PMID- 35170966 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20220716 IS - 1948-7185 (Electronic) IS - 1948-7185 (Linking) VI - 13 IP - 7 DP - 2022 Feb 24 TI - Insights into the Transport and Thermodynamic Properties of a Bis(fluorosulfonyl)imide-Based Ionic Liquid Electrolyte for Battery Applications. PG - 1734-1741 LID - 10.1021/acs.jpclett.1c04246 [doi] AB - Ionic liquid electrolytes (ILEs) have become popular in various advanced Li-ion battery chemistries because of their high electrochemical and thermal stability and low volatility. However, because of their relatively high viscosity and poor Li(+) diffusion, it is thought large concentration gradients form, reducing their rate capability. Herein, we utilize operando Raman microspectroscopy to visualize ILE concentration gradients for the first time. Specifically, using lithium bis(fluorosulfonyl)imide (LiFSI) in N-propyl-N-methylpyrrolidinium FSI, its "apparent" diffusion coefficient, lithium transference number, thermodynamic factor, ionic conductivity, and resistance of charge transfer against lithium metal were isolated. Furthermore, the analysis of these concentration gradients led to insights into the bulk structure of ILEs, which we propose are composed of large, ordered aggregates. FAU - Fawdon, Jack AU - Fawdon J AD - Department of Materials, University of Oxford, Parks Road, Oxford OX1 3PH, U.K. FAU - Rees, Gregory J AU - Rees GJ AD - Department of Materials, University of Oxford, Parks Road, Oxford OX1 3PH, U.K. AD - The Faraday Institution Quad One, Harwell Science and Innovation Campus, Didcot OX11 0RA, U.K. FAU - La Mantia, Fabio AU - La Mantia F AUID- ORCID: 0000-0001-7743-4198 AD - Universtat Bremen, Energiespeicher-und Energiewandlersysteme, Bibliotechkstrasse 1, Bremen 28359, Germany. FAU - Pasta, Mauro AU - Pasta M AUID- ORCID: 0000-0002-2613-4555 AD - Department of Materials, University of Oxford, Parks Road, Oxford OX1 3PH, U.K. AD - The Faraday Institution Quad One, Harwell Science and Innovation Campus, Didcot OX11 0RA, U.K. LA - eng PT - Journal Article DEP - 20220216 PL - United States TA - J Phys Chem Lett JT - The journal of physical chemistry letters JID - 101526034 SB - IM PMC - PMC9084600 COIS- The authors declare no competing financial interest. EDAT- 2022/02/17 06:00 MHDA- 2022/02/17 06:01 PMCR- 2022/05/09 CRDT- 2022/02/16 12:14 PHST- 2022/02/17 06:00 [pubmed] PHST- 2022/02/17 06:01 [medline] PHST- 2022/02/16 12:14 [entrez] PHST- 2022/05/09 00:00 [pmc-release] AID - 10.1021/acs.jpclett.1c04246 [doi] PST - ppublish SO - J Phys Chem Lett. 2022 Feb 24;13(7):1734-1741. doi: 10.1021/acs.jpclett.1c04246. Epub 2022 Feb 16.