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Polymers
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Biodegradable Polymers for Controlled Drug Release and Delivery
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Biodegradable Polymers for Controlled Drug Release and Delivery

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: closed (20 August 2023) | Viewed by 22327

Special Issue Editors

Prof. Dr. Trong-Ming Don

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Guest Editor
Department of Chemical and Materials Engineering, Tamkang University, New Taipei City 251, Taiwan
Interests: chemical modification and applications of chitosan and chitosan-derived materials studies on biodegradable nanocomposites; chemical modification of epoxies and epoxyacrylates
Special Issues, Collections and Topics in MDPI journals
Dr. Chih-Yu Kuo

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Guest Editor
Department of Chemical Engineering and Biotechnology, National Taipei University of Technology, Taipei City 10608, Taiwan
Interests: RAFT Polymerization; Self-Assembly Control of Stimuli-Responsive Polymers; Drug Controlled Release; Trigger-responsive peptidyl liposome

Special Issue Information

Owing to their versatile functionality, polymers are the most investigated materials for controlled drug release and delivery system. Biodegradable polymers including both natural and synthetic polymers such as polysaccharides and aliphatic polyesters, mostly are considered to be biocompatible and bioactive. Moreover, biodegradable polymers can also be modified to own the tuneable physical, chemical and mechanical properties. These biodegradable polymers are frequently applied as the building block of drug carriers to encapsulate and store the therapeutic drugs from immune clearance and to deliver them to illness sites. They are also adapted to possess stimuli-responsive properties for triggering and controlling the release of laden drugs through biological, chemical or physical reactions at targeting region. In this Special Issue, we would like to invite the short communications, reviews and research articles to collect the most advanced results including the synthesis, characterization, properties of natural and synthetic biodegradable polymers, with particular aim to their controlled release behaviors as well as the drug delivery applications.

Prof. Dr. Trong-Ming Don
Dr. Chih-Yu Kuo
Guest Editors

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.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

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Published Papers (7 papers)

