Injectable and self‐healing biobased composite hydrogels as future anticancer therapeutic biomaterials

Abstract

Self-healing composite hydrogels are prepared from sustainable biopolymers by a green chemistry approach and analyzed by physicochemical and mechanical characterization techniques for future injectable anticancer biomaterials. Watersoluble chitosan (WSC) was prepared by grafting polyethylene glycol (PEG), glutamic acid and gallic acid onto the chitosan chain by carbodiimide chemistry. This WSC showed fast gelation (t ≈ < 60 seconds) with benzaldehyde-terminated 4-arm-PEG as a crosslinker through an amine/aldehyde Schiff base reaction.The compression modulus of these gels can be controlled between 6 and 67 kPa, which was dependent on both the crosslinker content as well as the total solid content (T%). It showed injectability and complete self-healing ability at the lower solid content (T = 2%). The hydrogel nanocomposites (HNCs) were synthesized together with gold (Au) and silver (Ag) nanoparticles (NPs) and tested for cytotoxicity using fibroblast cells (WI-38) for 48 hours, which showed good biocompatibility. The in-vitro assay against cancer cells (U87MG) for 48 hours indicated that only the HNCs with incorporated AuNPs were effective agents for cancer cell apoptosis in contrast to pristine gel, pure NPs (Ag and AuNPs) and HCNs with AgNPs. Therefore, these HNCs could be effective chemotherapeutic materials for designing anticancer nanomedicines in the future.

Gallic acid: design of a pyrogallol-containing hydrogel and its biomedical applications

“…Moreover, van der Waals forces are also involved in the formation of the hydrogel network, but due to the low molecular weight of GA, the van der Waals forces in GA are comparatively weaker than those in other phenolic molecules. 63 Hydrophobic interactions are entropy-driven spontaneous interactions that cause nonpolar molecules in solution to exhibit self-aggregation properties. 64 Owing to the presence of hydrophobic aromatic groups, hydrophobic interactions also contribute to the formation of GA-containing hydrogel systems.…”

A Comprehensive Review of Cross-Linked Gels as Vehicles for Drug Delivery to Treat Central Nervous System Disorders

“…Gallic acid (GA) also known as 3,4,5-trihydroxybenzoic acid is tannin and is the major phenolic compound in plants, fruits such as grapes, berries, mango, areca nut, walnut, and green tea. GA has advanced anti-carcinogenic, anti-viral, antibacterial, antifungal, anti-inflammatory, and anti-malarial properties [ 138 , 139 ]. Additionally, GA possesses antioxidant activities equal to a well-established antioxidant vitamin C [ 140 ].…”

“…Xie et al suggest that it is a valuable approach to graft GA onto chitosan to reduce the intra- and intermolecular hydrogen bond networks and increase the antioxidant ability of CS [ 138 ]. Chemical or enzyme-modified GA-chitosan conjugate presented improved bioactivities such as antioxidant, antibacterial, anticancer, and inhibitory effects on digestive enzymes when compared to free GA or biopolymer [ 139 ].…”

Starch/Pectin as Emerging Renewable Materials for Fabrication of Sustainable Bioplastics for Food Packaging Applications

“…However, lm of pure starch has poor mechanical performance and the addition of secondary co-biopolymers is vital to improve the mechanical properties [11]. Addition of chitosan, a linear polysaccharide abundantly available after cellulose with non-toxicity, biodegradability and antibacterial properties can improve the mechanical factor of starch based lm [12,13]. The addition of plasticizer is important to overcome the brittleness of starch/chitosan blend lm such as sorbitol and glycerol [14].…”