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Photo-selective delivery of model therapeutics from hydrogels.

ABSTRACT: Hydrogels are commonly used in biomedical applications to sequester and release therapeutics. Covalently tethering therapeutic agents to a hydrogel through a degradable linkage allows their controlled release, but temporally separating the release of multiple therapeutics from a single hydrogel remains a major challenge. In this report, we use of a series of photodegradable ortho-nitrobenzyl (o-NB) groups with varying structures to link model therapeutic agents (fluorescein, rhodamine and aminomethylcoumarin acetate) to poly(ethylene glycol) macromers. We polymerized the macromers into hydrogel networks via redox polymerization and quantified the apparent rate constants of degradation (kapp) of each of the photoreleasable compounds. By exploiting differences in reactivity of the different o-NB groups, we are able to create complex, multi-stage release profiles. We demonstrate the ability to switch between concurrent and biased release of model therapeutics simply by switching wavelengths. We also demonstrate a complex four-stage release profile in which the release of three separate model therapeutics is controlled by varying wavelength, intensity and exposure time. This is the first report of photo-selective release of therapeutics from a hydrogel, allowing user-dictated real-time spatial and temporal control over multiple chemical signals in a cell microenvironment in 2D and 3D.

SUBMITTER: Griffin DR

PROVIDER: S-EPMC4180678 | biostudies-literature | 2012 Nov

REPOSITORIES: biostudies-literature

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Photo-selective delivery of model therapeutics from hydrogels.

Griffin Donald R DR Kasko Andrea M AM

ACS macro letters 20121101 11

Hydrogels are commonly used in biomedical applications to sequester and release therapeutics. Covalently tethering therapeutic agents to a hydrogel through a degradable linkage allows their controlled release, but temporally separating the release of multiple therapeutics from a single hydrogel remains a major challenge. In this report, we use of a series of photodegradable <i>ortho</i>-nitrobenzyl (<i>o</i>-NB) groups with varying structures to link model therapeutic agents (fluorescein, rhodam ...[more]

PMID: 25285242

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Project description:Embedding nanomaterials into polymer hydrogels enables the design of functional materials with tailored chemical, mechanical, and optical properties. Nanocapsules that protect interior cargo and disperse readily through a polymeric matrix have drawn particular interest for their ability to integrate chemically incompatible systems and to further expand the parameter space for polymer nanocomposite hydrogels. The properties of polymer nanocomposite hydrogels depend on the material composition and processing route, which were explored systematically in this work. The gelation kinetics of network-forming polymer solutions with and without silica-coated nanocapsules bearing polyethylene glycol (PEG) surface ligands were investigated using in situ dynamic rheology measurements. Network-forming polymers comprised either 4-arm or 8-arm star PEG with terminal anthracene groups, which dimerize upon irradiation with ultraviolet (UV) light. The PEG-anthracene solutions exhibited rapid gel formation upon UV exposure (365 nm); gel formation was observed as a crossover from liquid-like to solid-like behavior during in situ small-amplitude oscillatory shear rheology. This crossover time was non-monotonic with polymer concentration. Far below the overlap concentration (c/c* ≪ 1), spatially separated PEG-anthracene molecules were subject to forming intramolecular loops over intermolecular cross-links, thereby slowing the gelation process. Near the polymer overlap concentration (c/c* ∼ 1), rapid gelation was attributed to the ideal proximity of anthracene end groups from neighboring polymer molecules. Above the overlap concentration (c/c* > 1), increased solution viscosities hindered molecular diffusion, thereby reducing the frequency of dimerization reactions. Adding nanocapsules to PEG-anthracene solutions resulted in faster gelation than nanocapsule-free PEG-anthracene solutions with equivalent effective polymer concentrations. The final elastic modulus of nanocomposite hydrogels increased with nanocapsule volume fraction, signifying synergistic mechanical reinforcement by nanocapsules despite not being cross-linked into the polymer network. Overall, these findings quantify the impact of nanocapsule addition on the gelation kinetics and mechanical properties of polymer nanocomposite hydrogels, which are promising materials for applications in optoelectronics, biotechnology, and additive manufacturing.

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Photo-selective delivery of model therapeutics from hydrogels.

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Photo-selective delivery of model therapeutics from hydrogels.

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