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Molecularly Imprinted Polymers: Impactful Technology vs. Academic Exercise

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Organic Chemistry".

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 20561

Special Issue Editor

Division of Biomaterials and Tissue Engineering, UCL Eastman Dental Institute, Royal Free Hospital, UCL Medical School, Rowland Hill Street, London NW3 2PF, UK
Interests: molecular imprinting; nanotechnology; drug delivery; tissue engineering; biomaterials; biodegradable polymers; solid-phase synthesis

Special Issue Information

Dear Colleagues,

Molecular imprinting technology allows the introduction of specific recognition sites within a polymeric material by introducing the desired target molecule, called template, during the polymerisation process. There are many factors driving the successful production of a molecularly imprinted polymer (MIP), including the adequate selection of monomers capable of establishing a molecular interaction with the template, as well as the adjustment of the process parameters (including the template removal) to the final format of the polymer to be produced. Almost 90 years have passed since the publication of what is considered to be the first example of molecular imprinting; however, it is debated whether molecular imprinting is still limited to an academic intellectual exercise or if it is actually making an impact on various applications (such as separations, sensing, catalysis, imaging, and drug delivery) beyond academia.

 

The present Special Issue, “Molecularly Imprinted Polymers: Impactful Technology vs. Academic Exercise”, aims to assemble a diverse collection of articles describing innovative aspects of MIP synthesis and application. In particular, contributions are welcome concerning the generation of MIPs for commercial applications; the translation of MIPs usage beyond academia; as well as bold and innovative synthetic routes, design and formats for MIPs with either extremely promising or established impact beyond the academic scenario. Both research articles and reviews will be considered.


Dr. Alessandro Poma
Guest Editor

Manuscript Submission Information

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Keywords

  • Molecularly imprinted polymer
  • Molecular imprinting
  • Molecular imprinting impact
  • Synthetic biology
  • Plastic antibodies
  • Biomimetic materials
  • Drug delivery
  • Separation
  • Sensing
  • Imaging
  • Catalysis

Published Papers (6 papers)

