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Projeto de investigação
Green strategy on the development of plastic antibodies for bio-recognition
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Biomolecular Fishing
Publication . Furtado, Ana I.; Viveiros, R.; Bonifácio, Vasco D. B.; Melo, André; Casimiro, T.; DQ - Departamento de Química; LAQV@REQUIMTE; ACS - American Chemical Society
Biopurification is a challenging and growing market. Despite great efforts in the past years, current purification strategies still lack specificity, efficiency, and cost-effectiveness. The development of more sustainable functional materials and processes needs to address pressing environmental goals, efficiency, scale-up, and cost. Herein, l-leucine (LEU)-molecularly imprinted polymers (MIPs), LEU-MIPs, are presented as novel biomolecular fishing polymers for affinity sustainable biopurification. Rational design was performed using quantum mechanics calculations and molecular modeling for selecting the most appropriate monomers. LEU-MIPs were synthesized for the first time by two different green approaches, supercritical carbon dioxide (scCO2) technology and mechanochemistry. A significant imprinting factor of 12 and a binding capacity of 27 mg LEU/g polymer were obtained for the LEU-MIP synthesized in scCO2 using 2-vinylpyridine as a functional monomer, while the LEU-MIP using acrylamide as a functional monomer synthesized by mechanochemistry showed an imprinting factor of 1.4 and a binding capacity of 18 mg LEU/g polymer, both systems operating at a low binding concentration (0.5 mg LEU/mL) under physiological conditions. As expected, at a higher concentration (1.5 mg LEU/mL), the binding capacity was considerably increased. Both green technologies show high potential in obtaining ready-to-use, stable, and low-cost polymers with a molecular recognition ability for target biomolecules, being promising materials for biopurification processes.
Development of Smart Polymers using Clean Technologies for Application in Bio-purification Processes
Publication . Furtado, Ana Isabel Carreiro; Casimiro, Teresa; Viveiros, Raquel
The production of biological products is increasing, with a consequent intensification of the separation and purification processes involved. The existing technologies are very expensive, and in some cases, cannot achieve high efficiency and have no specificity. In order to find solutions to the limitations present in the bioindustry, herein synthetic smart affinity polymers were developed for the first time towards a biomolecule, L-Leucine, using green technologies. The polymers were obtained in two steps: a polymer synthesis by Molecular Imprinting Technique (MIT) using acrylamide as the functional monomer in supercritical carbon dioxide (scCO2), and a polymer post-complexation with beryllium. In the first step, a molecularly crosslinked polymer was prepared using a 1:50:100 molar ratio of template/functional
monomer/crosslinker and 2% by weight of initiator at a pressure of 200 bar and a temperature of 40 °C. The yield of synthesis was about 30%. Subsequently, the polymers produced were post-complexed by a mechanochemical process using a planetary ball mill (rotation speed of 500 rpm for 10 min.
The polymers, obtained as dry powders, were characterized by SEM, FTIR, XRD and particle size distribution, as well as mean particle diameter, using the Morphologi G3 equipment. Binding tests were also performed for different L-Leucine concentrations at pH = 7.4. The results of these tests for the polymers obtained in the first step are very promising (Q = 1815 mg LEU/g polymer), presenting an imprinting factor of 3.07. This process has proven to be very attractive, simple and low cost, with potential application in biopurification processes. The post-complexed polymers were less promising than the non-complexed polymers.
Development of affinity polymeric particles for the removal of 4-dimethylaminopyridine (DMAP) from active pharmaceutical ingredient crude streams using a green technology
Publication . Viveiros, Raquel; Pinto, José J.; Costa, Nuno; Heggie, William; Casimiro, Teresa; LAQV@REQUIMTE; DQ - Departamento de Química; Elsevier
Polymeric particles with affinity for 4-dimethylaminipyridine (DMAP) were developed by molecular imprinting using supercritical carbon dioxide (scCO2) technology, for cleanup of this potentially genotoxic impurity from crude mixtures of Active Pharmaceutical Ingredients (APIs). DMAP-molecularly imprinted polymer (DMAP-MIP) and the respective control, the non-molecularly imprinted polymer (NIP) were produced by free radical polymerization using methacrylic acid as monomer, ethylene glycol dimethacrylate as crosslinker and AIBN as free-radical initiator in scCO2. The materials were obtained in high yield and were characterized chemically, physically and morphologically. Their extraction efficiency was evaluated by dynamic binding experiments using two solutions: i) a solution containing 104 ppm DMAP solution; ii) model pharmaceutical mixture containing 104 ppm of DMAP and 1018 ppm of Mometasone furoate (API). Particles were able to remove 18.3 µmol DMAP/g polymer from a 104 ppm DMAP solution (i) and 1004.6 µmol DMAP/g API (ii). In addition, high recoveries of both DMAP and API were obtained, above 99%.
Iron-free mechanochemical limonene inverse vulcanization
Publication . Tedjini, Rima; Viveiros, Raquel; Casimiro, Teresa; Bonifácio, Vasco D. B.; LAQV@REQUIMTE; RSC - Royal Society of Chemistry
An iron-free mechanochemical-assisted limonene inverse vulcanization is reported. The process makes use of only limonene and sulphur, industrial waste by-products, under mild conditions (ca. 40 °C) and short time (2 h) using a zirconium oxide reactor and a planetary ball mil. The obtained high value products are light yellow solids, readily soluble in chloroform, optically active oligosulfides, which are different from polysulfides reported under conventional conditions (ca. 185 °C), as confirmed by NMR spectroscopy and mass spectrometry. A general reaction mechanism is proposed, initiated by homolytic sulphur ring opening triggered by mechanical stress, and involving thiirane intermediates, via an addition–elimination reaction of sulphur to the limonene double bonds.
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Fundação para a Ciência e a Tecnologia
Programa de financiamento
3599-PPCDT
Número da atribuição
PTDC/EQU-EQU/32473/2017