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Design of Functional Polymer Materials for Drug Controlled Release

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Special Issue Information
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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Macromolecular Chemistry".

Deadline for manuscript submissions: closed (31 December 2022) | Viewed by 19740

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Special Issue Editor

Prof. Dr. Hua Wei

E-Mail Website1 Website2
Guest Editor

1. Hunan Province Cooperative Innovation Center for Molecular Target New Drug Study, School of Pharmaceutical Science, University of South China, Hengyang 421001, China
2. State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, and College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China
Interests: polymer chemistry; cyclic polymer; controlled drug release; gene delivery; tissue engineering

Special Issue Information

Dear Colleagues,

Design of functional polymeric materials via the modulation of stimuli-responsiveness and polymer topology has enabled rapid development of various advanced polymeric materials with better properties and improved performance for controlled drug release applications.

Stimuli-responsive polymers capable of responding to the various bio-relevant triggers, such as the pH gradients between the extracellular pH of a normal tissue and the pH of a diseased site, a slight elevation of the localized temperature from the normal physiological value to a hyperthermia one, and the reducing or oxidizing microenvironment, can provide an elegant solution to the sufficient extracellular stability vs. intracellular destabilization dilemma of the delivery vehicles for enhanced therapeutic efficiency.

Meanwhile, polymers with advanced topologies, including comb-like, star-shaped, dendrimer-like, hyperbranched, and cyclic-derived structures, have endowed polymers with unique properties that are inaccessible through the use of conventional linear analogues. The reported better performance resulting from the advanced topological structures for biomedical applications lies in the improved drug loading capacity, extended circulation time and greater cellular uptake, and enhanced therapeutic efficiency.

Considering the tremendous progresses made in these research fields, Molecules is launching a Special Issue with an aim to highlight the most exciting work in the design of functional polymer materials for drug controlled release. Topics covered in this Special Issue include, but are not exclusively limited to, the following: stimuli-responsive polymers; polymers with advanced topologies; polymers based on natural and renewable resources; degradable polymers; polymer conjugates; polymeric drugs; biomacromolecular assembly; original polymer design and synthesis for diverse biomedical applications such as immunotherapy, drug delivery, gene delivery, antimicrobial applications, diagnostic imaging, and biosensing; polymers in tissue engineering and regenerative medicine; polymeric scaffolds; and hydrogels for cell culture and delivery. Research papers and up-to-date review articles are all welcome.

The official deadline for submission is 15 October 2021. We look forward to your contribution to this Special Issue in Molecules.

Prof. Dr. Hua Wei
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

Controlled drug release
Stimuli-responsive polymers
Polymer topology
Macromolecular engineering
Polymer chemistry

Published Papers (5 papers)

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Research

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17 pages, 3215 KiB

Open AccessArticle

Gold/Pentablock Terpolymer Hybrid Multifunctional Nanocarriers for Controlled Delivery of Tamoxifen: Effect of Nanostructure on Release Kinetics

by Maria-Teodora Popescu and Constantinos Tsitsilianis

Molecules 2022, 27(12), 3764; https://doi.org/10.3390/molecules27123764 - 11 Jun 2022

Cited by 2 | Viewed by 1131

Abstract

Here, we describe the preparation and characterization of organic/inorganic hybrid polymer multifunctional nanocarriers. Novel nanocomposites of gold nanoparticles using pH-responsive coordination pentablock terpolymers of poly(ε-caprolactone)-b-poly(ethylene oxide)-b-poly(2-vinylpyridine)-b-poly(ethylene oxide)-b-poly(ε-caprolactone), bearing or not bearing partially quaternized vinylpyridine moieties, were studied. The template morphology of the coordination pentablock terpolymer at physiological pH ranges from crew-cut to multicompartmentalized micelles which can be tuned by chemical modification of the central block. Additionally, the presence of 2VP groups allows the coordination of gold ions, which can be reduced in situ to construct gold@polymer nanohybrids. Furthermore, the possibility of tuning the gold distribution in the micelles, through partial quaternization of the central P2VP block, was also investigated. Various morphological gold colloidal nanoparticles such as gold@core-corona nanoparticles and gold@core-gold@corona nanoparticles were synthesized on the corresponding template of the pentablock terpolymer, first by coordination with gold ions, followed by reduction with NaBH₄. The pentablock and gold@pentablock nanoparticles could sparingly accommodate a water-soluble drug, Tamoxifen (TAX), in their hydrophobic micellar cores. The nanostructure of the nanocarrier remarkably affects the TAX delivery kinetics. Importantly, the hybrid gold@polymer nanoparticles showed prolonged release profiles for the guest molecule, relative to the corresponding bare amphiphilic pentablock polymeric micelles. These Gold@pentablock terpolymer hybrid nanoparticles could act as a multifunctional theranostic nanoplatform, integrating sustainable pH-controlled drug delivery, diagnostic function and photothermal therapy. Full article

