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Polymers for Controlled Drug Release

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A topical collection in Polymers (ISSN 2073-4360). This collection belongs to the section "Polymer Applications".

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Editors

Prof. Dr. Alexey L. Iordanskii

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Collection Editor

N. N. Semenov Federal Research Center for Chemical Physics Academy of Science, 119991 Moscow, Russia
Interests: biodegradable polymers; transport phenomena; electrospun fibers; controlled release; polymer blends; composites; water in macromolecular systems; sorption; gas permeability
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Prof. Dr. Sabu Thomas

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Collection Editor

Vice Chancellor, Mahatma Gandhi University, Priyadarshini Hills, Kottayam 686 560, Kerala, India
Interests: nanomaterials; polymer blends; fiber-filled polymer composites; polymer nanocomposites; aging and degradation; pervaporation phenomena; sorption and diffusion; interpenetrating polymer systems; recyclability and reuse of waste plastics and rubbers; elastomer crosslinking; dual porous nanocomposite scaffolds for tissue engineering; polymer nanocomposites for electronic applications; water purification; energy storage
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Dear Colleagues,

Academic and industrial engagement has currently been directed to a required growth in the human lifespan and life quality that is supported by advances in biomedicine, environmental protection, packaging upgrading, etc. The holistic approach to the healthcare therapeutic strategy, innovative packaging development, and eco-friendly material design is based on the creation of conditions for bioactive component release/delivery specifically for drugs in medicine, food-modifying agents in packaging, and pheromones and insecticides in agriculture, correspondingly. Because of the wide implementation of controlled release as the specific phenomenon, it is critical to clearly establish its mechanism and kinetic profile as well as market economic consequences of replacement of traditional medical and packaging formulations by modern polymeric systems, ensuring the prolonged and programmed delivery of bioactive agents.

A series of significant contemplations are outlined in this Collection to establish spatial–temporary patterns for bioactive entities loaded in polymer vehicles of synthetic and bio-based origin. In a release systems design, one of the most important unit operations is the size reduction to the nanoscale and molecular levels. In biomedicine, the final object of drug-controlled delivery application comprises a spatial–temporary pattern setting to carry out the most favorable treatment of patients. Novel miniature therapeutic systems with drug targeting characteristics have irrefutable advantages such as enhanced bioavailability, reduced toxicity, tailored release profiles, improved stability, and others, which take precedence over regular dosage forms. The variety of geometrical forms for polymer therapeutic systems at the submicron levels, namely, spheres, Janus particles, ellipsoid-like beds, rods, ribbon and cylindrical fibers, slabs, and the like, creates a great opportunity to set up original kinetic release profiles combined with improved bio-accessibility for cells and tissues. The next step after nanotechnology engineering includes the principles of polymer science, which coherently seek a relationship between structure–morphology polymer features and drug diffusion transport characteristics. Modeling and experimental studies of transport phenomena should assist the development of next-generation drug release therapeutic systems.

In this collection, it is our aim to provide Polymers MDPI readers with the latest developments in the design, characterization, and applications of controlled release systems with different composition and geometry.

Topics include but are not limited to the following list:

The fundamental principles and breakthrough innovations of controlled release/delivery as the specific phenomenon occurring in stable (petrol-based) and biodegradable (bio-based) polymers;
Micro engineering and nanotechnology of polymeric systems procuring the controlled release;
Elaboration of controlled release micro- and nano-arrays with diverse geometry such as embedded dots, conjugated dendrimers, loaded particles, fibers, slabs;
Structure–morphology peculiarities of homogeneous, heterogeneous, and multilayered polymer composites as the factor of release profile regulation;
The impact of the balance of hydrophilicity–hydrophobicity on the mechanism of controlled release for drugs and polymer matrices, and the problem of poor-dissolved drugs with low-dosage activity;
Specific performance of drug-controlled release systems for gels, elastic, and glassy-state polymer constructs for vehicles performing in different areas of medicine, namely, in ophthalmology, reconstructive surgery, cardiovascular therapy; social and orphan decease treatment, dentistry, neurology, and others;
Controlled release for tissue engineering, growth factor delivery from ultrathin fibers;
Controlled release for food packaging as the fundament of active packaging development;
Controlled release for environmentally benign areas;
Modeling and computer data operations to create novel polymer release systems with bioactive agent temporal–spatial patterning in the human body, active barrier polymers, and the environment.

