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1D and 2D NMR Spectroscopy of Bonding Interactions within Stable and Phase-Separating Organic Electrolyte-Cellulose Solutions

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Title: 1D and 2D NMR Spectroscopy of Bonding Interactions within Stable and Phase-Separating Organic Electrolyte-Cellulose Solutions
Authors: Clough, MT
Fares, C
Rinaldi, R
Item Type: Journal Article
Abstract: Organic electrolyte solutions (i.e. mixtures containing an ionic liquid and a polar, molecular co-solvent) are highly versatile solvents for cellulose. However, the underlying solvent–solvent and solvent–solute interactions are not yet fully understood. Herein, mixtures of the ionic liquid 1-ethyl-3-methylimidazolium acetate, the co-solvent 1,3-dimethyl-2-imidazolidinone, and cellulose are investigated using 1D and 2D NMR spectroscopy. The use of a triply-13C-labelled ionic liquid enhances the signal-to-noise ratio for 13C NMR spectroscopy, enabling changes in bonding interactions to be accurately pinpointed. Current observations reveal an additional degree of complexity regarding the distinct roles of cation, anion, and co-solvent toward maintaining cellulose solubility and phase stability. Unexpectedly, the interactions between the dialkylimidazolium ring C2−H substituent and cellulose become more pronounced at high temperatures, counteracted by a net weakening of acetate–cellulose interactions. Moreover, for mixtures that exhibit critical solution behavior, phase separation is accompanied by the apparent recombination of cation–anion pairs.
Issue Date: 17-Aug-2017
Date of Acceptance: 24-Jul-2017
URI: http://hdl.handle.net/10044/1/57152
DOI: https://dx.doi.org/10.1002/cssc.201701042
ISSN: 0003-4592
Publisher: Wiley-VCH Verlag
Start Page: 3452
End Page: 3458
Journal / Book Title: ChemSusChem
Volume: 10
Issue: 17
Copyright Statement: This is the peer reviewed version of the following article: M. T. Clough, C. Farès, R. Rinaldi, ChemSusChem 2017, 10, 3452., which has been published in final form at https://dx.doi.org/10.1002/cssc.201701042.  This article may be used for non-commercial purposes in accordance With Wiley Terms and Conditions for self-archiving.
Keywords: Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY
Chemistry
Science & Technology - Other Topics
cellulose
hydrogen bonding
ionic liquids
NMR
organic electrolytes
IONIC LIQUIDS
I-BETA
DISSOLUTION
COSOLVENT
SOLVENT
SIMULATIONS
TRANSITION
MECHANISM
ACETATE
SYSTEMS
Cellulose
Electrolytes
Imidazoles
Ionic Liquids
Magnetic Resonance Spectroscopy
Solutions
0399 Other Chemical Sciences
General Chemistry
Organic Chemistry
Publication Status: Published
Appears in Collections:Chemical Engineering
Faculty of Engineering