(This article belongs to the Special Issue Design of Functional Polymer Materials for Drug Controlled Release)

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23 pages, 5419 KiB

Open AccessArticle

Construction of Enzyme-Responsive Micelles Based on Theranostic Zwitterionic Conjugated Bottlebrush Copolymers with Brush-on-Brush Architecture for Cell Imaging and Anticancer Drug Delivery

by Fangjun Liu, Dun Wang, Jiaqi Wang, Liwei Ma, Cuiyun Yu and Hua Wei

Molecules 2022, 27(9), 3016; https://doi.org/10.3390/molecules27093016 - 07 May 2022

Cited by 4 | Viewed by 2217

Abstract

Bottlebrush copolymers with different chemical structures and compositions as well as diverse architectures represent an important kind of material for various applications, such as biomedical devices. To our knowledge, zwitterionic conjugated bottlebrush copolymers integrating fluorescence imaging and tumor microenvironment-specific responsiveness for efficient intracellular drug release have been rarely reported, likely because of the lack of an efficient synthetic approach. For this purpose, in this study, we reported the successful preparation of well-defined theranostic zwitterionic bottlebrush copolymers with unique brush-on-brush architecture. Specifically, the bottlebrush copolymers were composed of a fluorescent backbone of polyfluorene derivate (PFONPN) possessing the fluorescence resonance energy transfer with doxorubicin (DOX), primary brushes of poly(2-hydroxyethyl methacrylate) (PHEMA), and secondary graft brushes of an enzyme-degradable polytyrosine (PTyr) block as well as a zwitterionic poly(oligo (ethylene glycol) monomethyl ether methacrylate-co-sulfobetaine methacrylate) (P(OEGMA-co-SBMA)) chain with super hydrophilicity and highly antifouling ability via elegant integration of Suzuki coupling, NCA ROP and ATRP techniques. Notably, the resulting bottlebrush copolymer, PFONPN₉-g-(PHEMA₁₅-g-(PTyr₁₆-b-P(OEGMA₆-co-SBMA₆)₂)) (P₂) with a lower MW ratio of the hydrophobic side chains of PTyr and hydrophilic side chains of P(OEGMA-co-SBMA) could self-assemble into stabilized unimolecular micelles in an aqueous phase. The resulting unimolecular micelles showed a fluorescence quantum yield of 3.9% that is mainly affected by the pendant phenol groups of PTyr side chains and a drug-loading content (DLC) of approximately 15.4% and entrapment efficiency (EE) of 90.6% for DOX, higher than the other micelle analogs, because of the efficient supramolecular interactions of π–π stacking between the PTyr blocks and drug molecules, as well as the moderate hydrophilic chain length. The fluorescence of the PFONPN backbone enables fluorescence resonance energy transfer (FRET) with DOX and visualization of intracellular trafficking of the theranostic micelles. Most importantly, the drug-loaded micelles showed accelerated drug release in the presence of proteinase K because of the enzyme-triggered degradation of PTyr blocks and subsequent deshielding of P(OEGMA-co-SBMA) corona for micelle destruction. Taken together, we developed an efficient approach for the synthesis of enzyme-responsive theranostic zwitterionic conjugated bottlebrush copolymers with a brush-on-brush architecture, and the resulting theranostic micelles with high DLC and tumor microenvironment-specific responsiveness represent a novel nanoplatform for simultaneous cell image and drug delivery. Full article

(This article belongs to the Special Issue Design of Functional Polymer Materials for Drug Controlled Release)

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23 pages, 3757 KiB

Open AccessArticle

Chitosan, Polyethylene Glycol and Polyvinyl Alcohol Modified MgFe₂O₄ Ferrite Magnetic Nanoparticles in Doxorubicin Delivery: A Comparative Study In Vitro

by Deevak Ramnandan, Seipati Mokhosi, Aliscia Daniels and Moganavelli Singh

Molecules 2021, 26(13), 3893; https://doi.org/10.3390/molecules26133893 - 25 Jun 2021

