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Molecularly Imprinted Materials: New Vistas and Challenge

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

Deadline for manuscript submissions: closed (31 March 2023) | Viewed by 28020

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Prof. Dr. Jieping Fan

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Guest Editor

Department of Chemical Engineering, Nanchang University, Nanchang 330031, China
Interests: separation; natural products; molecularly imprinted materials; preparation; characteristics; molecular recognition; chemical engineering; analytical chemistry; functional polymers
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Ruixia Gao

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Guest Editor

School of Chemistry, Xi'an Jiaotong University, Xi'an 710049, China
Interests: magnetic separation; preparation; molecularly imprinted polymers; functional monomers; adsorption

Special Issue Information

Dear Colleagues,

Molecular imprinting is a powerful technology to create artificial receptors within polymer networks, mimicking natural antibodies. Molecularly imprinted materials have attracted considerable attention as separation materials because of their unique properties, such as the tailor-made recognition sites for target molecules, high affinity and selectivity, excellent stability, and easy preparation. Their ability to replace expensive and complex affinity materials has high potential in a wide range of areas, and very interesting materials have appeared in recent years.

The present Special Issue, “Molecularly Imprinted Materials: New Vistas and Challenge”, aims to assemble a diverse collection of articles describing innovative aspects of Molecularly imprinted materials synthesis and application. In particular, contributions are welcome on all aspects of molecularly imprinted materials development, for all kinds of applications, including synthesis, modeling, progress in analytical chemistry, preparation methods and characteristics for separation or analysis of natural products including proteins, polysaccharides, alkaloids, etc., (bio) sensors, nanotechnology, catalysis, molecularly imprinted materials development for bio-recognition, etc. This Special Issue will provide a collection of high-quality full research papers, communications, and critical reviews covering both applied and fundamental aspects of molecular imprinting technology.

Prof. Dr. Jieping Fan
Prof. Dr. Ruixia Gao
Guest Editors

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Keywords

molecularly imprinted materials
molecularly Imprinted Polymers (MIPs)
preparation
characteristics
separation
analysis
sensors
catalysis
molecular recognition
natural products

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Published Papers (9 papers)

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Research

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14 pages, 3163 KiB

Open AccessArticle

A Fluorescent Molecularly Imprinted Polymer-Coated Paper Sensor for On-Site and Rapid Detection of Glyphosate

by Meng Wang, Jun Qiu, Chennuo Zhu, Yunyan Hua, Jie Yu, Lulu Jia, Jianhong Xu, Jianlin Li and Qianjin Li

Molecules 2023, 28(5), 2398; https://doi.org/10.3390/molecules28052398 - 6 Mar 2023

Cited by 8 | Viewed by 2959

Abstract

Due to the massive use and abuse of pesticides, practices which have led to serious threats to human health, the research community must develop on-site and rapid detection technology of pesticide residues to ensure food safety. Here, a paper-based fluorescent sensor, integrated with molecularly imprinted polymer (MIP) targeting glyphosate, was prepared by a surface-imprinting strategy. The MIP was synthesized by a catalyst-free imprinting polymerization technique and exhibited highly selective recognition capability for glyphosate. The MIP-coated paper sensor not only remained selective, but also displayed a limit of detection of 0.29 µmol and a linear detection range from 0.5 to 10 µmol. Moreover, the detection time only took about 5 min, which is beneficial for rapid detection of glyphosate in food samples. The detection accuracy of such paper sensor was good, with a spiked recovery rate of 92–117% in real samples. The fluorescent MIP-coated paper sensor not only has good specificity, which is helpful to reduce the food matrix interference and shorten the sample pretreatment time, but it also has the merits of high stability, low-cost and ease of operation and carrying, displaying great potential for application in the on-site and rapid detection of glyphosate for food safety. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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12 pages, 3471 KiB

Open AccessArticle

Molecularly Imprinted Polymer Nanospheres with Hydrophilic Shells for Efficient Molecular Recognition of Heterocyclic Aromatic Amines in Aqueous Solution

by Peijian Sun, Yipeng Wang, Song Yang, Xuehui Sun, Bin Peng, Lining Pan, Yunzhen Jia, Xiaobing Zhang and Cong Nie

Molecules 2023, 28(5), 2052; https://doi.org/10.3390/molecules28052052 - 22 Feb 2023

