Abstract
In this work, we report the design and fabrication of a dual-function integrated system to monitor, in real time, the release of previously loaded 2-methyl-1,4-naphthoquinone (MeNQ), also named vitamin K3. The newly developed system consists of poly(3,4-ethylenedioxythiophene) (PEDOT) nanoparticles, which were embedded into a poly-γ-glutamic acid (γ-PGA) biohydrogel during the gelling reaction between the biopolymer chains and the cross-linker, cystamine. After this, agglomerates of PEDOT nanoparticles homogeneously dispersed inside the biohydrogel were used as polymerization nuclei for the in situ anodic synthesis of poly(hydroxymethyl-3,4-ethylenedioxythiophene) in aqueous solution. After characterization of the resulting flexible electrode composites, their ability to load and release MeNQ was proven and monitored. Specifically, loaded MeNQ molecules, which organized in shells around PEDOT nanoparticles agglomerates when the drug was simply added to the initial gelling solution, were progressively released to a physiological medium. The latter process was successfully monitored using an electrode composite through differential pulse voltammetry. The fabrication of electroactive flexible biohydrogels for real-time release monitoring opens new opportunities for theranostic therapeutic approaches.
Highlights
Over the last decade, hydrophilic polymers organized in self-assembled and/or cross-linked hydrogels were widely studied considering a great variety of physical formats, including microparticles [1,2], nanoparticles [3,4], and films [5,6,7]
PEDOT NPs and MeNQ were loaded into a biocompatible γ-PGA hydrogel
An MeNQ release system able to monitor the concentration of the delivered drug was developed by incorporating conducting polymers (CPs) into a γ-PGA biohydrogel
Summary
Hydrophilic polymers organized in self-assembled and/or cross-linked hydrogels were widely studied considering a great variety of physical formats, including microparticles [1,2], nanoparticles [3,4], and films [5,6,7]. In contrast to self-assembled hydrogels, which are typically made of low-molecular-weight compounds interacting through non-covalent interactions (i.e., hydrogen bonding, van der Waals, charge transfer, dipole–dipole, π–π stacking, and coordination interactions), cross-linked hydrogels are based on covalent bonds. In the latter structures, non-covalent interactions play a less important role, mainly related to the packing of non-cross-linked segments. Physical interactions usually provide reversible gel-to-phase transitions in self-assembled hydrogels, which are sometimes undesired for biomedical applications, while cross-linked hydrogels remain stable despite environmental changes. As a result of the progress in chemical design and synthesis, hydrogels were used in many biomedical applications, for example, tissue engineering [8,9], regenerative medicine [6,9,10], cellular immobilization [11], biosensors [1,12,13], and drug release [3,4,7,14,15].
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