Polysaccharide-based functional hydrogels: luminescence characteristics
摘要
This study aims to design environmentally friendly and biocompatible, polysaccharide-based hydrogels with strong and stable emission properties for biomedical applications. Single-polymer hydrogels (SPHs) and hybrid hydrogels (HHs) (using two different polymers) were synthesized via a free radical polymerization mechanism, employing various polysaccharides—including chitosan, karaya gum, dextrin, and xanthan gum—through grafting and cross-linking techniques. The synthesized hydrogels exhibited both biocompatibility and cytocompatibility. Manifold enhancement in emission intensity (clusteroluminescence) was observed in the grafted and cross-linked hydrogels compared to their native counterparts. Deconvolution of the emission spectrum revealed two primary emission centres, which are attributed to transitions involving π electrons and nonbonding electrons, respectively, interacting via through-space interactions (TSIs). The hydrogels exhibited long emission decay times indicative of delayed luminescence. The decay times of SPHs and HHs were in the range of 127.02–172.2 µs and 118–123 µs, respectively. Moreover, careful selection of polysaccharide components enabled the enhancement of the photoluminescence quantum yield, reaching up to 26.25% for SPHs. Fluorescence microscopy revealed the intracellular distribution of hydrogels with blue luminescence without any cellular stress, representing their suitability for bioimaging. Theoretical modelling confirmed the presence of strong TSIs in the synthesized hydrogels, evidenced by short heteroatom contacts below the sum of their van der Waals radii. The heterogeneous distribution of these interactions indicates heteroatom clustering, leading to the formation of multiple emission centres within the hydrogel network. The present study highlights the findings on the suitability of the synthesized hydrogels as environmentally friendly alternatives for advanced luminescent systems.