Probing the Structural and Binding Mechanism Heterogeneity of Molecularly Imprinted Polymers

Schauperl, Michael; Lewis, Dewi W.

doi:10.1021/jp506157x

Cited by 23 publications

(16 citation statements)

References 45 publications

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“…This model well fit the saturation phenomena which are always observed when a sufficiently high amount of A is adsorbed on the MIP i.e., when [A] >> 1/K A , and [A] = c R . Equation (2) and the derived Equation (3) hold when only one kind of interaction sites is present in MIP, however different kinds of sites with different affinities for A can be present in the non-covalent MIPs [20], due to their inherent heterogeneity. The presence of multiple classes of sites is indicated by a curvature of the Scatchard plot.…”

Section: Methodsmentioning

confidence: 99%

“…For this reason the investigation of the binding properties of these materials is of wide interest for sensing applications. The evaluation of the binding properties of MIPs can be a challenging task, due to the existence of heterogeneous binding sites in MIPs, particularly those synthesized by a non-covalent bulk procedure [18,19,20,21]. The heterogeneity may diminish the performance of MIPs in some analytical application.…”

Section: Introductionmentioning

confidence: 99%

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Sensing by Molecularly Imprinted Polymer: Evaluation of the Binding Properties with Different Techniques

Pesavento

Marchetti

Maria

et al. 2019

Sensors

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The possibility of investigating the binding properties of the same molecularly imprinted polymer (MIP), most probably heterogeneous, at various concentration levels by different methods such as batch equilibration and sensing, is examined, considering two kinds of sensors, based respectively on electrochemical and surface plasmon resonance (SPR) transduction. As a proof of principle, the considered MIP was obtained by non-covalent molecular imprinting of 2-furaldehyde (2-FAL). It has been found that different concentration ranges of 2-FAL in aqueous matrices can be measured by the two sensing methods. The SPR sensor responds in a concentration range from 1 × 10−4 M down to about 1 × 10−7 M, while the electrochemical sensor from about 5 × 10−6 M up to about 9 × 10−3 M. The binding isotherms have been fit to the Langmuir adsorption model, in order to evaluate the association constant. Three kinds of sites with different affinity for 2-FAL have been detected. The sites at low affinity are similar to the interaction sites of the corresponding NIP since they have a similar association constant. This is near to the affinity evaluated by batch equilibration too. The same association constant has been evaluated in the same concentration range. The sensing methods have been demonstrated to be very convenient for the characterization of the binding properties of MIP in comparison to the batch equilibration, in terms of reproducibility and low amount of material required for the investigation.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Sensing by Molecularly Imprinted Polymer: Evaluation of the Binding Properties with Different Techniques

Pesavento

Marchetti

Maria

et al. 2019

Sensors

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“…The use of a computationally determined ratio alone, which is calculated under ideal conditions, has been reported to produce an inferior MIP with a high incidence of non-specific and heterogeneous binding behaviour caused by the disruption of the majority of the template-FM complexes by the solvent and cross-linker (49). For this reason, an excess of monomer as a 'factor of safety' was added to the calculated ideal ratio.…”

Section: Thermodynamic Calculation Of Stoichiometric Ratio and Mip Comentioning

confidence: 99%

“…Two radical initiators were selected for polymerisation both of which had differing rates of decomposition (k d ) with AIBN at 60ºC and AICN at 80ºC decomposing at rates of approximately A c c e p t e d M a n u s c r i p t 21 17x10 -5 s -1 and 6.5x10 -6 s -1 respectively (49). The latter can also be initiated via UV excitation at room temperature.…”

Section: Selection Of Initiator and Polymerisation Temperaturementioning

confidence: 99%

Computational design of molecularly imprinted polymer for direct detection of melamine in milk

Bates

Busato

Piletska

et al. 2017

Separation Science and Technology

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A novel protocol for use of molecularly imprinted polymer (MIP) in analysis of melamine is presented. Design of polymer for melamine has been achieved using a combination of computational techniques and laboratory trials, the former greatly reducing the duration of the latter. The compatibility and concerted effect of monomers and solvents were also investigated and discussed. Two novel open source tools were presented which are: the online polymer calculator from mipdatabase.com and the application of the Gromacs modelling suite to determine the ideal stoichiometric ratio between template and functional monomer. A c c e p t e d M a n u s c r i p t 2

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“…Greater understanding of the interactions between the target and the binding site is necessary for MIPs to achieve their maximum potential as extracting and sensing agents, as well as to recognize the theoretical limitations of the technology. For us to explore these limitations, it is necessary to explore theoretically “perfect” binding sites …”

Section: Introductionmentioning

confidence: 99%

In silico characterization of enantioselective molecularly imprinted binding sites

Terracina

Sharfstein

Bergkvist

2017

J of Molecular Recognition

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A 2-step molecular mechanical and quantum mechanical geometry optimization scheme (MM ➔ QM) was used to "computationally imprint" chiral molecules. Using a docking technique, we show the imprinted binding sites to exhibit an enantioselective preference for the imprinted molecule over its enantiomer. Docking of structurally similar chiral molecules showed that the sites computationally imprinted with R- or S-tBOC-tyrosine were able to differentiate between R- and S-forms of other tyrosine derivatives. The cross-enantioselectivity did not hold for chiral molecules that did not share the tyrosine H-bonding functional group orientations. Further analysis of the individual monomer-target interactions within the binding site lead us to conclude that H-bonding functional groups that are located immediately next to the chiral center and therefore spatially fixed relative to the chiral center will have a stronger contribution to the enantioselectivity of the site than those groups separated from the chiral center by 2 or more rotatable bonds. Here, we present our novel approach for computationally imprinting and characterizing enantioselective binding sites. All modeling schemes were designed to minimize the computational expense. In silico analysis of the properties of molecularly imprinted polymer systems will ultimately allow for the fabrication of more sensitive and selective materials.

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Probing the Structural and Binding Mechanism Heterogeneity of Molecularly Imprinted Polymers

Cited by 23 publications

References 45 publications

Sensing by Molecularly Imprinted Polymer: Evaluation of the Binding Properties with Different Techniques

Sensing by Molecularly Imprinted Polymer: Evaluation of the Binding Properties with Different Techniques

Computational design of molecularly imprinted polymer for direct detection of melamine in milk

In silico characterization of enantioselective molecularly imprinted binding sites

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