Cited by 4 | Viewed by 1619

Abstract

Heterocyclic aromatic amine molecularly imprinted polymer nanospheres with surface-bound dithioester groups (haa-MIP) were firstly synthesized via reversible addition-fragmentation chain transfer (RAFT) precipitation polymerization. Then, a series of core-shell structural heterocyclic aromatic amine molecularly imprinted polymer nanospheres with hydrophilic shells (MIP-HSs) were subsequently prepared by grafting the hydrophilic shells on the surface of haa-MIP via on-particle RAFT polymerization of 2-hydroxyethyl methacrylate (HEMA), itaconic acid (IA), and diethylaminoethyl methacrylate (DEAEMA). The haa-MIP nanospheres showed high affinity and specific recognition toward harmine and its structural analogs in organic solution of acetonitrile, but lost the specific binding ability in aqueous solution. However, after the grafting of the hydrophilic shells on the haa-MIP particles, the surface hydrophilicity and water dispersion stability of the polymer particles of MIP-HSs greatly improved. The binding of harmine by MIP-HSs with hydrophilic shells in aqueous solutions is about two times higher than that of NIP-HSs, showing an efficient molecular recognition of heterocyclic aromatic amines in aqueous solution. The effect of hydrophilic shell structure on the molecular recognition property of MIP-HSs was further compared. MIP-PIA with carboxyl groups containing hydrophilic shells showed the highest selective molecular recognition ability to heterocyclic aromatic amines in aqueous solution. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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16 pages, 5044 KiB

Open AccessArticle

Composite Hydrogel Microspheres Encapsulating Hollow Mesoporous Imprinted Nanoparticles for Selective Capture and Separation of 2′-Deoxyadenosine

by Lu Liu, Mengdie Zhou and Jianming Pan

Molecules 2022, 27(21), 7444; https://doi.org/10.3390/molecules27217444 - 2 Nov 2022

Cited by 3 | Viewed by 2356

Abstract

Hollow mesoporous silica nanoparticles have been widely applied as a carrier material in the molecular imprinting process because of their excellent properties, with high specific surface area and well-defined active centers. However, these kinds of materials face the inevitable problem that they have low mass transfer efficiency and cannot be conveniently recycled. In order to solve this problem, this work has developed a composite hydrogel microsphere (MMHSG) encapsulated with hollow mesoporous imprinted nanoparticles for the selective extraction of 2’-deoxyadenosine (dA). Subsequently, the hollow mesoporous imprinted polymers using dA as template molecule and synthesized 5-(2-carbomethoxyvinyl)-2′-deoxyuridine (AcrU) as functional monomer were encapsulated in hydrogel. MMHSG displayed good performance in specifically recognizing and quickly separating dA, whereas no imprinting effect was observed among 2′-deoxyguanosine (dG), deoxycytidine (dC), or 5′-monophosphate disodium salt (AMP). Moreover, the adsorption of dA by MMHSG followed chemisorption and could reach adsorption equilibrium within 60 min; the saturation adsorption capacity was 20.22 μmol·g⁻¹. The introduction of AcrU could improve selectivity through base complementary pairing to greatly increase the imprinting factor to 3.79. Therefore, this was a successful attempt to combine a hydrogel with hollow mesoporous silica nanoparticles and molecularly imprinted material. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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19 pages, 7300 KiB

Open AccessArticle

Preparation and Characterization of Protein Molecularly Imprinted Poly (Ionic Liquid)/Calcium Alginate Composite Cryogel Membrane with High Mechanical Strength for the Separation of Bovine Serum Albumin

by Jie-Ping Fan, Wen-Ya Dong, Xue-Hong Zhang, Jia-Xin Yu, Cong-Bo Huang, Li-Juan Deng, Hui-Ping Chen and Hai-Long Peng

Molecules 2022, 27(21), 7304; https://doi.org/10.3390/molecules27217304 - 27 Oct 2022

Cited by 8 | Viewed by 1751

Abstract

In order to improve the mechanical strength and imprinting efficiency, a novel bovine serum albumin (BSA) molecularly imprinted poly(ionic liquid)/calcium alginate composite cryogel membrane (MICM) was prepared. The results of the tensile test indicated that the MICM had excellent mechanical strength which could reach up to 90.00 KPa, 30.30 times higher than the poly (ionic liquid) membrane without calcium alginate; the elongation of it could reach up to 93.70%, 8.28 times higher than the poly (ionic liquid) membrane without calcium alginate. The MICM had a very high welling ratio of 1026.56% and macropore porosity of 62.29%, which can provide effective mass transport of proteins. More remarkably, it had a very high adsorption capacity of 485.87 mg g⁻¹ at 20 °C and 0.66 mg mL⁻¹ of the initial concentration of BSA. Moreover, MICM also had good selective and competitive recognition toward BSA, exhibiting potential utility in protein separation. This work can provide a potential method to prepare the protein-imprinted cryogel membrane with both high mechanical strength and imprinting efficiency. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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Review

