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Issue 11, 2021
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Spatial and temporal diffusion-control of dynamic multi-domain self-assembled gels

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Abstract

The dynamic assembly of a pH-responsive low-molecular-weight gelator (LMWG) within the pre-formed matrix of a second LMWG has been achieved via diffusion of an acid from a reservoir cut into the gel. Self-assembly of the acid-triggered LMWG as it converts from micellar aggregates at basic pH into gel nanofibers at lower pH values can be both spatially and temporally controlled. The pH-responsive LMWG has an impact on the stiffness of the pre-formed gel in the domains in which it assembles. When low acid concentrations are used, LMWG assembly is transient – after the initial proton diffusion phase, the pH rises and disassembly occurs as the system equilibrates. Re-application of additional acid as ‘fuel’ can then re-assemble the LMWG network. Using glucono-δ-lactone (which slowly hydrolyses to gluconic acid) instead of HCl gives slower, more spatially-restricted assembly, and creates longer-lasting pH gradients within the gel. The presence of an agarose polymer gel network improves the mechanical strength of the gels and appears to slightly enhance the rate of proton diffusion. More sophisticated reservoir shapes can be cut into these more mechanically robust gels, enabling the creation of diffusion waves with different geometries, and hence different patterns of LMWG activation. Multiple reservoirs can be used to create overlapping proton diffusion waves, hence achieving differentiated pH patterns in the gel. Using acid diffusion in this way within gels is an intriguing and powerful way of dynamic patterning. The ability to temporally-evolve spatially-resolved patterns using biocompatible weak acids, and the change in rheological performance of the triggered domains, suggest potential future applications of this strategy in tissue engineering.

Graphical abstract: Spatial and temporal diffusion-control of dynamic multi-domain self-assembled gels

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Supplementary files

Article information


Submitted
16 Dec 2020
Accepted
04 Feb 2021
First published
08 Feb 2021

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2021,12, 4162-4172
Article type
Edge Article

Spatial and temporal diffusion-control of dynamic multi-domain self-assembled gels

L. Schlichter, C. C. Piras and D. K. Smith, Chem. Sci., 2021, 12, 4162
DOI: 10.1039/D0SC06862D

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