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Issue 39, 2015
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Using solution state NMR spectroscopy to probe NMR invisible gelators

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Abstract

Supramolecular hydrogels are formed via the self-assembly of gelator molecules upon application of a suitable trigger. The exact nature of this self-assembly process has been widely investigated as a practical understanding is vital for the informed design of these materials. Solution-state NMR spectroscopy is an excellent non-invasive tool to follow the self-assembly of supramolecular hydrogels. However, in most cases the self-assembled aggregates are silent by conventional 1H NMR spectroscopy due to the low mobility of the constituent molecules, limiting NMR spectroscopy to following only the initial assembly step(s). Here, we present a new solution-state NMR spectroscopic method which allows the entire self-assembly process of a dipeptide gelator to be followed. This gelator forms transparent hydrogels by a multi-stage assembly process when the pH of an initially alkaline solution is lowered via the hydrolysis of glucono-δ-lactone (GdL). Changes in the charge, hydrophobicity and relative arrangement of the supramolecular aggregates can be followed throughout the assembly process by measuring the residual quadrupolar couplings (RQCs) of various molecular probes (here, 14NH4+ and isopropanol-d8), along with the NMR relaxation rates of 23Na+. The initially-formed aggregates comprise negatively charged fibrils which gradually lose their charge and become increasingly hydrophobic as the pH falls, eventually resulting in a macroscopic contraction of the hydrogel. We also demonstrate that the in situ measurement of pH by NMR spectroscopy is both convenient and accurate, representing a useful tool for the characterisation of self-assembly processes by NMR.

Graphical abstract: Using solution state NMR spectroscopy to probe NMR invisible gelators

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Publication details

The article was received on 16 Jul 2015, accepted on 21 Aug 2015 and first published on 21 Aug 2015


Article type: Paper
DOI: 10.1039/C5SM01760B
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Citation: Soft Matter, 2015,11, 7739-7747
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    Using solution state NMR spectroscopy to probe NMR invisible gelators

    M. Wallace, J. A. Iggo and D. J. Adams, Soft Matter, 2015, 11, 7739
    DOI: 10.1039/C5SM01760B

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