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Research

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15 pages, 33522 KiB  
Article
A Disposable Sensor Chip Using a Paste Electrode with Surface-Imprinted Graphite Particles for Rapid and Reagentless Monitoring of Theophylline
by Aaryashree, Tomoji Ohishi and Yasuo Yoshimi
Molecules 2022, 27(8), 2456; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules27082456 - 11 Apr 2022
Cited by 2 | Viewed by 2928
Abstract
This work focuses on a carbon-based imprinted polymer composite, employed as a molecular recognition and sensing interface in fabricating a disposable electrochemical sensor. The carbon-paste electrode was made of a molecularly imprinted polymer comprising a copolymer of methacrylic acid as the functional monomer [...] Read more.
This work focuses on a carbon-based imprinted polymer composite, employed as a molecular recognition and sensing interface in fabricating a disposable electrochemical sensor. The carbon-paste electrode was made of a molecularly imprinted polymer comprising a copolymer of methacrylic acid as the functional monomer and blended crosslinking monomers of N,N′-methylenebisacrylamide, and ethylene glycol dimethacrylate, with theophylline as the template. The analytical properties of the proposed theophylline sensor were investigated, and the findings revealed an increase in differential pulse voltammetric current compared to the non-imprinted electrode. Under optimized conditions, the sensor has shown high sensitivity, high selectivity, lower detection limit (2.5 µg/mL), and satisfactory long-term stability. Further, the sensor was tested in whole bovine blood and validated without any matrix effect and cross-reactivity. Additionally, chronoamperometry of the sensor chip supported a rapid determination of THO with a short response time of 3 s. This carbon-paste electrode is highly specific for theophylline and may be applied as a drug sensor for clinical use. Full article
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19 pages, 2275 KiB  
Article
Molecular Imprinting Using a Functional Chain Transfer Agent
by Phonlakrit Muang-Non, K. Fremielle Lim, Anthony Katselas and Clovia I. Holdsworth
Molecules 2022, 27(4), 1162; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules27041162 - 09 Feb 2022
Viewed by 1385
Abstract
This study demonstrates the feasibility of molecular imprinting using a functional chain transfer agent sans a functional monomer. Ethylene glycol dimethacrylate (EGDMA)-based MIPs were synthesised in the presence of thioglycolic acid (TGA) possessing a carboxylic acid group, capable of interacting with the chosen [...] Read more.
This study demonstrates the feasibility of molecular imprinting using a functional chain transfer agent sans a functional monomer. Ethylene glycol dimethacrylate (EGDMA)-based MIPs were synthesised in the presence of thioglycolic acid (TGA) possessing a carboxylic acid group, capable of interacting with the chosen test template R,S-(±)-propranolol (PNL) and a labile S-H bond to facilitate an efficient chain transfer reaction. Quantitative 1H NMR measurements showed high PNL and TGA incorporation within the MIP, indicating an efficient chain transfer process and a favourable interaction between PNL and TGA. TGA-50, with the lowest amount of CTA, showed the largest imprinting effect and an imprinting factor (IF) of 2.1. The addition of MAA to the formulation improved the binding capacity of PNL to the MIP but also increased NIP binding, resulting in a slightly decreased IF of 1.5. The Kd for the high-affinity sites of the TGA/MAA MIP were found to be two times lower (10 ± 1 μM) than that for the high-affinity sites of the TGA-only MIPs, suggesting that the incorporation of the functional monomer MAA increases the affinity towards the PNL template. Selectivity studies, cross-reactivity as well as binary competitive and displacement assays showed the TGA-based MIPs to be highly selective towards PNL against pindolol and slightly competitive against atenolol. The morphologies of the polymers were shown to be affected by the concentration of the TGA, transforming into discrete macrospheres (from small aggregates) at a higher TGA concentration. Full article
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16 pages, 1739 KiB  
Article
A Molecularly Imprinted Polymer-based Dye Displacement Assay for the Rapid Visual Detection of Amphetamine in Urine
by Joseph W. Lowdon, Kasper Eersels, Rocio Arreguin-Campos, Manlio Caldara, Benjamin Heidt, Renato Rogosic, Kathia L. Jimenez-Monroy, Thomas J. Cleij, Hanne Diliën and Bart van Grinsven
Molecules 2020, 25(22), 5222; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25225222 - 10 Nov 2020
Cited by 15 | Viewed by 3158
Abstract
The rapid sensing of drug compounds has traditionally relied on antibodies, enzymes and electrochemical reactions. These technologies can frequently produce false positives/negatives and require specific conditions to operate. Akin to antibodies, molecularly imprinted polymers (MIPs) are a more robust synthetic alternative with the [...] Read more.
The rapid sensing of drug compounds has traditionally relied on antibodies, enzymes and electrochemical reactions. These technologies can frequently produce false positives/negatives and require specific conditions to operate. Akin to antibodies, molecularly imprinted polymers (MIPs) are a more robust synthetic alternative with the ability to bind a target molecule with an affinity comparable to that of its natural counterparts. With this in mind, the research presented in this article introduces a facile MIP-based dye displacement assay for the detection of (±) amphetamine in urine. The selective nature of MIPs coupled with a displaceable dye enables the resulting low-cost assay to rapidly produce a clear visual confirmation of a target’s presence, offering huge commercial potential. The following manuscript characterizes the proposed assay, drawing attention to various facets of the sensor design and optimization. To this end, synthesis of a MIP tailored towards amphetamine is described, scrutinizing the composition and selectivity (ibuprofen, naproxen, 2-methoxphenidine, quetiapine) of the reported synthetic receptor. Dye selection for the development of the displacement assay follows, proceeded by optimization of the displacement process by investigating the time taken and the amount of MIP powder required for optimum displacement. An optimized dose–response curve is then presented, introducing (±) amphetamine hydrochloride (0.01–1 mg mL−1) to the engineered sensor and determining the limit of detection (LoD). The research culminates in the assay being used for the analysis of spiked urine samples (amphetamine, ibuprofen, naproxen, 2-methoxphenidine, quetiapine, bupropion, pheniramine, bromopheniramine) and evaluating its potential as a low-cost, rapid and selective method of analysis. Full article
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Review