Prof. Dr. Alexey Iordanskii
Prof. Dr. Sabu Thomas
Collection Editors

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Published Papers (9 papers)

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2024

Jump to: 2023, 2022, 2021, 2020

17 pages, 6852 KiB

Open AccessArticle

Chitosan Nanoparticles Embedded in In Situ Gel for Nasal Delivery of Imipramine Hydrochloride: Short-Term Stage Development and Controlled Release Evaluation

by Samer Adwan, Teiba Obeidi and Faisal Al-Akayleh

Polymers 2024, 16(21), 3062; https://doi.org/10.3390/polym16213062 - 30 Oct 2024

Viewed by 740

Abstract

Imipramine hydrochloride (IMP), a tricyclic antidepressant used for major depression, enuresis, and neuropathic pain, is limited by gastrointestinal complications, low oral bioavailability (44%), and complex dosing requirements. This study aimed to explore a novel non-invasive nasal delivery system using chitosan nanoparticles (Cs NPs) embedded in an in situ gel to address the limitations of oral IMP administration. Cs NPs loaded with IMP were synthesized via ionic gelation and assessed for precision in drug concentration using a validated HPLC method. The particles were integrated into a thermoresponsive polymer, Pluronic F127, to form an in situ gel suitable for nasal administration. The formulation was characterized for gelation temperature, duration, viscosity, mucoadhesive strength, and overall gel robustness. Drug release kinetics and the controlled release mechanism were studied using ex vivo permeation tests with Franz diffusion cells and nasal sheep mucosa. The optimized nanoparticle formulation (F4-50) exhibited a consistent PS of 141.7 ± 2.2 nm, a zeta potential (ZP) of 16.79 ± 2.1 mV, and a high encapsulation efficiency of 67.71 ± 1.9%. The selected in situ gel formulation, F4-50-P1, demonstrated a gelation temperature of 33.6 ± 0.94 °C and a rapid gelation time of 48.1 ± 0.7 s. Transform-attenuated total reflectance infrared spectroscopy (ATR-IR) confirmed the compatibility and effective encapsulation of IMP within the formulation. The release profile of F4-50 included an initial burst release followed by a sustained release phase, with F4-50-P1 showing improved control over the burst release. The flux rates were 0.50 ± 0.01 mg/cm²/h for F4-50 and 0.33 ± 0.06 mg/cm²/h for F4-50-P1, indicating effective permeation. The developed chitosan nanoparticle-based in situ gel formulation provides a promising approach for the controlled release of IMP, enhancing therapeutic efficacy and patient compliance while mitigating the disadvantages associated with oral delivery. Full article

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19 pages, 5211 KiB

Open AccessArticle

Electrospun Polylactide—Poly(ε-Caprolactone) Fibers: Structure Characterization and Segmental Dynamic Response

by Svetlana G. Karpova, Anatoly A. Olkhov, Ivetta A. Varyan, Oksana I. Khan, Andrey A. Botin, Anna V. Naletova, Anatoly A. Popov and Alexey L. Iordanskii

Polymers 2024, 16(10), 1307; https://doi.org/10.3390/polym16101307 - 7 May 2024

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Abstract

Electrospun ultrathin fibers based on binary compositions of polylactide (PLA) and poly(ε-caprolactone) (PCL) with the various content from the polymer ratio from 0/100 to 100/0 have been explored. Combining thermal (DSC) and spectropy (ESR) techniques, the effect of biopolymer content on the characteristics of the crystal structure of PLA and PCL and the rotative diffusion of the stable TEMPO radical in the intercrystallite areas of PLA/PCL compositions was shown. It was revealed that after PLA and PCL blending, significant changes in the degree of crystallinity of PLA, PCL segment mobility, sorption of the Tempo probe, as well as its activation energy of rotation in the intercrystalline areas of PLA/PCL fibers, were evaluated. The characteristic region of biopolymers’ composition from 50/50 to 30/70% PLA/PCL blend ratio was found, where the inversion transition of PLA from dispersive medium to dispersive phase where an inversion transition is assumed when the continuous medium of the PLA transforms into a discrete phase. The performed studies made it possible, firstly, to carry out a detailed study of the effect of the system component ratio on the structural and dynamic characteristics of the PLA/PCL film material at the molecular level. Full article

