Multidomain Hybrid Hydrogels: Spatially Resolved Photopatterned Synthetic Nanomaterials Combining Polymer and Low‐Molecular‐Weight Gelators

Cornwell, Daniel J.; Okesola, Babatunde O.; Smith, David K.

doi:10.1002/anie.201405098

Cited by 69 publications

(41 citation statements)

References 43 publications

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“…96 By photopatterning the overall material using a mask in the presence of GdL as pH activator, we were able to obtain multi-domain gel-phase materials, in which those regions exposed to UV irradiation contained the photoactivated polymer gel along with the pH-activated DBS-CO 2 H supramolecular gel, while those areas covered by the mask only contained the supramolecular gel ( Fig. 96 By photopatterning the overall material using a mask in the presence of GdL as pH activator, we were able to obtain multi-domain gel-phase materials, in which those regions exposed to UV irradiation contained the photoactivated polymer gel along with the pH-activated DBS-CO 2 H supramolecular gel, while those areas covered by the mask only contained the supramolecular gel ( Fig.…”

Section: Polymers With Embedded Dbs Network For Enhanced Performancementioning

confidence: 99%

1,3:2,4-Dibenzylidene-d-sorbitol (DBS) and its derivatives – efficient, versatile and industrially-relevant low-molecular-weight gelators with over 100 years of history and a bright future

et al. 2015

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Dibenzylidene-D-sorbitol (DBS) has been a well-known low-molecular-weight gelator of organic solvents for over 100 years. As such, it constitutes a very early example of a supramolecular gel--a research field which has recently developed into one of intense interest. The ability of DBS to self-assemble into sample-spanning networks in numerous solvents is predicated upon its 'butterfly-like' structure, whereby the benzylidene groups constitute the 'wings' and the sorbitol backbone the 'body'--the two parts representing the molecular recognition motifs underpinning its gelation mechanism, with the nature of solvent playing a key role in controlling the precise assembly mode. This gelator has found widespread applications in areas as diverse as personal care products and polymer nucleation/clarification, and has considerable potential in applications such as dental composites, energy technology and liquid crystalline materials. Some derivatives of DBS have also been reported which offer the potential to expand the scope and range of applications of this family of gelators and endow the nansocale network with additional functionality. This review aims to explain current trends in DBS research, and provide insight into how by combining a long history of application, with modern methods of derivatisation and analysis, the future for this family of gelators is bright, with an increasing number of high-tech applications, from environmental remediation to tissue engineering, being within reach.

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Section: Polymers With Embedded Dbs Network For Enhanced Performancementioning

confidence: 99%

1,3:2,4-Dibenzylidene-d-sorbitol (DBS) and its derivatives – efficient, versatile and industrially-relevant low-molecular-weight gelators with over 100 years of history and a bright future

et al. 2015

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“…One simple way to improve the mechanical properties of these systems is to combine them with covalent polymers. Covalent polymers are robust, and their non‐covalent functionalization with supramolecular polymers results in composite hydrogels with much improved mechanical and other physical properties …”

Section: Figurementioning

confidence: 99%

Composite of Peptide‐Supramolecular Polymer and Covalent Polymer Comprises a New Multifunctional, Bio‐Inspired Soft Material

Chakraborty

Ghosh

Schnaider

et al. 2019

Macromol. Rapid Commun.