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Research

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20 pages, 4589 KiB  
Article
A Printable Magnetic-Responsive Iron Oxide Nanoparticle (ION)-Gelatin Methacryloyl (GelMA) Ink for Soft Bioactuator/Robot Applications
by Han-Wen Yang, Nien-Tzu Yeh, Tzu-Ching Chen, Yu-Chun Yeh, I-Chi Lee and Yi-Chen Ethan Li
Polymers 2024, 16(1), 25; https://doi.org/10.3390/polym16010025 - 20 Dec 2023
Viewed by 1624
Abstract
The features or actuation behaviors of nature’s creatures provide concepts for the development of biomimetic soft bioactuators/robots with stimuli-responsive capabilities, design convenience, and environmental adaptivity in various fields. Mimosa pudica is a mechanically responsive plant that can convert pressure to the motion of [...] Read more.
The features or actuation behaviors of nature’s creatures provide concepts for the development of biomimetic soft bioactuators/robots with stimuli-responsive capabilities, design convenience, and environmental adaptivity in various fields. Mimosa pudica is a mechanically responsive plant that can convert pressure to the motion of leaves. When the leaves receive pressure, the occurrence of asymmetric turgor in the extensor and flexor sides of the pulvinus from redistributing the water in the pulvinus causes the bending of the pulvinus. Inspired by the actuation of Mimosa pudica, designing soft bioactuators can convert external stimulations to driving forces for the actuation of constructs which has been receiving increased attention and has potential applications in many fields. 4D printing technology has emerged as a new strategy for creating versatile soft bioactuators/robots by integrating printing technologies with stimuli-responsive materials. In this study, we developed a hybrid ink by combining gelatin methacryloyl (GelMA) polymers with iron oxide nanoparticles (IONs). This hybrid ION-GelMA ink exhibits tunable rheology, controllable mechanical properties, magnetic-responsive behaviors, and printability by integrating the internal metal ion-polymeric chain interactions and photo-crosslinking chemistries. This design offers the inks a dual crosslink mechanism combining the advantages of photocrosslinking and ionic crosslinking to rapidly form the construct within 60 s of UV exposure time. In addition, the magnetic-responsive actuation of ION-GelMA constructs can be regulated by different ION concentrations (0–10%). Furthermore, we used the ION-GelMA inks to fabricate a Mimosa pudica-like soft bioactuator through a mold casting method and a direct-ink-writing (DIW) printing technology. Obviously, the pinnule leaf structure of printed constructs presents a continuous reversible shape transformation in an air phase without any liquid as a medium, which can mimic the motion characteristics of natural creatures. At the same time, compared to the model casting process, the DIW printed bioactuators show a more refined and biomimetic transformation shape that closely resembles the movement of the pinnule leaf of Mimosa pudica in response to stimulation. Overall, this study indicates the proof of concept and the potential prospect of magnetic-responsive ION-GelMA inks for the rapid prototyping of biomimetic soft bioactuators/robots with untethered non-contact magneto-actuations. Full article
(This article belongs to the Special Issue Biodegradable Polymers for Controlled Drug Release and Delivery)
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25 pages, 5136 KiB  
Article
In Situ Encapsulation of Camptothecin by Self-Assembly of Poly(acrylic acid)-b-Poly(N-Isopropylacrylamide) and Chitosan for Controlled Drug Delivery
by Yi-Cheng Huang, Yang-Jie Zeng, Yu-Wei Lin, Hung-Chih Tai and Trong-Ming Don
Polymers 2023, 15(11), 2463; https://doi.org/10.3390/polym15112463 - 26 May 2023
Cited by 6 | Viewed by 2304
Abstract
Camptothecin (CPT) has been shown to exhibit anticancer activity against several cancers. Nevertheless, CPT is very hydrophobic with poor stability, and thus its medical application is limited. Therefore, various drug carriers have been exploited for effectively delivering CPT to the targeted cancer site. [...] Read more.
Camptothecin (CPT) has been shown to exhibit anticancer activity against several cancers. Nevertheless, CPT is very hydrophobic with poor stability, and thus its medical application is limited. Therefore, various drug carriers have been exploited for effectively delivering CPT to the targeted cancer site. In this study, a dual pH/thermo-responsive block copolymer of poly(acrylic acid-b-N-isopropylacrylamide) (PAA-b-PNP) was synthesized and applied to encapsulate CPT. At temperatures above its cloud point, the block copolymer self-assembled to form nanoparticles (NPs) and in situ encapsulate CPT, owing to their hydrophobic interaction as evidenced by fluorescence spectrometry. Chitosan (CS) was further applied on the surface through the formation of a polyelectrolyte complex with PAA for improving biocompatibility. The average particle size and zeta potential of the developed PAA-b-PNP/CPT/CS NPs in a buffer solution were 168 nm and −30.6 mV, respectively. These NPs were still stable at least for 1 month. The PAA-b-PNP/CS NPs exhibited good biocompatibility toward NIH 3T3 cells. Moreover, they could protect the CPT at pH 2.0 with a very slow-release rate. At pH 6.0, these NPs could be internalized by Caco-2 cells, followed by intracellular release of the CPT. They became highly swollen at pH 7.4, and the released CPT was able to diffuse into the cells at higher intensity. Among several cancer cell lines, the highest cytotoxicity was observed for H460 cells. As a result, these environmentally-responsive NPs have the potential to be applied in oral administration. Full article
(This article belongs to the Special Issue Biodegradable Polymers for Controlled Drug Release and Delivery)
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20 pages, 3588 KiB  
Article
Application of Amyloid-Based Hybrid Membranes in Drug Delivery
by You-Ren Lai, Steven S.-S. Wang, Ti-Lun Hsu, Szu-Hui Chou, Su-Chun How and Ta-Hsien Lin
Polymers 2023, 15(6), 1444; https://doi.org/10.3390/polym15061444 - 14 Mar 2023
Cited by 10 | Viewed by 2634
Abstract
The properties of amyloid fibrils, e.g., unique structural characteristics and superior biocompatibility, make them a promising vehicle for drug delivery. Here, carboxymethyl cellulose (CMC) and whey protein isolate amyloid fibril (WPI-AF) were used to synthesize amyloid-based hybrid membranes as vehicles for the delivery [...] Read more.
The properties of amyloid fibrils, e.g., unique structural characteristics and superior biocompatibility, make them a promising vehicle for drug delivery. Here, carboxymethyl cellulose (CMC) and whey protein isolate amyloid fibril (WPI-AF) were used to synthesize amyloid-based hybrid membranes as vehicles for the delivery of cationic and hydrophobic drugs (e.g., methylene blue (MB) and riboflavin (RF)). The CMC/WPI-AF membranes were synthesized via chemical crosslinking coupled with phase inversion. The zeta potential and scanning electron microscopy results revealed a negative charge and a pleated surface microstructure with a high content of WPI-AF. FTIR analysis showed that the CMC and WPI-AF were cross-linked via glutaraldehyde and the interacting forces between membrane and MB or RF was found to be electrostatic interaction and hydrogen bonding, respectively. Next, the in vitro drug release from membranes was monitored using UV-vis spectrophotometry. Additionally, two empirical models were used to analyze the drug release data and relevant rate constant and parameters were determined accordingly. Moreover, our results indicated that in vitro drug release rates depended on the drug–matrix interactions and transport mechanism, which could be controlled by altering the WPI-AF content in membrane. This research provides an excellent example of utilizing two-dimensional amyloid-based materials for drug delivery. Full article
