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Systematic Computational and Experimental Investigation of Lithium-Ion Transport Mechanisms in Polyester-Based Polymer Electrolytes

Webb, Michael A. and Jung, Yukyung and Pesko, Danielle M. and Savoie, Brett M. and Yamamoto, Umi and Coates, Geoffrey W. and Balsara, Nitash P. and Wang, Zhen-Gang and Miller, Thomas F., III (2015) Systematic Computational and Experimental Investigation of Lithium-Ion Transport Mechanisms in Polyester-Based Polymer Electrolytes. ACS Central Science, 1 (4). pp. 198-205. ISSN 2374-7943. PMCID PMC4827473. http://resolver.caltech.edu/CaltechAUTHORS:20150724-073254175

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Abstract

Understanding the mechanisms of lithium-ion transport in polymers is crucial for the design of polymer electrolytes. We combine modular synthesis, electrochemical characterization, and molecular simulation to investigate lithium-ion transport in a new family of polyester-based polymers and in poly(ethylene oxide) (PEO). Theoretical predictions of glass-transition temperatures and ionic conductivities in the polymers agree well with experimental measurements. Interestingly, both the experiments and simulations indicate that the ionic conductivity of PEO, relative to the polyesters, is far higher than would be expected from its relative glass-transition temperature. The simulations reveal that diffusion of the lithium cations in the polyesters proceeds via a different mechanism than in PEO, and analysis of the distribution of available cation solvation sites in the various polymers provides a novel and intuitive way to explain the experimentally observed ionic conductivities. This work provides a platform for the evaluation and prediction of ionic conductivities in polymer electrolyte materials.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/acscentsci.5b00195DOIArticle
http://pubs.acs.org/doi/abs/10.1021/acscentsci.5b00195PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/acscentsci.5b00195PublisherSupporting Information
https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4827473/PubMed CentralArticle
ORCID:
AuthorORCID
Webb, Michael A.0000-0002-7420-4474
Pesko, Danielle M.0000-0002-4833-0119
Savoie, Brett M.0000-0002-7039-4039
Coates, Geoffrey W.0000-0002-3400-2552
Balsara, Nitash P.0000-0002-0106-5565
Wang, Zhen-Gang0000-0002-3361-6114
Miller, Thomas F., III0000-0002-1882-5380
Additional Information:© 2015 American Chemical Society. This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. Received: May 21, 2015; Published: July 10, 2015. This research was supported by the National Science Foundation under DMREF Award Number NSF-CHE-1335486. M.A.W. also acknowledges support from the Resnick Sustainability Institute.
Group:Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
NSFCHE-1335486
Resnick Sustainability InstituteUNSPECIFIED
PubMed Central ID:PMC4827473
Record Number:CaltechAUTHORS:20150724-073254175
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20150724-073254175
Official Citation:Systematic Computational and Experimental Investigation of Lithium-Ion Transport Mechanisms in Polyester-Based Polymer Electrolytes Michael A. Webb, Yukyung Jung, Danielle M. Pesko, Brett M. Savoie, Umi Yamamoto, Geoffrey W. Coates, Nitash P. Balsara, Zhen-Gang Wang, and Thomas F. Miller, III ACS Central Science 2015 1 (4), 198-205 DOI: 10.1021/acscentsci.5b00195
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:58999
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:24 Jul 2015 19:10
Last Modified:20 Mar 2019 19:38

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