Abstract
Aspects of the molecular-level basis for the function of ethylene glycol dimethacrylate and trimethylolproprane trimethacrylate crosslinked methacrylic acid copolymers molecularly imprinted with (S)-propranolol have been studied using a series of all-component and all-atom molecular dynamics studies of the corresponding prepolymerization systems. The crosslinking agents were observed to contribute to template complexation, and the results were contrasted with previously reported template-recognition behavior of the corresponding polymers. Differences in the extent to which the two crosslinkers interacted with the functional monomer were identified, and correlations were made to polymer-ligand recognition behavior and the results of nuclear magnetic resonance spectroscopic studies studies. This study demonstrates the importance of considering the functional monomer–crosslinker interaction when designing molecularly imprinted polymers, and highlights the often neglected general contribution of crosslinker to determining the nature of molecularly imprinted polymer-template selectivity.
Highlights
IntroductionMaterials capable of facilitating Angstrom- or nano-scale events such as in chemical catalysis or material-biomacromolecular interactions require architectures presenting functionalities and molecular-level features that permit high-fidelity molecular discrimination [1]
Materials capable of facilitating Angstrom- or nano-scale events such as in chemical catalysis or material-biomacromolecular interactions require architectures presenting functionalities and molecular-level features that permit high-fidelity molecular discrimination [1].Molecular imprinting [2,3,4,5,6,7,8] is a technique for producing highly selective synthetic receptors for molecular structures spanning in size from ions to biomacromolecules
We elected to use full-system all-atom molecular dynamics (MD)-based studies of two polymer systems previously described by Andersson [33] to examine the molecular basis for template recognition in the ethylene glycol dimethacrylate (EGDMA)- and TRIM-crosslinked methacrylic acid (MAA) copolymers reported in that seminal study
Summary
Materials capable of facilitating Angstrom- or nano-scale events such as in chemical catalysis or material-biomacromolecular interactions require architectures presenting functionalities and molecular-level features that permit high-fidelity molecular discrimination [1]. MIPs have demonstrated affinities and cross-reactivity profiles comparable to their biological counterparts [9,10,11,12] They have been employed as substitutes for biological antibodies in various application areas [13], e.g., medical diagnostic, forensic assay development, in solid phase extraction, as biosensor recognition elements and in catalysis. Efforts to understand the molecular-level basis for the molecular imprinting process have focused on the interaction of functional monomers and template, as reflected in the development of a wide range of novel functional monomers [18,19,20,21], a focus that is reflected in the early theoretical studies of MIP systems [22,23,24]. We have employed these computational tools to investigate the roles of EGDMA and TRIM in the SPR-MIP prepolymerization mixtures, and have drawn correlations with template recognition in the corresponding polymers, and with data from 1H-nuclear magnetic resonance (NMR) studies of the corresponding prepolymerization mixtures
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