Double diffusion for the programmable spatiotemporal patterning of multi-domain supramolecular gels.

Autor: Cooke HS; Department of Chemistry, University of York Heslington York YO10 5DD UK David.smith@york.ac.uk., Schlichter L; Department of Chemistry, University of York Heslington York YO10 5DD UK David.smith@york.ac.uk., Piras CC; Department of Chemistry, University of York Heslington York YO10 5DD UK David.smith@york.ac.uk., Smith DK; Department of Chemistry, University of York Heslington York YO10 5DD UK David.smith@york.ac.uk.
Jazyk: angličtina
Zdroj: Chemical science [Chem Sci] 2021 Aug 18; Vol. 12 (36), pp. 12156-12164. Date of Electronic Publication: 2021 Aug 18 (Print Publication: 2021).
DOI: 10.1039/d1sc03155d
Abstrakt: To achieve spatial resolution of a multi-component gel, a double diffusion approach is used which enables the precise programming of self-assembled patterned domains with well-defined shapes and sizes. The low-molecular-weight gelators (LMWGs) used in this study are pH-responsive DBS-CO 2 H and thermally-responsive DBS-CONHNH 2 (both based on 1,3:2,4-dibenzylidenesorbitol, DBS). A DBS-CONHNH 2 gel was initially assembled in a tray, and then loaded at carefully-selected positions with either basified DBS-CO 2 H ( i.e. DBS-carboxylate) or an acid. These soluble components subsequently diffuse through the pre-formed gel matrix, and in the domains when/where they mix, protonation of the DBS-carboxylate induces self-assembly of the DBS-CO 2 H network, leading to a patterned gel-in-gel object with well-defined shape and dimensions. Using a strong acid achieves fast gelation kinetics, creating smaller, better-defined macroscale objects but with less nanoscale order. Using a weak acid source with slow kinetics, gives slightly larger objects, but on the nanoscale the DBS-CO 2 H network formation is better controlled, giving more homogeneous nanoscale structures and stiffer objects. The patterned objects can be further reinforced by the presence of agarose polymer gelator. The shape of the patterning is programmed by both the shape of the central reservoir and the starting geometry in which the reservoirs are organised, with the balance between factors depending on assembly kinetics, as dictated by the choice of acid. This simple methodology therefore enables programming of patterned gels with spatiotemporal control and emergent patterning characteristics.
Competing Interests: There are no conflicts to declare.
(This journal is © The Royal Society of Chemistry.)
Databáze: MEDLINE
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