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Molecularly imprinted polymers (MIPs) are established artificial molecular recognition platforms with tailored selectivity towards a target molecule, whose synthesis and functionality are highly influenced by the nature of the solvent employed in their synthesis. Steps towards the "greenification" of molecular imprinting technology (MIT) has already been initiated by the elaboration of green MIT principles; developing MIPs in a solvent-free environment may not only offer an eco-friendly alternative, but could also significantly influence the affinity and expected selectivity of the resulting binding sites. In the current study the first solvent-free mechanochemical synthesis of MIPs via liquid-assisted grinding (LAG) is reported. The successful synthesis of the imprinted polymer was functionally demonstrated by measuring its template rebinding capacity and the selectivity of the molecular recognition process in comparison with the ones obtained by the conventional, non-covalent molecular imprinting process in liquid media. The results demonstrated similar binding capacities towards the template molecule and superior chemoselectivity compared to the solution-based MIP synthesis method. The adoption of green chemistry principles with all their inherent advantages in the synthesis of MIPs may not only be able to alleviate the potential environmental and health concerns associated with their analytical (e.g., selective adsorbents) and biomedical (e.g., drug carriers or reservoirs) applications, but might also offer a conceptual change in molecular imprinting technology. [ABSTRACT FROM AUTHOR]

(1) Background: The current limitations of glioblastoma (GBM) chemotherapy were addressed by developing a molecularly imprinted polymer (MIP)-based drug reservoir designed for the localized and sustained release of ruxolitinib (RUX) within the tumor post-resection cavity, targeting residual infiltrative cancerous cells, with minimum toxic effects toward normal tissue. (2) Methods: MIP reservoirs were synthesized by precipitation polymerization using acrylamide, trifluoromethacrylic acid, methacrylic acid, and styrene as monomers. Drug release profiles were evaluated by real-time and accelerated release studies in phosphate-buffered solution as a release medium. The cytotoxicity of polymers and free monomers was evaluated in vitro on GBM C6 cells using the Alamar Blue assay, optical microscopy, and CCK8 cell viability assay. (3) Results: Among the four synthesized MIPs, trifluoromethacrylic acid-based polymer (MIP 2) was superior in terms of loading capacity (69.9 μg RUX/mg MIP), drug release, and efficacy on GBM cells. Accelerated drug release studies showed that, after 96 h, MIP 2 released 42% of the loaded drug at pH = 7.4, with its kinetics fitted to the Korsmeyer–Peppas model. The cell viability assay proved that all studied imprinted polymers provided high efficacy on GBM cells. (4) Conclusions: Four different drug-loaded MIPs were developed and characterized within this study, with the purpose of obtaining a drug delivery system (DDS) embedded in a fibrin-based hydrogel for the local, post-surgical administration of RUX in GBM in animal models. MIP 2 emerged as superior to the others, making it more suitable and promising for further in vivo testing. [ABSTRACT FROM AUTHOR]

Molecularly imprinted polymers (MIPs) have been proven to be a promising candidate for drug delivery systems (DDS) due to their ability to provide a sustained and controlled drug release, making them useful for treating a wide range of medical conditions. MIP-based DDS offer many advantages, including the administration of a smaller drug doses, due to the higher drug payload or targeted delivery, resulting in fewer side effects, as well as the possibility of attaining high concentrations of the drug in the targeted tissues. Whether designed as drug reservoirs or targeted DDS, MIPs are of great value to drug delivery as conventional drug formulations can be redesigned as DDS to overcome the active pharmaceutical ingredient's (APIs) poor bioavailability, toxic effects, or other shortcomings that previously made them less efficient or unsuitable for therapy. Therefore, MIP design could be a promising alternative to the challenging research and development of new lead compounds. Research on MIPs is primarily conducted from a material science perspective, which often overlooks some of their key pharmaceutical requirements. In this review, we emphasize the specific features that make MIPs suitable for clinical use, from both a material science and a biopharmaceutical perspective. [ABSTRACT FROM AUTHOR]

This study is focused on the molecular recognition mechanism of a methacrylate-based R (+)-atenolol molecularly imprinted polymer (MIP), employed as a chiral sensing interface in the construction of a novel electrochemical sensor. The MIP was electrogenerated as an ultrathin-film onto the surface of a carbon paste working electrode under potentiodynamic conditions in a non-aqueous media. Differential pulse voltammetry served as signal transduction method for the direct and indirect (by means of two redox probes, [Fe(CN) 6 ] 3−/4− and 1,1′-ferrocene dimethanol, respectively) detection of the underlying molecular recognition process. The rebinding of the template enantiomer led to changes in solute permeability of the MIP-layer, indicating the presence of a “gate effect” as part of the molecular recognition process. [ABSTRACT FROM AUTHOR]