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2023

Jump to: 2024, 2022, 2021, 2020

44 pages, 12474 KiB

Open AccessReview

Recent Advances in Nanoparticle Development for Drug Delivery: A Comprehensive Review of Polycaprolactone-Based Multi-Arm Architectures

by Ridouan El Yousfi, Mohamed Brahmi, Mohammed Dalli, Nafea Achalhi, Omar Azougagh, Abdesselam Tahani, Rachid Touzani and Abderrahmane El Idrissi

Polymers 2023, 15(8), 1835; https://doi.org/10.3390/polym15081835 - 10 Apr 2023

Cited by 15 | Viewed by 3399

Abstract

Controlled drug delivery is a crucial area of study for improving the targeted availability of drugs; several polymer systems have been applied for the formulation of drug delivery vehicles, including linear amphiphilic block copolymers, but with some limitations manifested in their ability to form only nanoaggregates such as polymersomes or vesicles within a narrow range of hydrophobic/hydrophilic balance, which can be problematic. For this, multi-arm architecture has emerged as an efficient alternative that overcame these challenges, with many interesting advantages such as reducing critical micellar concentrations, producing smaller particles, allowing for various functional compositions, and ensuring prolonged and continuous drug release. This review focuses on examining the key variables that influence the customization of multi-arm architecture assemblies based on polycaprolactone and their impact on drug loading and delivery. Specifically, this study focuses on the investigation of the structure–property relationships in these formulations, including the thermal properties presented by this architecture. Furthermore, this work will emphasize the importance of the type of architecture, chain topology, self-assembly parameters, and comparison between multi-arm structures and linear counterparts in relation to their impact on their performance as nanocarriers. By understanding these relationships, more effective multi-arm polymers can be designed with appropriate characteristics for their intended applications. Full article

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2022

Jump to: 2024, 2023, 2021, 2020

16 pages, 2976 KiB

Open AccessArticle

L-Arginine-Derived Polyamidoamine Oligomers Bearing at Both Ends β-Cyclodextrin Units as pH-Sensitive Curcumin Carriers

by Sofia Treccani, Jenny Alongi, Amedea Manfredi, Paolo Ferruti, Roberta Cavalli, Giuseppina Raffaini and Elisabetta Ranucci

Polymers 2022, 14(15), 3193; https://doi.org/10.3390/polym14153193 - 5 Aug 2022

Cited by 10 | Viewed by 2111

Abstract

The aza-Michael polyaddition of L-arginine and N,N′-methylene-bis-acrylamide gives the biocompatible and easily cell-internalized polyamidoamine ARGO7. By controlled synthesis, two ARGO7 oligomers, namely a trimer and a pentamer, bearing acrylamide terminal units, were obtained as precursors of the β-cyclodextrin-end-terminated oligomers P3 and P5, which have been shown to encapsulate curcumin at both pH 7.4 and 4.5. After lyophilization, P3- and P5-curcumin complexes gave stable water solutions. The apparent solubility of encapsulated curcumin was in the range 20–51 μg mL⁻¹, that is, three orders of magnitude higher than the water solubility of free curcumin (0.011 μg mL⁻¹). The drug release profiles showed induction periods both at pH levels 4.5 and 7.4, suggesting a diffusive release mechanism, as confirmed by kinetic studies. The release rate of curcumin was higher at pH 7.4 than at pH 4.5 and, in both cases, it was higher for the P5 complex. Encapsulated curcumin was more photostable than the free drug. Molecular mechanics and molecular dynamics simulations explain at atomistic level the formation of aggregates due to favorable van der Waals interactions. The drug molecules interact with the external surface of carriers or form inclusion complexes with the β-cyclodextrin cavities. The aggregate stability is higher at pH 4.5. Full article

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19 pages, 7350 KiB

Open AccessArticle

Development of Statistically Optimized Chemically Cross-Linked Hydrogel for the Sustained-Release Delivery of Favipiravir

by Ahmad Salawi, Arooj Khan, Muhammad Zaman, Tehseen Riaz, Hafsa Ihsan, Muhammad Hammad Butt, Waqar Aman, Rahima Khan, Imtiaz Majeed, Yosif Almoshari and Meshal Alshamrani