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16 pages, 2640 KiB

Open AccessReview

Nucleoside Analogs: A Review of Its Source and Separation Processes

by Pan Wang, Tao Cheng and Jianming Pan

Molecules 2023, 28(20), 7043; https://doi.org/10.3390/molecules28207043 - 12 Oct 2023

Cited by 2 | Viewed by 2726

Abstract

Nucleoside analogs play a crucial role in the production of high-value antitumor and antimicrobial drugs. Currently, nucleoside analogs are mainly obtained through nucleic acid degradation, chemical synthesis, and biotransformation. However, these methods face several challenges, such as low concentration of the main product, the presence of complex matrices, and the generation of numerous by-products that significantly limit the development of new drugs and their pharmacological studies. Therefore, this work aims to summarize the universal separation methods of nucleoside analogs, including crystallization, high-performance liquid chromatography (HPLC), column chromatography, solvent extraction, and adsorption. The review also explores the application of molecular imprinting techniques (MITs) in enhancing the identification of the separation process. It compares existing studies reported on adsorbents of molecularly imprinted polymers (MIPs) for the separation of nucleoside analogs. The development of new methods for selective separation and purification of nucleosides is vital to improving the efficiency and quality of nucleoside production. It enables us to obtain nucleoside products that are essential for the development of antitumor and antiviral drugs. Additionally, these methods possess immense potential in the prevention and control of serious diseases, offering significant economic, social, and scientific benefits to the fields of environment, biomedical research, and clinical therapeutics. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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33 pages, 5209 KiB

Open AccessReview

Molecularly Imprinted Nanomaterials with Stimuli Responsiveness for Applications in Biomedicine

by Yan Zhang, Qinghe Wang, Xiao Zhao, Yue Ma, Hongbo Zhang and Guoqing Pan

Molecules 2023, 28(3), 918; https://doi.org/10.3390/molecules28030918 - 17 Jan 2023

Cited by 22 | Viewed by 3836

Abstract

The review aims to summarize recent reports of stimuli-responsive nanomaterials based on molecularly imprinted polymers (MIPs) and discuss their applications in biomedicine. In the past few decades, MIPs have been proven to show widespread applications as new molecular recognition materials. The development of stimuli-responsive nanomaterials has successfully endowed MIPs with not only affinity properties comparable to those of natural antibodies but also the ability to respond to external stimuli (stimuli-responsive MIPs). In this review, we will discuss the synthesis of MIPs, the classification of stimuli-responsive MIP nanomaterials (MIP-NMs), their dynamic mechanisms, and their applications in biomedicine, including bioanalysis and diagnosis, biological imaging, drug delivery, disease intervention, and others. This review mainly focuses on studies of smart MIP-NMs with biomedical perspectives after 2015. We believe that this review will be helpful for the further exploration of stimuli-responsive MIP-NMs and contribute to expanding their practical applications especially in biomedicine in the near future. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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26 pages, 2962 KiB

Open AccessReview

Recent Advances in Molecularly Imprinted Polymers for Antibiotic Analysis

by Guangli Zhao, Yue Zhang, Dani Sun, Shili Yan, Yuhao Wen, Yixiao Wang, Guisheng Li, Huitao Liu, Jinhua Li and Zhihua Song

Molecules 2023, 28(1), 335; https://doi.org/10.3390/molecules28010335 - 1 Jan 2023