(This article belongs to the Special Issue Biodegradable Polymers for Controlled Drug Release and Delivery)
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20 pages, 4505 KiB  
Article
In Situ Release of Ulvan from Crosslinked Ulvan/Chitosan Complex Films and Their Evaluation as Wound Dressings
by Trong-Ming Don, Chen-Han Ma and Yi-Cheng Huang
Polymers 2022, 14(24), 5382; https://doi.org/10.3390/polym14245382 - 8 Dec 2022
Cited by 4 | Viewed by 2198
Abstract
When a wound forms due to any injuries, it should be covered with a functional wound dressing for accelerating wound healing and reducing infection. In this study, crosslinked ulvan/chitosan complex films were prepared with or without the addition of glycerol and chlorophyll, and [...] Read more.
When a wound forms due to any injuries, it should be covered with a functional wound dressing for accelerating wound healing and reducing infection. In this study, crosslinked ulvan/chitosan complex films were prepared with or without the addition of glycerol and chlorophyll, and their wound healing properties were evaluated for potential application in wound dressing. The results showed that the tensile strength and elongation at break of the prepared ulvan/chitosan complex films were 2.23−2.48 MPa and 83.8−108.5%, respectively. Moreover, their water vapor transmission rates (WVTRs) were in the range of 1791−2029 g/m2-day, providing suitable environment for wound healing. Particularly, these complex films could release ulvan in situ in a short time, and the film with chlorophyll added had the highest release rate, reaching 62.8% after 20 min of releasing. In vitro studies showed that they were biocompatible toward NIH 3T3 and HaCaT cells, and promoted the migration of NIH 3T3 cells. These complex films could protect HaCaT cells from oxidative damage and reduce the production of reactive oxygen species (ROS); the addition of chlorophyll also effectively reduced the inflammatory response induced by LPS as found in the reduction in both NO and IL-6. Animal models showed that the complex films added with glycerol and chlorophyll could promote wound healing in the early stage, while accelerating the regeneration of dermal glands and collagen production. Briefly, these ulvan/chitosan complex films had good physiochemical properties and biological activity, and could accelerate wound healing both in vitro and in vivo. Full article
(This article belongs to the Special Issue Biodegradable Polymers for Controlled Drug Release and Delivery)
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14 pages, 3802 KiB  
Article
Magnetic Graphene-Based Nanosheets with Pluronic F127-Chitosan Biopolymers Encapsulated α-Mangosteen Drugs for Breast Cancer Cells Therapy
by Andri Hardiansyah, Ahmad Randy, Rizna Triana Dewi, Marissa Angelina, Nurfina Yudasari, Sri Rahayu, Ika Maria Ulfah, Faiza Maryani, Yu-Wei Cheng and Ting-Yu Liu
Polymers 2022, 14(15), 3163; https://doi.org/10.3390/polym14153163 - 3 Aug 2022
Cited by 5 | Viewed by 2597
Abstract
In this study, multifunctional chitosan-pluronic F127 with magnetic reduced graphene oxide (MRGO) nanocomposites were developed through the immobilization of chitosan and an amphiphilic polymer (pluronic F127) onto the MRGO. Physicochemical characterizations and in-vitro cytotoxicity of nanocomposites were investigated through field emission scanning electron [...] Read more.
In this study, multifunctional chitosan-pluronic F127 with magnetic reduced graphene oxide (MRGO) nanocomposites were developed through the immobilization of chitosan and an amphiphilic polymer (pluronic F127) onto the MRGO. Physicochemical characterizations and in-vitro cytotoxicity of nanocomposites were investigated through field emission scanning electron microscopy (FESEM), X-ray diffraction (XRD), Fourier-transform infrared (FTIR) spectroscopy, particle size analysis, vibrating sample magnetometer, Raman spectroscopy and resazurin-based in-vitro cytotoxicity assay. FESEM observation shows that the magnetic nanoparticles could tethered on the surface of MRGO, promoting the magnetic properties of the nanocomposites. FTIR identification analysis revealed that the chitosan/pluronic F127 were successfully immobilized on the surface of MRGO. Furthermore, α-mangosteen, as a model of natural drug compound, was successfully encapsulated onto the chitosan/pluronic F127@MRGO nanocomposites. According to in-vitro cytotoxicity assay, α-mangosteen-loaded chitosan/pluronic F127@MRGO nanocomposites could significantly reduce the proliferation of human breast cancer (MFC-7) cells. Eventually, it would be anticipated that the novel α-mangosteen-loaded chitosan/pluronic F127@MRGO nanocomposites could be promoted as a new potential material for magnetically targeting and killing cancer cells. Full article
(This article belongs to the Special Issue Biodegradable Polymers for Controlled Drug Release and Delivery)
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17 pages, 4477 KiB  
Article
Biodegradable Nanoparticles Prepared from Chitosan and Casein for Delivery of Bioactive Polysaccharides
by Chi Lin, Fang-Yu Hsu, Wei-Ting Lin, Chia-Yun Cha, Yi-Cheng Ho and Fwu-Long Mi
Polymers 2022, 14(14), 2966; https://doi.org/10.3390/polym14142966 - 21 Jul 2022
Cited by 9 | Viewed by 2745
Abstract
Ophiopogon japonicus polysaccharides (OJPs) have great anti-inflammation and immunomodulatory abilities. However, the low bioavailability of OJPs reduces its applicability in the biomedical and pharmaceutical fields. Chitosan (CS) has excellent mucoadhesive properties and absorption-enhancing ability in oral administration. Casein hydrolysate (CL) has good interfacial [...] Read more.
Ophiopogon japonicus polysaccharides (OJPs) have great anti-inflammation and immunomodulatory abilities. However, the low bioavailability of OJPs reduces its applicability in the biomedical and pharmaceutical fields. Chitosan (CS) has excellent mucoadhesive properties and absorption-enhancing ability in oral administration. Casein hydrolysate (CL) has good interfacial diffusivity and emulsifying ability, and can interact with polysaccharides to form complexes combining the individual properties of both. Therefore, chitosan and casein hydrolysate are good candidates for developing nanoformulations for oral delivery. In this study, bioactive polysaccharides (OJPs), CS and CL, were combined to prepare CS/OJPs/CL co-assembled biodegradable nanoparticles. The interactions between polysaccharides (CS and OJPs) and peptide (CL) resulted in the formation of nanoparticles with an average particle size of 198 nm and high OJPs loading efficiency. The colloidal properties of the nanoparticles were pH-dependent, which were changed significantly in simulated digestive fluid at different pH values. OJPs released from the CS/OJPs/CL nanoparticles were greatly affected by pH and enzymatic degradation (trypsin and lysozyme). The nanoparticles were easily internalized by macrophages, thereby enhancing the OJPs’ inhibitory ability against Ni2+-induced cytotoxicity and LPS-induced nitric oxide production. This study demonstrates that prepared polysaccharide/protein co-assembled nanoparticles can be potential nanocarriers for the oral delivery of bioactive polysaccharides with anti-inflammatory functions. Full article
(This article belongs to the Special Issue Biodegradable Polymers for Controlled Drug Release and Delivery)
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Review

