Benzenetrispeptides: a versatile building block to design supramolecular polymer bottlebrushes and hydrogels

Benzentrispeptides that can form 1-dimensional supramolecular polymer bottlebrushes (SPBs) in water were synthesised and investigated. Initially, the focus was on the correlation between the molecular motif and the shape of the obtained aggregates. Thus, the hydrogen-bonding peptide segment, the hydrophobic alkyl spacer, and the hydrophilic polymer were systematically varied to reveal the motifs limits at which different aggregate shapes, besides SPBs, are obtained. Moreover, the dynamic behaviours of the most promising BTP motifs were investigated, showing that the employed BTP systems are non-dynamic under normal conditions. However, a dynamic exchange of benzentrispeptide units between the fibrous aggregates could be triggered by external stimuli. Lastly, supramolecular hydrogels based on BTPs were prepared, which displayed a good stress responsiveness and self-healing behaviour in rheological characterisation, and good biocompatibility in cell-growth tests.