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231224s2014 xx |||||o 00| ||eng c |
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|a 10.1021/la501641q
|2 doi
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|a eng
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|a Caragheorgheopol, Agneta
|e verfasserin
|4 aut
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|a Using EPR spectroscopy as a unique probe of molecular-scale reorganization and solvation in self-assembled gel-phase materials
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|c 2014
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|a Text
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|a ƒaComputermedien
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|a ƒa Online-Ressource
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|a Date Completed 11.05.2015
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|a Date Revised 05.08.2014
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a We describe the synthesis of spin-labeled bis-ureas which coassemble with bis-urea gelators and report on self-assembly as detected using electron paramagnetic resonance spectroscopy (EPR). Specifically, EPR detects the gel-sol transition and allows us to quantify how much spin-label is immobilized within the gel fibers and how much is present in mobile solvent pools-as controlled by temperature, gelator structure, and thermal history. EPR is also able to report on the initial self-assembly processes below the gelation threshold which are not macroscopically visible and appears to be more sensitive than NMR to intermediate-sized nongelating oligomeric species. By studying dilute solutions of gelator molecules and using either single or double spin-labels, EPR allows quantification of the initial steps of the hierarchical self-assembly process in terms of cooperativity and association constant. Finally, EPR enables us to estimate the degree of gel-fiber solvation by probing the distances between spin-labels. Comparison of experimental data against the predicted distances assuming the nanofibers are only composed of gelator molecules indicates a significant difference, which can be assigned to the presence of a quantifiable number of explicit solvent molecules. In summary, EPR provides unique data and yields powerful insight into how molecular-scale mobility and solvation impact on assembly of supramolecular gels
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|a Journal Article
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|a Edwards, William
|e verfasserin
|4 aut
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|a Hardy, John G
|e verfasserin
|4 aut
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|a Smith, David K
|e verfasserin
|4 aut
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|a Chechik, Victor
|e verfasserin
|4 aut
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|t Langmuir : the ACS journal of surfaces and colloids
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|u http://dx.doi.org/10.1021/la501641q
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