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Evaluation of Polyurea-Crosslinked Alginate Aerogels for Seawater Decontamination.

ABSTRACT: Polyurea-crosslinked Ca-alginate (X-Ca-alginate) aerogel beads (diameter: 3.3 mm) were evaluated as adsorbents of metal ions, organic solvents, and oils. They were prepared via reaction of an aromatic triisocyanate (Desmodur RE) with pre-formed Ca-alginate wet gels and consisted of 54% polyurea and 2% calcium. X-Ca-alginate aerogels are hydrophobic nanoporous materials (90% v/v porosity), with a high BET surface area (459 m2/g-1), and adsorb PbII not only from ultrapure water (29 mg/g-1) but also from seawater (13 mg/g-1) with high selectivity. The adsorption mechanism involves replacement of CaII by PbII ions coordinated to the carboxylate groups of the alginate backbone. After treatment with a Na2EDTA solution, the beads can be reused, without significant loss of activity for at least two times. X-Ca-alginate aerogels can also uptake organic solvents and oil from seawater; the volume of the adsorbate can be as high as the total pore volume of the aerogel (6.0 mL/g-1), and the absorption is complete within seconds. X-Ca alginate aerogels are suitable for the decontamination of aquatic environments from a broader range of inorganic and organic pollutants.

SUBMITTER: Paraskevopoulou P

PROVIDER: S-EPMC8005931 | biostudies-literature | 2021 Mar

REPOSITORIES: biostudies-literature

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Evaluation of Polyurea-Crosslinked Alginate Aerogels for Seawater Decontamination.

Paraskevopoulou Patrina P Raptopoulos Grigorios G Leontaridou Faidra F Papastergiou Maria M Sakellari Aikaterini A Karavoltsos Sotirios S

Gels (Basel, Switzerland) 20210304 1

Polyurea-crosslinked Ca-alginate (X-Ca-alginate) aerogel beads (diameter: 3.3 mm) were evaluated as adsorbents of metal ions, organic solvents, and oils. They were prepared via reaction of an aromatic triisocyanate (Desmodur RE) with pre-formed Ca-alginate wet gels and consisted of 54% polyurea and 2% calcium. X-Ca-alginate aerogels are hydrophobic nanoporous materials (90% v/v porosity), with a high BET surface area (459 m2/g-1), and adsorb PbII not only from ul ...[more]

PMID: 33806357

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Project description:Alginate hydrogels have been investigated for a broad variety of medical applications. The ability to assemble hydrogels at neutral pH and mild temperatures makes alginate a popular choice for the encapsulation and delivery of cells and proteins. Alginate has been studied extensively for the delivery of islets as a treatment for type 1 diabetes. However, poor stability of the encapsulation systems after implantation remains a challenge. In this paper, alginate was modified with 2-aminoethyl methacrylate hydrochloride (AEMA) to introduce groups that can be photoactivated to generate covalent bonds. This enabled formation of dual crosslinked structure upon exposure to ultraviolet light following initial ionic crosslinking into bead structures. The degree of methacrylation was varied and in vitro stability, long term swelling, and cell viability examined. At low levels of the methacrylation, the beads could be formed by first ionic crosslinks followed by exposure to ultraviolet light to generate covalent bonds. The methacrylated alginate resulted in more stable beads and cells were viable following encapsulation. Alginate microbeads, ionic (unmodified) and dual crosslinked, were implanted into a rat omentum pouch model. Implantation was performed with a local injection of 100 µl of 50 µg/ml of Lipopolysaccharide (LPS) to stimulate a robust inflammatory challenge in vivo. Implants were retrieved at 1 and 3 weeks for analysis. The unmodified alginate microbeads had all failed by week 1, whereas the dual-crosslinked alginate microbeads remained stable up through 3 weeks. The modified alginate microbeads may provide a more stable alternative to current alginate-based systems for cell encapsulation.Statement of significanceAlginate, a naturally occurring polysaccharide, has been used for cell encapsulation to prevent graft rejection of cell transplants for people with type I diabetes. Although some success has been observed in clinical trials, the lack of reproducibility and failure to reach insulin dependence for longer periods of time indicates the need for improvements in the procedure. A major requirement for the long-term function of alginate encapsulated cells is the mechanical stability of microcapsules. Insufficient mechanical integrity of the capsules can lead to immunological reactions in the recipients. In this work, alginate was modified to allow photoactivatable groups in order to allow formation of covalent crosslinks in addition to ionic crosslinking. The dual crosslinking design prevents capsule breakdown following implantation in vivo.

Project description:Tunable porous composite materials to control metal and metal oxide functionalization, conductivity, pore structure, electrolyte mass transport, mechanical strength, specific surface area, and magneto-responsiveness are critical for a broad range of energy storage, catalysis, and sensing applications. Biotemplated transition metal composite aerogels present a materials approach to address this need. To demonstrate a solution-based synthesis method to develop cobalt and cobalt oxide aerogels for high surface area multifunctional energy storage electrodes, carboxymethyl cellulose nanofibers (CNF) and alginate biopolymers were mixed to form hydrogels to serve as biotemplates for cobalt nanoparticle formation via the chemical reduction of cobalt salt solutions. The CNF-alginate mixture forms a physically entangled, interpenetrating hydrogel, combining the properties of both biopolymers for monolith shape and pore size control and abundant carboxyl groups that bind metal ions to facilitate biotemplating. The CNF-alginate hydrogels were equilibrated in CaCl2 and CoCl2 salt solutions for hydrogel ionic crosslinking and the prepositioning of transition metal ions, respectively. The salt equilibrated hydrogels were chemically reduced with NaBH4, rinsed, solvent exchanged in ethanol, and supercritically dried with CO2 to form aerogels with a specific surface area of 228 m2/g. The resulting aerogels were pyrolyzed in N2 gas and thermally annealed in air to form Co and Co3O4 porous composite electrodes, respectively. The multifunctional composite aerogel's mechanical, magnetic, and electrochemical functionality was characterized. The coercivity and specific magnetic saturation of the pyrolyzed aerogels were 312 Oe and 114 emu/gCo, respectively. The elastic moduli of the supercritically dried, pyrolyzed, and thermally oxidized aerogels were 0.58, 1.1, and 14.3 MPa, respectively. The electrochemical testing of the pyrolyzed and thermally oxidized aerogels in 1 M KOH resulted in specific capacitances of 650 F/g and 349 F/g, respectively. The rapidly synthesized, low-cost, hydrogel-based synthesis for tunable transition metal multifunctional composite aerogels is envisioned for a wide range of porous metal electrodes to address energy storage, catalysis, and sensing applications.

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Evaluation of Polyurea-Crosslinked Alginate Aerogels for Seawater Decontamination.

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Evaluation of Polyurea-Crosslinked Alginate Aerogels for Seawater Decontamination.

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