Cited by 32 | Viewed by 4385

Abstract

Cancer-based magnetic theranostics has gained significant interest in recent years and can contribute as an influential archetype in the effective treatment of cancer. Owing to their excellent biocompatibility, minute sizes and reactive functional surface groups, magnetic nanoparticles (MNPs) are being explored as potential drug delivery systems. In this study, MgFe₂O₄ ferrite MNPs were evaluated for their potential to augment the delivery of the anticancer drug doxorubicin (DOX). These MNPs were successfully synthesized by the glycol-thermal method and functionalized with the polymers; chitosan (CHI), polyvinyl alcohol (PVA) and polyethylene glycol (PEG), respectively, as confirmed by Fourier transform infrared (FTIR) spectroscopy. X-ray diffraction (XRD) confirmed the formation of the single-phase cubic spinel structures while vibrating sample magnetometer (VSM) analysis confirmed the superparamagnetic properties of all MNPs. Transmission electron microscopy (TEM) and nanoparticle tracking analysis (NTA) revealed small, compact structures with good colloidal stability. CHI-MNPs had the highest DOX encapsulation (84.28%), with the PVA-MNPs recording the lowest encapsulation efficiency (59.49%). The 3-(4,5-dimethylthiazol-2-yl)-2,5 diphenyl tetrazolium bromide (MTT) cytotoxicity assays conducted in the human embryonic kidney (HEK293), colorectal adenocarcinoma (Caco-2), and breast adenocarcinoma (SKBR-3) cell lines showed that all the drug-free polymerized MNPs promoted cell survival, while the DOX loaded MNPs significantly reduced cell viability in a dose-dependent manner. The DOX-CHI-MNPs possessed superior anticancer activity (<40% cell viability), with approximately 85.86% of the drug released after 72 h in a pH-responsive manner. These MNPs have shown good potential in enhancing drug delivery, thus warranting further optimizations and investigations. Full article

(This article belongs to the Special Issue Design of Functional Polymer Materials for Drug Controlled Release)

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Review

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0 pages, 2097 KiB

Open AccessReview

Advances on Delivery of Cytotoxic Enzymes as Anticancer Agents

by Akmal M. Asrorov, Bahtiyor Muhitdinov, Bin Tu, Sharafitdin Mirzaakhmedov, Huiyuan Wang and Yongzhuo Huang

Molecules 2022, 27(12), 3836; https://doi.org/10.3390/molecules27123836 - 14 Jun 2022

Cited by 4 | Viewed by 2880

Abstract

Cancer is one of the most serious human diseases, causing millions of deaths worldwide annually, and, therefore, it is one of the most investigated research disciplines. Developing efficient anticancer tools includes studying the effects of different natural enzymes of plant and microbial origin on tumor cells. The development of various smart delivery systems based on enzyme drugs has been conducted for more than two decades. Some of these delivery systems have been developed to the point that they have reached clinical stages, and a few have even found application in selected cancer treatments. Various biological, chemical, and physical approaches have been utilized to enhance their efficiencies by improving their delivery and targeting. In this paper, we review advanced delivery systems for enzyme drugs for use in cancer therapy. Their structure-based functions, mechanisms of action, fused forms with other peptides in terms of targeting and penetration, and other main results from in vivo and clinical studies of these advanced delivery systems are highlighted. Full article

(This article belongs to the Special Issue Design of Functional Polymer Materials for Drug Controlled Release)

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23 pages, 9218 KiB

Open AccessReview

Polymeric Drug Delivery System Based on Pluronics for Cancer Treatment

by Jialin Yu, Huayu Qiu, Shouchun Yin, Hebin Wang and Yang Li

Molecules 2021, 26(12), 3610; https://doi.org/10.3390/molecules26123610 - 12 Jun 2021

Cited by 53 | Viewed by 8307

Abstract

Pluronic polymers (pluronics) are a unique class of synthetic triblock copolymers containing hydrophobic polypropylene oxide (PPO) and hydrophilic polyethylene oxide (PEO) arranged in the PEO-PPO-PEO manner. Due to their excellent biocompatibility and amphiphilic properties, pluronics are an ideal and promising biological material, which is widely used in drug delivery, disease diagnosis, and treatment, among other applications. Through self-assembly or in combination with other materials, pluronics can form nano carriers with different morphologies, representing a kind of multifunctional pharmaceutical excipients. In recent years, the utilization of pluronic-based multi-functional drug carriers in tumor treatment has become widespread, and various responsive drug carriers are designed according to the characteristics of the tumor microenvironment, resulting in major progress in tumor therapy. This review introduces the specific role of pluronic-based polymer drug delivery systems in tumor therapy, focusing on their physical and chemical properties as well as the design aspects of pluronic polymers. Finally, using newer literature reports, this review provides insights into the future potential and challenges posed by different pluronic-based polymer drug delivery systems in tumor therapy. Full article

(This article belongs to the Special Issue Design of Functional Polymer Materials for Drug Controlled Release)

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