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Title: Structure and Ionic Conductivity of Polystyrene-block-poly(ethylene oxide) Electrolytes in the High Salt Concentration Limit

Abstract

We explore the relationship between the morphology and ionic conductivity of block copolymer electrolytes over a wide range of salt concentrations for the system polystyrene-block-poly(ethylene oxide) (PS-b-PEO, SEO) mixed with lithium bis-(trifluoromethanesulfonyl)imide salt (LiTFSI). Two SEO polymers were studied, SEO(16-16) and SEO(4.9-5.5), over the salt concentration range r = 0.03-0.55. The numbers x and y in SEO(x-y) are the molecular weights of the blocks in kg mol -1, and the r value is the molar ratio of salt to ethylene oxide moieties. Small-angle X-ray scattering was used to characterize morphology and grain size at 120 °C, differential scanning calorimetry was used to study the crystallinity and the glass transition temperature of the PEO-rich microphase, and ac impedance spectroscopy was used to measure ionic conductivity as a function of temperature. The most surprising observation of our study is that ionic conductivity in the concentration regime 0.11 ≤ r ≤ 0.21 increases in SEO electrolytes but decreases in PEO electrolytes. The maximum in ionic conductivity with salt concentration occurs at about twice the salt concentration in SEO (r = 0.21) as in PEO (r = 0.11). Here, we propose that these observations are due to the effect of salt concentration on themore » grain structure in SEO electrolytes.« less

Authors:
 [1];  [2];  [3];  [2];  [4];  [5];  [6];  [7];  [8]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  3. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  4. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research (JCESR)
  5. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research (JCESR); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research (JCESR); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Environmental Energy Technologies Division
  8. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research (JCESR); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Environmental Energy Technologies Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1474926
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 49; Journal Issue: 5; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Chintapalli, Mahati, Le, Thao N. P., Venkatesan, Naveen R., Mackay, Nikolaus G., Rojas, Adriana A., Thelen, Jacob L., Chen, X. Chelsea, Devaux, Didier, and Balsara, Nitash P. Structure and Ionic Conductivity of Polystyrene-block-poly(ethylene oxide) Electrolytes in the High Salt Concentration Limit. United States: N. p., 2016. Web. doi:10.1021/acs.macromol.5b02620.
Chintapalli, Mahati, Le, Thao N. P., Venkatesan, Naveen R., Mackay, Nikolaus G., Rojas, Adriana A., Thelen, Jacob L., Chen, X. Chelsea, Devaux, Didier, & Balsara, Nitash P. Structure and Ionic Conductivity of Polystyrene-block-poly(ethylene oxide) Electrolytes in the High Salt Concentration Limit. United States. doi:10.1021/acs.macromol.5b02620.
Chintapalli, Mahati, Le, Thao N. P., Venkatesan, Naveen R., Mackay, Nikolaus G., Rojas, Adriana A., Thelen, Jacob L., Chen, X. Chelsea, Devaux, Didier, and Balsara, Nitash P. Fri . "Structure and Ionic Conductivity of Polystyrene-block-poly(ethylene oxide) Electrolytes in the High Salt Concentration Limit". United States. doi:10.1021/acs.macromol.5b02620. https://www.osti.gov/servlets/purl/1474926.
@article{osti_1474926,
title = {Structure and Ionic Conductivity of Polystyrene-block-poly(ethylene oxide) Electrolytes in the High Salt Concentration Limit},
author = {Chintapalli, Mahati and Le, Thao N. P. and Venkatesan, Naveen R. and Mackay, Nikolaus G. and Rojas, Adriana A. and Thelen, Jacob L. and Chen, X. Chelsea and Devaux, Didier and Balsara, Nitash P.},
abstractNote = {We explore the relationship between the morphology and ionic conductivity of block copolymer electrolytes over a wide range of salt concentrations for the system polystyrene-block-poly(ethylene oxide) (PS-b-PEO, SEO) mixed with lithium bis-(trifluoromethanesulfonyl)imide salt (LiTFSI). Two SEO polymers were studied, SEO(16-16) and SEO(4.9-5.5), over the salt concentration range r = 0.03-0.55. The numbers x and y in SEO(x-y) are the molecular weights of the blocks in kg mol-1, and the r value is the molar ratio of salt to ethylene oxide moieties. Small-angle X-ray scattering was used to characterize morphology and grain size at 120 °C, differential scanning calorimetry was used to study the crystallinity and the glass transition temperature of the PEO-rich microphase, and ac impedance spectroscopy was used to measure ionic conductivity as a function of temperature. The most surprising observation of our study is that ionic conductivity in the concentration regime 0.11 ≤ r ≤ 0.21 increases in SEO electrolytes but decreases in PEO electrolytes. The maximum in ionic conductivity with salt concentration occurs at about twice the salt concentration in SEO (r = 0.21) as in PEO (r = 0.11). Here, we propose that these observations are due to the effect of salt concentration on the grain structure in SEO electrolytes.},
doi = {10.1021/acs.macromol.5b02620},
journal = {Macromolecules},
issn = {0024-9297},
number = 5,
volume = 49,
place = {United States},
year = {2016},
month = {2}
}

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