Polymers 2022, 14(12), 2369; https://doi.org/10.3390/polym14122369 - 11 Jun 2022

Cited by 15 | Viewed by 2438

Abstract

Nowadays, the use of statistical approaches, i.e., Box–Bhenken designs, are becoming very effective for developing and optimizing pharmaceutical drug formulations. In the current work, a Box–Bhenken design was employed using Design Expert version 11 to develop, evaluate, and optimize a hydrogel-based formulation for sustained release of an antiviral drug, i.e., favipiravir. The hydrogels were prepared using the free radical polymerization technique. β-Cyclodextrin (β-CD), N,N′-methylenebisacrylamide (MBA), acrylic acid (AA), and potassium per sulfate (KPS) were used as oligomer, crosslinker, monomer, and initiator, respectively. Three variables, including β-CD (X₁), MBA (X₂), and AA (X₃) were used at various concentrations for the preparation of hydrogels, followed by evaluation of a sol–gel fraction, swelling, porosity, chemical compatibilities, in vitro drug release, and entrapment efficiency. The results of the studies revealed that the degree of swelling was pH dependent, the best swelling being at pH 7.2 (1976%). On the other hand, for the low sol fraction of 0.2%, the reasonable porosity made the hydrogel capable of loading 99% favipiravir, despite its hydrophobic nature. The maximum entrapment efficiency (99%) was observed in optimized hydrogel formulation (F15). Similarly, in vitro drug release studies showed that the prepared hydrogels exhibited a good, sustained release effect till the 24th hour. The kinetic modelling of drug release data revealed that the Korsmeyer–Peppas model was best fit model, describing a diffusion type of drug release from the prepared hydrogels. Conclusively, the outcomes predict that the hydrogel-based system could be a good choice for developing a sustained-release, once-daily dosage form of favipiravir for improved patient compliance. Full article

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2021

Jump to: 2024, 2023, 2022, 2020

15 pages, 1620 KiB

Open AccessArticle

Aggressive Impacts Affecting the Biodegradable Ultrathin Fibers Based on Poly(3-Hydroxybutyrate), Polylactide and Their Blends: Water Sorption, Hydrolysis and Ozonolysis

by Anatoly A. Olkhov, Polina M. Tyubaeva, Alexandre A. Vetcher, Svetlana G. Karpova, Alexander S. Kurnosov, Svetlana Z. Rogovina, Alexey L. Iordanskii and Alexander A. Berlin

Polymers 2021, 13(6), 941; https://doi.org/10.3390/polym13060941 - 18 Mar 2021

Cited by 9 | Viewed by 2977

Abstract

Ultrathin electrospun fibers of pristine biopolyesters, poly(3-hydroxybutyrate) (PHB) and polylactic acid (PLA), as well as their blends, have been obtained and then explored after exposure to hydrolytic (phosphate buffer) and oxidative (ozone) media. All the fibers were obtained from a co-solvent, chloroform, by solution-mode electrospinning. The structure, morphology, and segmental dynamic behavior of the fibers have been determined by optical microscopy, SEM, ESR, and others. The isotherms of water absorption have been obtained and the deviation from linearity (the Henry low) was analyzed by the simplified model. For PHB-PLA fibers, the loss weight increments as the reaction on hydrolysis are symbate to water absorption capacity. It was shown that the ozonolysis of blend fibrils has a two-stage character which is typical for O₃ consumption, namely, the pendant group’s oxidation and the autodegradation of polymer molecules with chain rupturing. The first stage of ozonolysis has a quasi-zero-order reaction. A subsequent second reaction stage comprising the back-bone destruction has a reaction order that differs from the zero order. The fibrous blend PLA/PHB ratio affects the rate of hydrolysis and ozonolysis so that the fibers with prevalent content of PLA display poor resistance to degradation in aqueous and gaseous media. Full article

