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Investigating the effect of supramolecular gel phase crystallization on gel nucleation.

Dawn, Arnab and Mirzamani, Marzieh and Jones, Christopher D. and Yufit, Dmitry S. and Qian, Shuo and Steed, Jonathan W. and Kumari, Harshita (2018) 'Investigating the effect of supramolecular gel phase crystallization on gel nucleation.', Soft matter., 14 (46). pp. 9489-9497.


Supramolecular gel phase crystallization offers a new strategy for drug polymorph screening and discovery. In this method, the crystallization outcome depends on the interaction between solute and gel fibre. While supramolecular gels have shown success in producing new polymorphs and crystals with novel morphologies, role of the gel and nature of gel–solute interaction remains largely unexplored. The present study aims to provide a comprehensive picture of the structural evolution of a supramolecular gel produced from a bis(urea) based gelator (G) in the presence of a polymorphic drug carbamazepine (CBZ). The structural aspects of the gel have been assessed by single crystal X-ray analysis, X-ray powder diffraction (XRPD) and solid state NMR spectroscopy. Small Angle Neutron Scattering (SANS) has been used to follow the changes in gel structure in the presence of CBZ. Visual evidence from morphological study and structural evolution observed at a macroscopic level from rheological measurements, shows good agreement with the SANS results. The concentration of the gelator and the relative proportion of G to CBZ were found to be crucial factors in determining the competitive nucleation events involving gelation and crystallization. At a critical G to CBZ ratio the effect of CBZ on gel structure was maximum and fiber bundling in the gel was found to be critically affected. This study offers important information about how the interplay of gelator assembly and gel–solute interactions can fine-tune the nucleation events in a supramolecular gel phase crystallization.

Item Type:Article
Full text:(AM) Accepted Manuscript
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Date accepted:06 November 2018
Date deposited:16 November 2018
Date of first online publication:08 November 2018
Date first made open access:06 November 2019

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