X-Ray absorption spectroscopy of LiBF4 in propylene carbonate: a model lithium ion battery electrolyte

Jacob W. Smith; Royce K. Lam; Alex T. Sheardy; Orion Shih; Anthony M. Rizzuto; Oleg Borodin; Stephen J. Harris; David Prendergast; Richard J. Saykally

doi:10.1039/C4CP03240C

You do not have JavaScript enabled. Please enable JavaScript to access the full features of the site or access our non-JavaScript page.

X-Ray absorption spectroscopy of LiBF₄ in propylene carbonate: a model lithium ion battery electrolyte†

Jacob W. Smith,^ab Royce K. Lam,^ab Alex T. Sheardy,^ab Orion Shih,^a Anthony M. Rizzuto,^a Oleg Borodin,^c Stephen J. Harris,^d David Prendergast^e and Richard J. Saykally*^ab

Author affiliations

* Corresponding authors

^a Department of Chemistry, University of California, Berkeley, California 94720, USA
E-mail: saykally@berkeley.edu

^b Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

^c Electrochemistry Branch, U.S. Army Research Laboratory, Adelphi, Maryland 20783, USA

^d Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

^e Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

Abstract

Since their introduction into the commercial marketplace in 1991, lithium ion batteries have become increasingly ubiquitous in portable technology. Nevertheless, improvements to existing battery technology are necessary to expand their utility for larger-scale applications, such as electric vehicles. Advances may be realized from improvements to the liquid electrolyte; however, current understanding of the liquid structure and properties remains incomplete. X-ray absorption spectroscopy of solutions of LiBF₄ in propylene carbonate (PC), interpreted using first-principles electronic structure calculations within the eXcited electron and Core Hole (XCH) approximation, yields new insight into the solvation structure of the Li⁺ ion in this model electrolyte. By generating linear combinations of the computed spectra of Li⁺-associating and free PC molecules and comparing to the experimental spectrum, we find a Li⁺–solvent interaction number of 4.5. This result suggests that computational models of lithium ion battery electrolytes should move beyond tetrahedral coordination structures.

Download options Please wait...

Supplementary files

Supplementary information PDF (111K)

Article information

DOI: https://doi.org/10.1039/C4CP03240C
Article type: Paper
Submitted: 22 Jul 2014
Accepted: 19 Aug 2014
First published: 20 Aug 2014
This article is Open Access

Download Citation

Phys. Chem. Chem. Phys., 2014,16, 23568-23575

Author version available

Download author version (PDF)

Permissions

Request permissions

X-Ray absorption spectroscopy of LiBF₄ in propylene carbonate: a model lithium ion battery electrolyte

J. W. Smith, R. K. Lam, A. T. Sheardy, O. Shih, A. M. Rizzuto, O. Borodin, S. J. Harris, D. Prendergast and R. J. Saykally, Phys. Chem. Chem. Phys., 2014, 16, 23568 DOI: 10.1039/C4CP03240C

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. You can use material from this article in other publications, without requesting further permission from the RSC, provided that the correct acknowledgement is given and it is not used for commercial purposes.

To request permission to reproduce material from this article in a commercial publication, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party commercial publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Social activity

Fetching data from CrossRef.
This may take some time to load.

Physical Chemistry Chemical Physics