Cited by 35 | Viewed by 4763

Abstract

The abuse and residues of antibiotics have a great impact on the environment and organisms, and their determination has become very important. Due to their low contents, varieties and complex matrices, effective recognition, separation and enrichment are usually required prior to determination. Molecularly imprinted polymers (MIPs), a kind of highly selective polymer prepared via molecular imprinting technology (MIT), are used widely in the analytical detection of antibiotics, as adsorbents of solid-phase extraction (SPE) and as recognition elements of sensors. Herein, recent advances in MIPs for antibiotic residue analysis are reviewed. Firstly, several new preparation techniques of MIPs for detecting antibiotics are briefly introduced, including surface imprinting, nanoimprinting, living/controlled radical polymerization, and multi-template imprinting, multi-functional monomer imprinting and dummy template imprinting. Secondly, several SPE modes based on MIPs are summarized, namely packed SPE, magnetic SPE, dispersive SPE, matrix solid-phase dispersive extraction, solid-phase microextraction, stir-bar sorptive extraction and pipette-tip SPE. Thirdly, the basic principles of MIP-based sensors and three sensing modes, including electrochemical sensing, optical sensing and mass sensing, are also outlined. Fourthly, the research progress on molecularly imprinted SPEs (MISPEs) and MIP-based electrochemical/optical/mass sensors for the detection of various antibiotic residues in environmental and food samples since 2018 are comprehensively reviewed, including sulfonamides, quinolones, β-lactams and so on. Finally, the preparation and application prospects of MIPs for detecting antibiotics are outlined. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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25 pages, 3112 KiB

Open AccessReview

Applications of Molecular Imprinting Technology in the Study of Traditional Chinese Medicine

by Yue Zhang, Guangli Zhao, Kaiying Han, Dani Sun, Na Zhou, Zhihua Song, Huitao Liu, Jinhua Li and Guisheng Li

Molecules 2023, 28(1), 301; https://doi.org/10.3390/molecules28010301 - 30 Dec 2022

Cited by 17 | Viewed by 3798

Abstract

Traditional Chinese medicine (TCM) is one of the most internationally competitive industries. In the context of TCM modernization and internationalization, TCM-related research studies have entered a fast track of development. At the same time, research of TCM is also faced with challenges, such as matrix complexity, component diversity and low level of active components. As an interdisciplinary technology, molecular imprinting technology (MIT) has gained popularity in TCM study, owing to the produced molecularly imprinted polymers (MIPs) possessing the unique features of structure predictability, recognition specificity and application universality, as well as physical robustness, thermal stability, low cost and easy preparation. Herein, we comprehensively review the recent advances of MIT for TCM studies since 2017, focusing on two main aspects including extraction/separation and purification and detection of active components, and identification analysis of hazardous components. The fundamentals of MIT are briefly outlined and emerging preparation techniques for MIPs applied in TCM are highlighted, such as surface imprinting, nanoimprinting and multitemplate and multifunctional monomer imprinting. Then, applications of MIPs in common active components research including flavonoids, alkaloids, terpenoids, glycosides and polyphenols, etc. are respectively summarized, followed by screening and enantioseparation. Related identification detection of hazardous components from TCM itself, illegal addition, or pollution residues (e.g., heavy metals, pesticides) are discussed. Moreover, the applications of MIT in new formulation of TCM, chiral drug resolution and detection of growing environment are summarized. Finally, we propose some issues still to be solved and future research directions to be expected of MIT for TCM studies. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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18 pages, 2631 KiB

Open AccessReview

Preparation and Application of Molecularly Imprinted Polymers for Flavonoids: Review and Perspective

by Yurou Yang and Xiantao Shen

Molecules 2022, 27(21), 7355; https://doi.org/10.3390/molecules27217355 - 29 Oct 2022

Cited by 22 | Viewed by 3410

Abstract

The separation and detection of flavonoids from various natural products have attracted increasing attention in the field of natural product research and development. Depending on the high specificity of molecularly imprinted polymers (MIPs), MIPs are proposed as efficient adsorbents for the selective extraction and separation of flavonoids from complex samples. At present, a comprehensive review article to summarize the separation and purification of flavonoids using molecular imprinting, and the employment of MIP-based sensors for the detection of flavonoids is still lacking. Here, we reviewed the general preparation methods of MIPs towards flavonoids, including bulk polymerization, precipitation polymerization, surface imprinting and emulsion polymerization. Additionally, a variety of applications of MIPs towards flavonoids are summarized, such as the different forms of MIP-based solid phase extraction (SPE) for the separation of flavonoids, and the MIP-based sensors for the detection of flavonoids. Finally, we discussed the advantages and disadvantages of the current synthetic methods for preparing MIPs of flavonoids and prospected the approaches for detecting flavonoids in the future. The purpose of this review is to provide helpful suggestions for the novel preparation methods of MIPs for the extraction of flavonoids and emerging applications of MIPs for the detection of flavonoids from natural products and biological samples. Full article

(This article belongs to the Special Issue Molecularly Imprinted Materials: New Vistas and Challenge)

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