrochemical and structural investigation},
author = {Li, Ying and Raghavan, Rahul and Wagner, Nicholas A. and Davidowski, Stephen K. and Baggetto, Loic and Zhao, Ran and Cheng, Qian and Yarger, Jeffery L. and Veith, Gabriel M. and Ellis-Terrell, Carol and Miller, Michael A. and Chan, Kwai S. and Chan, Candace K.},
abstractNote = {In this study, silicon clathrates contain cage-like structures that can encapsulate various guest atoms or molecules. Here we present an electrochemical evaluation of type I silicon clathrates based on Ba8AlySi46-y for the anode material in lithium-ion batteries. Post-cycling characterization with NMR and XRD show no discernible structural or volume changes even after electrochemical insertion of 44 Li into the clathrate structure. The observed properties are in stark contrast with lithiation of other silicon anodes, which become amorphous and suffer from larger volume changes. The lithiation/delithiation processes are proposed to occur in single phase reactions at approximately 0.2 and 0.4 V vs. Li/Li+, respectively, distinct from other diamond cubic or amorphous silicon anodes. Reversible capacities as high as 499 mAh g-1 at a 5 mA g-1 rate were observed for silicon clathrate with composition Ba8Al8.54Si37.46, corresponding to Li:Si of 1.18:1. The results show that silicon clathrates could be promising durable anodes for lithium-ion batteries.},
doi = {10.1002/advs.201500057},
journal = {Advanced Science},
number = 6,
volume = 2,
place = {United States},
year = {Tue May 05 00:00:00 EDT 2015},
month = {Tue May 05 00:00:00 EDT 2015}
}
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https://doi.org/10.1002/advs.201500057
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High-performance lithium-ion anodes using a hierarchical bottom-up approach
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Superconductivity in Doped s p 3 Semiconductors: The Case of the Clathrates
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