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18 pages, 969 KiB  
Review
Cubosomes: Design, Development, and Tumor-Targeted Drug Delivery Applications
by Hassaan Umar, Habibah A. Wahab, Amirah Mohd Gazzali, Hafsa Tahir and Waqas Ahmad
Polymers 2022, 14(15), 3118; https://doi.org/10.3390/polym14153118 - 31 Jul 2022
Cited by 29 | Viewed by 6696
Abstract
Because of the extraordinary advancements in biomedical nanotechnology over the last few decades, traditional drug delivery systems have been transformed into smart drug delivery systems that respond to stimuli. These well-defined nanoplatforms can boost therapeutic targeting efficacy while reducing the side effects/toxicities of [...] Read more.
Because of the extraordinary advancements in biomedical nanotechnology over the last few decades, traditional drug delivery systems have been transformed into smart drug delivery systems that respond to stimuli. These well-defined nanoplatforms can boost therapeutic targeting efficacy while reducing the side effects/toxicities of payloads, which are crucial variables for enhancing patient compliance by responding to specific internal or external triggers. Cubosomes are lipid-based nano systems that are analogous to well-known vesicular systems, such as lipo- and niosomes. They could be used as part of a unique drug delivery system that includes hydro-, lipo-, and amphiphilic drug molecules. In this review, we critically analyze the relevant literature on cubosomesregarding theories of cubosomeself-assembly, composition, and manufacturing methods, with an emphasis on tumor-targeted drug delivery applications. Due to the bioadhesive and -compatible nature of cubosome dispersion, this review also focuses on a variety of drug delivery applications, including oral, ophthalmic and transdermal. Full article
(This article belongs to the Special Issue Biodegradable Polymers for Controlled Drug Release and Delivery)
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