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34 pages, 688 KiB  
Review
Molecularly Imprinted Polymers (MIPs) in Sensors for Environmental and Biomedical Applications: A Review
by Abbas J. Kadhem, Guillermina J. Gentile and Maria M. Fidalgo de Cortalezzi
Molecules 2021, 26(20), 6233; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26206233 - 15 Oct 2021
Cited by 52 | Viewed by 4670
Abstract
Molecular imprinted polymers are custom made materials with specific recognition sites for a target molecule. Their specificity and the variety of materials and physical shapes in which they can be fabricated make them ideal components for sensing platforms. Despite their excellent properties, MIP-based [...] Read more.
Molecular imprinted polymers are custom made materials with specific recognition sites for a target molecule. Their specificity and the variety of materials and physical shapes in which they can be fabricated make them ideal components for sensing platforms. Despite their excellent properties, MIP-based sensors have rarely left the academic laboratory environment. This work presents a comprehensive review of recent reports in the environmental and biomedical fields, with a focus on electrochemical and optical signaling mechanisms. The discussion aims to identify knowledge gaps that hinder the translation of MIP-based technology from research laboratories to commercialization. Full article
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10 pages, 240 KiB  
Review
A Note about Crosslinking Density in Imprinting Polymerization
by Anja Mueller
Molecules 2021, 26(17), 5139; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26175139 - 25 Aug 2021
Cited by 9 | Viewed by 1855
Abstract
Imprinting polymerization is an exciting technique since it leads to specific binding sites, which are the basis of a variety of applications, such as sensors, detectors, and catalysts. The specific binding sites are created using templates and then fixing the structure of the [...] Read more.
Imprinting polymerization is an exciting technique since it leads to specific binding sites, which are the basis of a variety of applications, such as sensors, detectors, and catalysts. The specific binding sites are created using templates and then fixing the structure of the binding site with crosslinking. The literature review of imprinting polymerizations shows that the crosslinking density governs the physical properties of the resulting molecularly imprinted polymer (MIP). It is also a factor governing the capacity and the selectivity of MIPs. Reviewing polymer science data and theory, the crosslinking density commonly used in MIP synthesis is unusually high. The data reviewed here suggest that more research is needed to determine the optimal crosslinking density for MIPs. Full article
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25 pages, 4948 KiB  
Review
Advances in Molecularly Imprinted Polymers as Drug Delivery Systems
by Rui Liu and Alessandro Poma
Molecules 2021, 26(12), 3589; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26123589 - 11 Jun 2021
Cited by 48 | Viewed by 5278
Abstract
Despite the tremendous efforts made in the past decades, severe side/toxic effects and poor bioavailability still represent the main challenges that hinder the clinical translation of drug molecules. This has turned the attention of investigators towards drug delivery vehicles that provide a localized [...] Read more.
Despite the tremendous efforts made in the past decades, severe side/toxic effects and poor bioavailability still represent the main challenges that hinder the clinical translation of drug molecules. This has turned the attention of investigators towards drug delivery vehicles that provide a localized and controlled drug delivery. Molecularly imprinted polymers (MIPs) as novel and versatile drug delivery vehicles have been widely studied in recent years due to the advantages of selective recognition, enhanced drug loading, sustained release, and robustness in harsh conditions. This review highlights the design and development of strategies undertaken for MIPs used as drug delivery vehicles involving different drug delivery mechanisms, such as rate-programmed, stimuli-responsive and active targeting, published during the course of the past five years. Full article
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