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Engineering of extracellular matrix (ECM) mimics, with most of the necessary features of a natural ECM, is a crucial requirement for the design of biomaterials. The natural ECM encompasses a 3D network of intertwined protein nanofibers which contains complex biomolecules for communication between cells.[1] Short peptide-based 3D nanostructured supramolecular hydrogels are excellent candidates for ECM mimicry as they provide networks of fibers which resemble the ECM structure. [2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21] Modifications of certain oligopeptide termini with bio-active ligands, aimed to introduce bio-active components into the system, have also been reported. [22][23][24][25] The tripeptide sequence Arg-Gly-Asp (RGD), which was first recognized in fibronectin as an independent cell attachment site, is the most commonly used bio-active ligand. [26] This tri-peptide sequence is recognized by the α v β 3 and α 5 β 1 integrins located in cell membranes, thus facilitating the coupling of the ECM with the cytoskeleton. [27] Owing to these attributes, the RGD ligand has been introduced into supramolecular or polymeric substrates to facilitate cell attachment. [28][29][30][31] Fmoc-RGD [Fmoc = N-(fluorenyl-9-methoxycarbonyl)] is one of the simplest RGD derivatives capable of forming hydrogels with an inter-connected fibrous network. [15,27] Ulijn's group reported Fmoc-RGD based supramolecular hydrogels in neutral aqueous solution by appropriate mixing of two short peptidebased building blocks, Fmoc-FF (F = phenylalanine) and Fmoc-RGD and utilized them as scaffolds for cell culture. [15] They proposed that Fmoc-RGD alone was not able to form β-sheet fibrils, although in the composite gels of Fmoc-FF and Fmoc-RGD (10-30 wt% Fmoc-RGD), signatures of β-sheet structures were found. We later reported flanking of the RGD sequence by aromatic moieties, demonstrating the hydrogelation of RGD derivatives, including Fmoc-FRGD and Fmoc-RGDF. [32] Hamley and co-workers showed that the simple Fmoc-RGD moiety, without any modification or mixing with other hydrogelator peptides, could from nano-fibrous hydrogels. [27] Castelletto and co-workers prepared monoliths of Fmoc-RGD gels at a high peptide concentration of 10 wt% which showed excellent Bio-Inspired Soft MaterialsPeptide-based supramolecular hydrogels are utilized as functional materials in tissue engineering, axonal regeneration, and controlled drug delivery. The Arg-Gly-Asp (RGD) ligand based supramolecular gels have immense potential in this respect, as this tripeptide is known to promote cell adhesion. Although several RGD-based supramolecular hydrogels have been reported, most of them are devoid of adequate resilience and long-range stability for in vitro cell culture. In a quest to improve the mechanical properties of these tripeptide-based gels and their durability in cell culture media, the Fmoc-RGD hydrogelator is non-covalently functionalized with a biocompatible and biodegradable polymer, chitosan, resulting in a composite hydrog...

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“…22). 110 Dye diffusion was rapid through the soft supramolecular gel domain, but prevented by the rigid PEGDM network. This indicates that spatially resolved control over the diffusion and release of active ingredients should be possible.…”

Section: Spatially Resolved Gelsmentioning

confidence: 99%

From fundamental supramolecular chemistry to self-assembled nanomaterials and medicines and back again – how Sam inspired SAMul

Smith

2018

Chem. Commun.

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This feature article provides a personal insight into the research from my group over the past 10 years. In particular, the article explains how, inspired in 2005 by meeting my now-husband, Sam, who had cystic fibrosis, and who in 2011 went on to have a double lung transplant, I took an active decision to follow a more applied approach to some of our research, attempting to use fundamental supramolecular chemistry to address problems of medical interest. In particular, our strategy uses self-assembly to fabricate biologically-active nanosystems from simple low-molecular-weight building blocks. These systems can bind biological polyanions in highly competitive conditions, allowing us to approach applications in gene delivery and coagulation control. In the process, however, we have also developed new fundamental principles such as self-assembled multivalency (SAMul), temporary 'on-off' multivalency, and adaptive/shape-persistent multivalent binding. By targeting materials with applications in drug formulation and tissue engineering, we have discovered novel self-assembling low-molecular-weight hydrogelators based on the industrially-relevant dibenzylidenesorbitol framework and developed innovative approaches to spatially-resolved gels and functional multicomponent hybrid hydrogels. In this way, taking an application-led approach to research has also delivered significant academic value and conceptual advances. Furthermore, beginning to translate fundamental supramolecular chemistry into real-world applications, starts to demonstrate the power of this approach, and its potential to transform the world around us for the better.

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Multidomain Hybrid Hydrogels: Spatially Resolved Photopatterned Synthetic Nanomaterials Combining Polymer and Low‐Molecular‐Weight Gelators

Cited by 69 publications

References 43 publications

1,3:2,4-Dibenzylidene-d-sorbitol (DBS) and its derivatives – efficient, versatile and industrially-relevant low-molecular-weight gelators with over 100 years of history and a bright future

1,3:2,4-Dibenzylidene-d-sorbitol (DBS) and its derivatives – efficient, versatile and industrially-relevant low-molecular-weight gelators with over 100 years of history and a bright future

Composite of Peptide‐Supramolecular Polymer and Covalent Polymer Comprises a New Multifunctional, Bio‐Inspired Soft Material

From fundamental supramolecular chemistry to self-assembled nanomaterials and medicines and back again – how Sam inspired SAMul

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