DOTAGEL: a hydrogen and amide bonded, gelatin based, tunable, antibacterial, and high strength adhesive synthesized in an unoxidized environment

Abstract

The development of bioadhesives that concurrently exhibit high adhesion strength, biocompatibility, and tunable properties and involve simple fabrication processes continues to be a significant challenge. In this study, a novel bioadhesive named DOTAGEL is synthesized by crosslinking gelatin (GA), dopamine (DA), and tannic acid (TA) in an unoxidized environment due to the advantage of controlling the degree of protonation in GA and TA, as well as controlling the degree of intermolecular amide and hydrogen bonding in the acidic medium. DOTAGEL (DA + TA + GA) shows superior adhesion strengths of 104.6 ± 46 kPa on dry skin and 35.6 ± 4.5 kPa on wet skin, up to 13 attachment–detachment cycles, retains adhesion strength under water for up to 10 days and is capable of joining two cut parts of internal organs of mice. Moreover, DOTAGEL shows strong antibacterial properties, self-healing, and biocompatibility since it contains TA, a natural and antibacterial cross-linker with abundant hydroxyl groups and the capability of forming non-covalent bonds in an unoxidized environment, and dopamine hydrochloride, a mussel inspired biomaterial containing both the amine and catechol groups for amide bonding and hydrogen bonding with TA and GA. The cross-linking among 20% (w/v) GA, 0.2% (w/v) DA, and 20% (w/v) TA is done by the centrifugation process at room temperature. Two different acids, hydrochloric acid and acetic acid, were used for tuning the pH of the medium, which led to two different samples named DOTAGEL/AA and DOTAGEL/HCL. The degree of cross-linking and mechanical and biochemical properties, like adhesion strength, degradation rate, antibacterial properties, stickiness, etc., are tuned by adjusting the pH of the medium. DOTAGEL/HCL showed 6.5 times faster degradation in 10 days, a faster release rate in the antibacterial study, 2 times adhesion strength in a dry medium, and more stickiness. The novelty lies not only in increased adhesion strength but also in the single-step fabrication process of the adhesive in the acidic medium. This research proposes the formation of a tunable antibacterial adhesive that is capable of working on wet surfaces within the body and that has the potential to become a successful tissue adhesive with a wide range of possibilities in controlled drug delivery at wound sites and other biomedical applications.