Multi-component hybrid hydrogels – understanding the extent of orthogonal assembly and its impact on controlled release

Abstract

This paper reports self-assembled multi-component hybrid hydrogels including a range of nanoscale systems and characterizes the extent to which each component maintains its own unique functionality, demonstrating that multi-functionality can be achieved by simply mixing carefully-chosen constituents.

Commercially Relevant Orthogonal Multi‐Component Supramolecular Hydrogels for Programmed Cell Growth

“…To control heparin, we also added C 16 ‐DAPMA, previously reported by us as a self‐assembling multivalent (SAMul) heparin binder, into the gels. At concentrations of C 16 ‐DAPMA up to 1.2 m m , the DBS‐CONHNH 2 hydrogel remained stable, with a T gel of 83–86 °C, the IR reflecting an overlap of the spectra of the individual components (Figure S1), and minimal impact on the CD spectrum of DBS‐CONHNH 2 (Figure S2) suggesting that the self‐ assembled micelles do not adversely impact the self‐assembly of the gel nanofibres (in contrast to our previous studies with DBS‐COOH) . TEM demonstrated the independent existence of DBS‐CONHNH 2 nanofibres and C 16 ‐DAPMA micelles (Figure A).…”

“…At concentrations of C 16 -DAPMA up to 1.2 mm,t he DBS-CONHNH 2 hydrogel remained stable, with a T gel of 83-86 8C, the IR reflecting ano verlap of the spectra of the individual components ( Figure S1), and minimal impact on the CD spectrum of DBS-CONHNH 2 ( Figure S2) suggesting that the self-assembled micelles do not adversely impact the selfassembly of the gel nanofibres (in contrastt oo ur previous studies with DBS-COOH). [20] TEM demonstrated the independent existence of DBS-CONHNH 2 nanofibres and C 16 -DAPMA micelles ( Figure 4A). Rheologyi ndicated thatt he presenceo fm icelles had limited impact on gel stiffness, withG ' remaining similar,but the stabilityt owards strain reducedt o1%.…”

“…We previously reported multi‐component hydrogels based on a different gelator 1,3:2,4‐dibenzylidene‐ d ‐sorbitol‐ p,p′ ‐dicarboxylic acid (DBS‐COOH), but these were not stable above pH 5.5, and were unsuitable for tissue culture. For this study, we focussed attention on 1,3:2,4‐dibenzylidene‐ d ‐sorbitol‐ p‐p′ ‐diacylhydrazide (DBS‐CONHNH 2 , Figure ), which is stable from ca.…”

“…Self-sorting within gels that contain am ixture of components,t oy ield materials capable of orthogonal functionh as emerged as one of the key advantages of using LMWGs. [19] We previously reported multi-component hydrogels based on ad ifferent gelator 1,3:2,4-dibenzylidene-d-sorbitol-p,p'-di-carboxylic acid (DBS-COOH), [20] but these were not stable above pH 5.5, and were unsuitable for tissue culture. For this study,w ef ocussed attention on 1,3:2,4-dibenzylidene-d-sorbitol-p-p'-diacylhydrazide (DBS-CONHNH 2 ,F igure 1), which is stable from ca.…”

Sequential Assembly of Mutually Interactive Supramolecular Hydrogels and Fabrication of Multi‐Domain Materials

“…[20] Studies on heparin releasef rom DBS-COOH and DBS-CONHNH 2 gels individually have been reported previously by us. [9,21] We, therefore, appliedo ur already optimised method based on the use of Mallard Blue (MalB), [22] a high-affinity heparin binder,t oa nalyse heparin release from the gels by UV/Vis absorption spectroscopy.T he DBS-CONHNH 2 /DBS-COOH two-component gels loaded with heparin were prepared simplyb ya dding heparin (1 mm)t ot he LMWG mixture prior to gelation. This can be considered to be am ulti-component system.T he properties of these gels were fully studied by IR spectroscopy,m icroscopy,t hermals tability analysisa nd rheology.I na ll cases, gelation still occurred in the presence of heparin, although there was some evidencet hat the components are not all truly orthogonal (see Supporting Information for full details).…”