Chemical and Biomedical Engineering - Research Publications
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ItemSelf-Assembly of a Metal-Phenolic Sorbent for Broad-Spectrum Metal Sequestration(AMER CHEMICAL SOC, 2020-01-08)Metal contamination of water bodies from industrial effluents presents a global threat to the aquatic ecosystem. To address this challenge, metal sequestration via adsorption onto solid media has been explored extensively. However, existing sorbent systems typically involve energy-intensive syntheses and are applicable to a limited range of metals. Herein, a sorbent system derived from physically cross-linked polyphenolic networks using tannic acid and ZrIV ions has been explored for high-affinity, broad-spectrum metal sequestration. The network formation step (gelation) of the sorbent is complete within 3 min and requires no special apparatus. The key to this system design is the formation of a highly stable coordination network with an optimized metal–ligand ratio (1.2:1), affording access to a major fraction of the chelating sites in tannic acid for capturing diverse metal ions. This system is stable over a pH range of 1–9, thermally stable up to ∼200 °C, and exhibits a negative surface charge (at pH 5). The sorbent system effectively sequesters 28 metals in single- and multielement model wastes, with removal efficiencies exceeding 99%. Furthermore, it is demonstrated that this system can be processed as membrane coatings, thin films, or wet gels to capture metal ions and that both the sorbent and captured metal ions can be regenerated or directly used as composite catalysts.
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ItemNanoengineering of Poly(ethylene glycol) Particles for Stealth and Targeting(AMER CHEMICAL SOC, 2018-09-18)The assembly of particles composed solely or mainly of poly(ethylene glycol) (PEG) is an emerging area that is gaining increasing interest within bio-nano science. PEG, widely considered to be the "gold standard" among polymers for drug delivery, is providing a platform for exploring fundamental questions and phenomena at the interface between particle engineering and biomedicine. These include the targeting and stealth behaviors of synthetic nanomaterials in biological environments. In this feature article, we discuss recent work in the nanoengineering of PEG particles and explore how they are enabling improved targeting and stealth performance. Specific examples include PEG particles prepared through surface-initiated polymerization, mesoporous silica replication via postinfiltration, and particle assembly through metal-phenolic coordination. This particle class exhibits unique in vivo behavior (e.g., biodistribution and immune cell interactions) and has recently been explored for drug delivery applications.
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ItemLigand-Functionalized Poly(ethylene glycol) Particles for Tumor Targeting and Intracellular Uptake.(American Chemical Society, 2019)Drug carriers typically require both stealth and targeting properties to minimize nonspecific interactions with healthy cells and increase specific interaction with diseased cells. Herein, the assembly of targeted poly(ethylene glycol) (PEG) particles functionalized with cyclic peptides containing Arg-Gly-Asp (RGD) (ligand) using a mesoporous silica templating method is reported. The influence of PEG molecular weight, ligand-to-PEG molecule ratio, and particle size on cancer cell targeting to balance stealth and targeting of the engineered PEG particles is investigated. RGD-functionalized PEG particles (PEG-RGD particles) efficiently target U-87 MG cancer cells under static and flow conditions in vitro, whereas PEG and cyclic peptides containing Arg-Asp-Gly (RDG)-functionalized PEG (PEG-RDG) particles display negligible interaction with the same cells. Increasing the ligand-to-PEG molecule ratio improves cell targeting. In addition, the targeted PEG-RGD particles improve cell uptake via receptor-mediated endocytosis, which is desirable for intracellular drug delivery. The PEG-RGD particles show improved tumor targeting (14% ID g-1) when compared with the PEG (3% ID g-1) and PEG-RDG (7% ID g-1) particles in vivo, although the PEG-RGD particles show comparatively higher spleen and liver accumulation. The targeted PEG particles represent a platform for developing particles aimed at balancing nonspecific and specific interactions in biological systems.
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ItemGel-Mediated Electrospray Assembly of Silica Supraparticles for Sustained Drug Delivery(AMER CHEMICAL SOC, 2018-09-19)Supraparticles (SPs) composed of smaller colloidal particles provide a platform for the long-term, controlled release of therapeutics in biomedical applications. However, current synthesis methods used to achieve high drug loading and those involving biocompatible materials are often tedious and low throughput, thereby limiting the translation of SPs to diverse applications. Herein, we present a simple, effective, and automatable alginate-mediated electrospray technique for the assembly of robust spherical silica SPs (Si-SPs) for long-term (>4 months) drug delivery. The Si-SPs are composed of either porous or nonporous primary Si particles within a decomposable alginate matrix. The size and shape of the Si-SPs can be tailored by controlling the concentrations of alginate and silica primary particles used and key electrospraying parameters, such as flow rate, voltage, and collector distance. Furthermore, the performance (including drug loading kinetics, loading capacity, loading efficiency, and drug release) of the Si-SPs can be tuned by changing the porosity of the primary particles and through the retention or removal (via calcination) of the alginate matrix. The structure and morphology of the Si-SPs were characterized by electron microscopy, dynamic light scattering, N2 adsorption-desorption analysis, and X-ray photoelectron spectroscopy. The cytotoxicity and degradability of the Si-SPs were also examined. Drug loading kinetics and loading capacity for six different types of Si-SPs, using a model protein drug (fluorescently labeled lysozyme), demonstrate that Si-SPs prepared from primary silica particles with large pores can load significant amounts of lysozyme (∼10 μg per SP) and exhibit sustained, long-term release of more than 150 days. Our experiments show that Si-SPs can be produced through a gel-mediated electrospray technique that is robust and automatable (important for clinical translation and commercialization) and that they present a promising platform for long-term drug delivery.
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ItemSupramolecular Metal-Phenolic Gels for the Crystallization of Active Pharmaceutical Ingredients(WILEY-V C H VERLAG GMBH, 2018-06-27)The use of supramolecular gel media for the crystallization of active pharmaceutical ingredients (APIs) is of interest for controlling crystal size, morphology, and polymorphism, as these features determine the performance of pharmaceutical formulations. In contrast to supramolecular systems prepared from synthetic gelators, herein, supramolecular metallogels based on a natural polyphenol (tannic acid) are used for the crystallization of APIs. The gel-grown API crystals exhibit considerable differences in size, morphology, and polymorphism when compared with those formed in solutions. These physical features can also be tailored by varying the gel composition and additives, suggesting an influence of the gel medium on the crystallization outcomes. Furthermore, these gel-API crystal composites can be used for sustained drug release, indicating their potential as drug delivery systems. The facile preparation of these supramolecular gels and the use of naturally abundant components in their synthesis provide a generic platform for studying gel-mediated crystallization of diverse APIs.