Researchers investigated the effect of various (bio)polymeric crosslinkers on the self-assembly process of this reaction-coupled hydrazide-aldehyde gelator into hydrogel materials as a model system. They selected duplex DNA, which acted as a stiff, negatively charged rigid rod below its persistence length ideal for the construction of (nano)materials,[38–40] and compared it against a soft, neutral poly(ethylene glycol) (PEG) polymer of comparable size. Aldehyde moieties were specifically incorporated at the terminal ends of the (bio)polymers to introduce them during the self-assembly of the reaction-coupled network composed another set of (bio)polymers. The researchers also examined the effect of these two crosslinkers on the gelation of the reaction-coupled monomers into hydrogels over several length scales and compared their resultant materials properties.

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In recent years, we have developed a low molecular weight hydrogelator system that is formed in situ under ambient conditions through catalysed hydrazone formation between two individually non-gelating components. In this contribution, we describe a molecular toolbox based on this system which allows us to (1) investigate the limits of gel formation and fine-tuning of their bulk properties, (2) introduce multicolour fluorescent probes in an easy fashion to enable high-resolution imaging, and (3) chemically modify the supramolecular gel fibres through click and non-covalent chemistry, to expand the functionality of the resultant materials. In this paper we show preliminary applications of this toolbox, enabling covalent and non-covalent functionalisation of the gel network with proteins and multicolour imaging of hydrogel networks with embedded mammalian cells and their substructures. Overall, the results show that the toolbox allows for on demand gel network visualisation and functionalisation, enabling a wealth of applications in the areas of chemical biology and smart materials.@en