In silico screening of molecular imprinting prepolymerization systems: oseltamivir selective polymers through full-system molecular dynamics-based studies (original) (raw)
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The influence of polymer morphology on the performance of molecularly imprinted polymers
Polymer, 2010
This is the first in-depth study examining the effect of morphology on the performance of 2-aminopyridine (2-apy) imprinted polymers. A series of polymers were prepared by varying the amount of crosslinking monomer (EGDMA) whilst the other polymer components remained constant. Physical characterisation was carried out using conventional techniques, such as nitrogen sorption porosimetry and solvent swelling studies. The use of a novel thermal desorption GC-MS technique suggested higher levels of polymer degradation with prolonged exposure to elevated temperatures for those polymers formed with lower amounts of EGDMA. The thermal desorption GC-MS profiles obtained correlated with the physical characteristics of the polymers, where higher levels of polymer bleed was found to occur with larger average pore diameters. Polymer physical characteristics were also found to correlate with the binding parameters (number of binding sites and polymer-template association energy) obtained from the Langmuir-Freundlich Isotherm (L-FI) and affinity distribution spectra (AD). The flexibility of the polymers formed from lower amounts of EGDMA combined the swelling effect of the solvents on the polymers resulted in an increase in affinity, which was both specific and non-specific in nature.
Molecularly Imprinted Polymers: Present and Future Prospective
International Journal of Molecular Sciences, 2011
Molecular Imprinting Technology (MIT) is a technique to design artificial receptors with a predetermined selectivity and specificity for a given analyte, which can be used as ideal materials in various application fields. Molecularly Imprinted Polymers (MIPs), the polymeric matrices obtained using the imprinting technology, are robust molecular recognition elements able to mimic natural recognition entities, such as antibodies and biological receptors, useful to separate and analyze complicated samples such as biological fluids and environmental samples. The scope of this review is to provide a general overview on MIPs field discussing first general aspects in MIP preparation and then dealing with various application aspects. This review aims to outline the molecularly imprinted process and present a summary of principal application fields of molecularly imprinted polymers, focusing on chemical sensing, separation science, drug delivery and catalysis. Some significant aspects about preparation and application of the molecular imprinting polymers with examples taken from the recent literature will be discussed. Theoretical and experimental parameters for MIPs design in terms of the interaction between template and polymer functionalities will be considered and synthesis methods for the improvement of MIP recognition properties will also be presented.
The Application of Molecularly Imprinted Polymers
Molecularly imprinted technology (MIT) has the characteristics of specificity and high selectivity, which is one of the most promising methodologies. Besides, the polymers are made using MIT as the functional material of solid-phase extraction and chromatographic fractionating and sensor, because of the characteristics of the high selectivity, the better stability and easy preparation. This review introduces the progress in the application of MIT and summarizes its application in the chemistry.
Biosensors and Bioelectronics, 2008
Molecularly imprinted polymers (MIPs) for zearalenone analysis have been synthesized using the template mimics cyclododecyl 2,4-dihydroxybenzoate (CDHB), resorcinol and resorcylic acid. The MIPs are photochemically prepared from 2-(diethylamino)ethyl methacrylate (2-DAEM), 4-vinylpyridine (VIPY), 2-hydroxyethyl methacrylate (HEMA) or 1-allylpiperazine (1-ALPP) as the functional monomers, trimethylolpropane trimethacrylate (TRIM) as cross-linker, azobis(isobutyronitrile) as initiator and acetonitrile as porogen. Non-imprinted polymers have been also synthesized for reference purposes. The textural properties of the novel polymers (BET areas, pore volumes and pore size distributions) have been determined from nitrogen adsorption-desorption isotherms. These parameters have shown to be strongly dependent on the presence of the template and the monomer nature. Scanning electron microscopy and solvent uptake experiments support these findings. Microporosity contributes less than 7% to the total pore volume for all the polymers prepared. Interestingly, a 3.5 nm pore opening is observed for all the polymers and additional pore apertures in the 20-40 nm region for VIPY-, HEMA-and 2-DAEM-based MIPs whereas a much wider opening size distribution has been measured for the 1-ALPP-based MIP. Molecular modeling and, particularly, 1 H NMR experiments demonstrate the strong (2:1) complex formed between 1-ALPP and the diphenolic CDHB (K 11 = 4.7 × 10 4 M −1 and K 12 = 2.6 × 10 2 M −1 in acetonitrile) that make the corresponding MIP the most suitable for zearalenone recognition in real samples.
Molecularly imprinted polymers: synthesis and characterisation
Journal of Chromatography B-analytical Technologies in The Biomedical and Life Sciences, 2004
This short review aims to present, in clear English, a summary of the principal synthetic considerations pertaining to good practice in the polymerisation aspects of molecular imprinting, and is primarily aimed at researchers familiar with molecular imprinting methods but with little or no prior experience in polymer synthesis. It is our hope that this will facilitate researchers to plan their own syntheses of molecular imprints in a more logical and structured fashion, and to begin to appreciate the limitations of the present synthetic approaches in this molecularly complex area, as well as the scope for rationally designing improved imprinted materials in the future.
A comparative study of the potential of acrylic and sol–gel polymers for molecular imprinting
Analytica Chimica Acta, 2005
The successful molecular imprinting of 2-aminopyridine (2-apy) in bulk polymerisations of acrylic and sol-gel based polymers has been achieved. Both polymeric systems reveal varying degrees of affinity in rebinding the original template as well as a number of structural analogues. Rebinding was conducted in chloroform, acetonitrile and methanol in order to assess the role of hydrogen bonding in imprinting. The acrylic imprinted polymer retained approximately 50% of the template in rebinding studies in chloroform compared to 100% for the sol-gel. However, this higher affinity for the sol-gel was accompanied by a higher degree of non-specific binding. While the acrylic polymer performed poorly in acetonitrile, the sol-gel maintained a high degree of discrimination.
European Polymer Journal, 2017
In this report, we have investigated factors contributing to the morphology and template recognition of bupivacaine-imprinted copolymers of methacrylic acid (MAA) and ethyleneglycol dimethacrylate (EGDMA). To this end, MAA, the most commonly used functional monomer in noncovalent molecular imprinting protocols, was compared and contrasted with the closely related acrylic acid (AA) in terms of polymer morphologies, recognition characteristics, and molecular level events in the corresponding pre-polymerization mixtures. Two series of analogous bupivacaine-imprinted EGDMA-copolymers containing increasing fractions of either AA or MAA were studied through allcomponent MD simulations in the pre-polymerization phase, equilibrium binding experiments on corresponding synthesized polymers and morphology characterization by N 2-sorption measurements. A higher degree of hydrogen bonding frequency between respective functional monomer and bupivacaine was recorded for the mixtures containing AA compared to those containing MAA. In contrast, results from binding experiments demonstrated higher binding capacities for the polymers prepared with MAA than for those prepared with AA, which is explained by differences in polymer morphology. The surface areas and pore volumes of the AA-polymers were higher than for the MAA-polymers and the overall 2 pore structure in the AA-polymers was ink-bottle shaped while the pores in the MAA-polymers were slit-shaped. We suggest that the methyl substituent of MAA contributes to differences in the reaction kinetics for AA and MAA during polymerization and resulted in different morphologies, in particular pore shape, which affected mass-transfer and consequently the binding qualities of the materials.