Effect of molar ratio and concentration on the rheological properties of two-component supramolecular hydrogels: tuning of the morphological and drug releasing behaviour

Abstract

Self-assembled supramolecular hydrogels offer great potential as biomaterials and drug delivery systems. Specifically, peptide-based multicomponent hydrogels are promising materials due to their advantage that their mechanical and physical properties can be tuned to enhance their functionalities and broaden their applications. Herein, we report two-component assembly and formation of hydrogels containing inexpensive complementary anionic, BUVV-OH (A), and cationic, KFFC₁₂ (B), peptide amphiphiles. Individually, neither of these components formed a hydrogel, while mixtures with compositions 1 : 1, 1 : 2, and 2 : 1 (molar ratio) as A : B show hydrogel formation (Milli-Q water, at pH = 6.79). These hydrogels displayed a good shear-thinning behaviour with different mechanical stabilities and nano-fibrous network structures. The 1 : 1 hydrogel shows good cell viability for human embryonic kidney (HEK-293) cells and CHO cells indicating its non-cytotoxicity. The biocompatible, thixotropic 1 : 1 hydrogel with a nanofiber network structure shows the highest mechanical strength with a storage modulus of 3.4 × 10³ Pa. The hydrogel is able to encapsulate drugs including antibiotics amoxicillin and rifampicin, and anticancer drug doxorubicin, and it exhibits sustainable release of 76%, 70%, and 81% respectively in vitro after 3 days. The other two mixtures (composition 1 : 2 and 2 : 1) are unable to form a hydrogel when they are loaded with these drugs. Interestingly, it is noticed that with an increase in concentration, the mechanical strength of a 1 : 1 hydrogel is significantly enhanced, showing potential that may act as a scaffold for tissue engineering. The two-component gel offers tunable mechanical properties, thixotropy, injectability, and biocompatibility and has great potential as a scaffold for sustained drug release and tissue engineering.