The development of a chiral electrochemical sensor using an electrogenerated molecularly imprinted polymer (MIP)-based ultrathin film using R(+)-atenolol (ATNL) as a template was reported. The proposed sensor exhibited distinctive enantiospecific oxidation peaks toward the R-antipodes of four β-blocker representatives and additional oxidation peaks common to both enantiomers of each studied β-blocker, allowing thus the simultaneous analysis of all of their enantiomers in a single analysis. The specific preconditioning of the polymer by alternative exposure to aqueous and nonaqueous medium was proven to be essential for the chiral recognition ability of the obtained sensor. The rebinding property of the MIP film was studied by using a well-known redox probe, a change in the morphology and diffusive permeability of the thin polymeric layer in the presence of its template being observed. The applicability of the optimized analytical procedure was demonstrated by the analysis of ATNL's enantiomers in the range of 1.88 × 10-7-1.88 × 10-5 mol/L. The developed polymeric interface is the first reported transductor of a chiral electrochemical sensor able to exhibit simultaneous enantiospecificity toward several β-blocker representatives extensively used in the pharmaceutical and biomedical fields, offering good prospects in the simple, cost-effective, and fast assessment of their enantiomeric ratio and total concentration. [ABSTRACT FROM AUTHOR]

Although the human eye is an easily accessible sensory organ, it remains a challenge for drug administration due to the presence of several anatomical and physiological barriers which limit the access of drugs to its internal structures. Molecular imprinting technology may be considered the avant-garde approach in advanced drug delivery applications and, in particular, in ocular therapy. In fact, molecularly imprinted polymers hold the promise to compensate for the current shortcomings of the available arsenal of drug delivery systems intended for ocular therapy. The present manuscript aims to review the recent advances, the current challenges and most importantly to raise awareness on the underexplored potential and future perspectives of molecularly imprinted polymer-based drug delivery systems intended for the treatment of eye diseases. [ABSTRACT FROM AUTHOR]

An innovative sandwich MIP-based electrochemical sensor was fabricated for the fast and selective detection of adenosine. The covalent-imprinted biomimetic recognition element relies on two overlapping polymeric films, an underlaying composite boronate-affinity and poly(bithiophene)-structural layer and an overlaying poly(3-indolacetic acid) coating bearing carboxyl groups, intended to further shape the selectivity of the sensor towards adenosine. The sensor's behavior and analytical performance was characterized by cyclic voltammetry (CV), differential pulse voltammetry (DPV) and electrochemical impedance spectroscopy (EIS). The recorded DPVs showed a linear response to increasing concentration of adenosine in the range of 0.37 μM–37.4 μM with a limit of detection of 0.21 μM. The selectivity of the MIP sensor towards adenosine was demonstrated against more than 10 structurally related interferents. The developed sensor was applied for the fast and quantitative assessment of adenosine in spiked urine samples with good recoveries (102.98%–106.34%), proving at least comparable bioanalytical performances in terms of sensitivity, yet greatly improved in terms of selectivity and analysis time to previously reported sensors. • First study reporting MIP-based electrochemical sensor for adenosine determination. • Biomimetic sandwich-structured sensing interface for the detection of adenosine. • Dual imprinting process by spatially-oriented covalent and non-covalent interactions. • Facile manufacturing of multi-use electrochemical sensor offering short analysis times. • Very good selectivity demonstrated on many analytically relevant interferents. [ABSTRACT FROM AUTHOR]

A highly selective and sensitive molecularly imprinted polymer (MIP)-based electrochemical sensor was fabricated for the determination of azithromycin, a broad-spectrum macrolide antibiotic, from various biological samples (urine, tears, plasma). The reversible boronate ester bond-mediated, thin (~75 nm) MIP-based biomimetic recognition layer was electrodeposited in non-aqueous media onto the surface of a glassy carbon electrode (GCE). The surface morphology and the analytical performances of the developed sensor were assessed by scanning electron (SEM) and atomic force microscopy (AFM), electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). By employing an indirect electrochemical detection in the presence of 10 mM ferro/ferricyanide as redox probe, the sensor exhibited a very wide dynamic range (13.33 nM–66.67 μM), with an estimated detection limit in the subnanomolar range (0.85 nM azithromycin). The simple to construct sensor demonstrates reusability and good shelf-life, exhibiting remarkable selectivity over a wide number of structurally related and non-related antibiotics, commonly associated drugs and endogenous compounds. • Biomimetic recognition layer using cyclic boronate ester-based imprinted polymer. • Subnanomolar sensitivity, excellent selectivity due to covalent imprinting approach. • Facile manufacturing of multi-use electrochemical sensor with good shelf-life. • Very good recoveries of AZI from various spiked biological fluids. • The first study reporting AZI assessment from tears using an electrochemical sensor. [ABSTRACT FROM AUTHOR]