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11 pages, 9829 KiB

Open AccessArticle

Particle and Gel Characterization of Irinotecan-Loaded Double-Reverse Thermosensitive Hydrogel

by Fakhar ud Din, Sung Giu Jin and Han-Gon Choi

Polymers 2021, 13(4), 551; https://doi.org/10.3390/polym13040551 - 13 Feb 2021

Cited by 33 | Viewed by 3262

Abstract

The irinotecan-loaded double-reverse thermosensitive hydrogel (DRTH) is a dispersed system of irinotecan-loaded solid lipid nanoparticles (SLN) in a thermosensitive hydrogel. To optimise the particle and gel properties of DRTHs for rectal administration of irinotecan, SLNs and DRTHs were prepared with tricaprin, triethanolamine, Tween 80, and Span 20. Among the SLNs tested, an SLN composed of 1 g irinotecan, 0.5 g lipid mixture, and 0.5 g combined surfactant gave the highest entrapment efficiency and smallest particle size. A DRTH composed of (poloxamer 407/poloxamer 188/combined surfactant/SLN dispersion/H₂O (10/15/17/4/54%)) showed easy administration, fast gelling, and strong gel-forming in the body. Full article

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2020

Jump to: 2024, 2023, 2022, 2021

14 pages, 1704 KiB

Open AccessEditor’s ChoiceArticle

Drug-Eluting Biodegradable Implants for the Sustained Release of Bisphosphonates

by Cintya Dharmayanti, Todd A. Gillam, Desmond B. Williams and Anton Blencowe

Polymers 2020, 12(12), 2930; https://doi.org/10.3390/polym12122930 - 7 Dec 2020

Cited by 19 | Viewed by 4431

Abstract

Despite being one of the first-line treatments for osteoporosis, the bisphosphonate drug class exhibits an extremely low oral bioavailability (<1%) due to poor absorption from the gastrointestinal tract. To overcome this, and to explore the potential for sustained drug release, bioerodible poly(lactic acid) (PLA) and poly(D,L-lactide-co-glycolide) (PLGA) implants loaded with the bisphosphonate alendronate sodium (ALN) were prepared via hot-melt extrusion. The rate of drug release in vitro was modulated by tailoring the ratio of lactide to glycolide in the polymer and by altering the ALN-loading of the implants. All investigated implants exhibited sustained ALN release in vitro between 25 to 130 days, where implants of greater glycolide composition and higher ALN-loadings released ALN more rapidly. All PLGA implants demonstrated a sigmoidal release profile, characterised by an initial surface dissolution phase, followed by a period of zero-order drug diffusion, then relaxation or erosion of the polymer chains that caused accelerated release over the subsequent days. Contrastingly, the PLA implants demonstrated a logarithmic release profile, characterised by a gradual decrease in ALN release over time. Full article

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18 pages, 11787 KiB

Open AccessEditor’s ChoiceArticle

Micellar Carriers Based on Amphiphilic PEG/PCL Graft Copolymers for Delivery of Active Substances

by Justyna Odrobińska and Dorota Neugebauer

Polymers 2020, 12(12), 2876; https://doi.org/10.3390/polym12122876 - 30 Nov 2020

Cited by 11 | Viewed by 3897

Abstract

Amphiphilic copolymers of alkyne functionalized 2-hydroxyethyl methacrylate (AlHEMA) and poly(ethylene glycol) methyl ether methacrylate (MPEGMA) with graft or V-shaped graft topologies were synthesized. The functionalization of poly(ε-caprolactone) (PCL) with azide group enabled attachment to P(AlHEMA-co-MPEGMA) copolymers via a “click” alkyne-azide reaction. The introduction of PCL as a second side chain type in addition to PEG resulted in heterografted copolymers with modified properties such as biodegradability. “Click” reactions were carried out with efficiencies between 17–70% or 32–50% (for lower molecular weight PCL, 4000 g/mol, or higher molecular weight PCL, 9000 g/mol, respectively) depending on the PEG grafting density. The graft copolymers were self-assembled into micellar superstructures with the ability to encapsulate active substances, such as vitamin C (VitC), arbutin (ARB) or 4-n-butylresorcinol (4nBRE). Drug loading contents (DLC) were obtained in the range of 5–55% (VitC), 39–91% (ARB) and 42–98% (4nBRE). In vitro studies carried out in a phosphate buffer saline (PBS) solution (at pH 7.4 or 5.5) gave the maximum release levels of active substances after 10–240 min depending on the polymer system. Permeation tests in Franz chambers indicated that the bioactive substances after release by micellar systems penetrated through the artificial skin membrane in small amounts, and a majority of the bioactive substances remained inside the membrane, which is satisfactory for most cosmetic applications. Full article

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Published Papers (9 papers)

2024

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2023

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2022

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2021

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2020

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