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Anion-driven, nanoscale polar-apolar structural organization is investigated in a solvate ionic liquid (SIL) setting by comparing sulfonate-based anions with long and short perfluorinated alkyl chains. Representative SILs are created from 1,2-bis(2-methoxyethoxy)ethane ("triglyme" or "G3"), lithium nonafluoro-1-butanesulfonate, and lithium trifluoromethanesulfonate. Molecular dynamics simulations, density functional theory computations, and vibrational spectroscopy provide insight into the overall liquid structure, cation-solvent interactions, and cation-anion association. Significant competition between G3 and anions for cation-binding sites characterizes the G3-LiCFSO mixtures. Only 50% of coordinating G3 molecules form tetradentate complexes with Li in [(G3)Li][CFSO]. Moreover, the SIL is characterized by extensive amounts of ion pairing. Based on these observations, [(G3)Li][CFSO] is classified as a "poor" SIL, similar to the analogous [(G3)Li][CFSO] system. Even though the comparable basicity of the CFSO and CFSO anions leads to similar SIL classifications, the hydrophobic fluorobutyl groups support extensive apolar domain formation. These apolar moieties permeate throughout [(G3)Li][CFSO] and persist even at relatively low dilution ratios of [(G3)Li][CFSO]. By way of comparison, the CF group is far too short to sustain polar-apolar segregation. This demonstrates how chemically modifying the anions to include hydrophobic groups can impart unique nanoscale organization to a SIL. Moreover, tuning these nano-segregated fluorinated domains could, in principle, control the presence of dimensionally ordered states in these mixtures without changing the coordination of the lithium ions.
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http://dx.doi.org/10.3390/molecules29092071 | DOI Listing |
Chemphyschem
December 2024
Universitat Rostock, Physikalische Chemie, Albert-Einstein-Straße 27, 18059, Rostock, GERMANY.
Glyme-based electrolyte solutions provide new concepts for developing suitable lithium-ion batteries. The so-called solvate ionic liquids (SILs) are promising electrolytes. They are most efficient in equimolar mixtures of lithium bis(trifluoromethanesulfonyl)imide ([Li][NTf2]) and glyme, wherein the [Li]+ cation is supposedly fully solvated by glyme molecules.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Department of Physics and Centre for Processable Electronics, Imperial College London, SW7 2AZ, London, United Kingdom.
Conjugated polymers (CPs) with polar side chains can conduct electronic and ionic charges simultaneously, making them promising for bioelectronics, electrocatalysis and energy storage. Recent work showed that adding alkyl spacers between CP backbones and polar side chains improved electronic charge carrier mobility, reduced swelling and enhanced stability, without compromising ion transport. However, how alkyl spacers impact polymer backbone conformation and, subsequently, electronic properties remain unclear.
View Article and Find Full Text PDFACS Macro Lett
December 2024
Department of Chemical Engineering, The University of California, Santa Barbara, Santa Barbara, California 93106, United States.
Ion-containing polymers are subject to a wide range of hydration conditions across electrochemical and water treatment applications. Significant work on dry polymer electrolytes for batteries and highly swollen membranes for water purification has informed our understanding of ion transport under extreme conditions. However, knowledge of intermediate conditions (i.
View Article and Find Full Text PDFACS Energy Lett
December 2024
Department of Materials, University of Oxford, Oxford OX1 3PH, United Kingdom.
The fluoride-ion battery (FIB) is a post-lithium anionic battery that utilizes the fluoride-ion shuttle, achieving high theoretical energy densities of up to 1393 Wh L without relying on critical minerals. However, developing liquid electrolytes for FIBs has proven arduous due to the low solubility of fluoride salts and the chemical reactivity of the fluoride ion. By introducing a chemically stable electrolyte based on 1,3-dimethylimidazolium [MMIm] bis(trifluoromethanesulfonyl)imide [TFSI] and tetramethylammonium fluoride (TMAF), we achieve an electrochemical stability window (ESW) of 4.
View Article and Find Full Text PDFACS Appl Polym Mater
December 2024
Institute for Frontier Materials (IFM), Deakin University, Burwood, Victoria 3125, Australia.
Poly(ethylene oxide)-(PEO-based solid polymer electrolytes (SPEs) are regarded as excellent candidates for solid-state lithium metal batteries (SSLMBs) due to their inherent safety advantages, processability, low cost, and excellent Li+ ion solvation. However, they suffer from limited oxidation stability (up to 4 V vs Li/Li). In this study, a crosslinked polymer-in-concentrated ionic liquid (PCIL) SPE consisting of PEO, -propyl--methylpyrrolidinium bis(fluorosulfonyl)imide (CmpyrFSI) ionic liquid (IL), and lithium bis(fluorosulfonyl)imide (LiFSI) salt is developed.
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