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A special issue of Marine Drugs (ISSN 1660-3397).

Deadline for manuscript submissions: closed (30 November 2019) | Viewed by 63710

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Prof. Dr. Giuseppina Sandri

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Guest Editor

Department of Drug Sciences, University of Pavia, Viale Taramelli 12, 27100 Pavia, Italy
Interests: nanoparticles; nanofibers; in situ gelling systems; scaffolds; tissue engineering
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Prof. Dr. Silvia Rossi

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Guest Editor

Department of Drug Sciences, University of Pavia, Viale Taramelli 12, 27100 Pavia, Italy
Interests: rheology and viscosimetry; mucoadhesion; in situ gelling polymers; micro- and nanoparticulate systems; statistical optimization techniques; wound dressings, nervous tissue repair
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

In the last few decades, there has been a progressive change in the concept of pharmaceutical excipients that are no longer considered as “inert supports”, but as multifunctional substances able to act in synergy with the active principle loaded in the drug delivery system. The pharmaceutical industry uses excipients from a wide variety of sources. In particular, polysaccharides of natural origin have been registering an ever- increasing interest, due to their peculiar properties such as biocompatibility, biodegradability and low cost.

Ocean is an ecosystem remarkably rich in diversified organisms that make it a wide source of natural substances. Among these, polysaccharides are the most abundant bioactive molecules in marine organisms. They can be obtained by algae (the main source), but also by animal sources, such as the skeleton of crustaceans and cartilaginous fish tissue, and by microorganisms such as some prokaryotes. These biomaterials have a wide range of applications in drug delivery, such as modified drug delivery, nanotechnology, drug targeting, gene delivery, and regenerative medicine.

This Special Issue of Marine Drugs will highlight the importance of marine polysaccharides/biopolymers in different aspects of the drug delivery, collecting novel research papers and original reviews focused on the use of marine polysaccharides/biopolymers as multifunctional excipients.

As Guest Editors, we encourage colleagues to contribute to this Special Issue of Marine Drugs with papers showing significant advances in this field.

Prof. Dr. Giuseppina Sandri
Prof. Dr. Silvia Rossi
Guest Editors

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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. Marine Drugs is an international peer-reviewed open access monthly journal published by MDPI.

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Published Papers (12 papers)

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Research

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18 pages, 2962 KiB

Open AccessArticle

Complex Polysaccharide-Based Nanocomposites for Oral Insulin Delivery

by Mar Collado-González, Maria Cristina Ferreri, Alessandra R. Freitas, Ana Cláudia Santos, Nuno R. Ferreira, Guzmán Carissimi, Joana A. D. Sequeira, F. Guillermo Díaz Baños, Gloria Villora, Francisco Veiga and Antonio Ribeiro

Mar. Drugs 2020, 18(1), 55; https://doi.org/10.3390/md18010055 - 15 Jan 2020

Cited by 20 | Viewed by 4316

Abstract

Polyelectrolyte nanocomposites rarely reach a stable state and aggregation often occurs. Here, we report the synthesis of nanocomposites for the oral delivery of insulin composed of alginate, dextran sulfate, poly-(ethylene glycol) 4000, poloxamer 188, chitosan, and bovine serum albumin. The nanocomposites were obtained by Ca²⁺-induced gelation of alginate followed by an electrostatic-interaction process among the polyelectrolytes. Chitosan seemed to be essential for the final size of the nanocomposites and there was an optimal content that led to the synthesis of nanocomposites of 400–600 nm hydrodynamic size. The enhanced stability of the synthesized nanocomposites was assessed with LUMiSizer after synthesis. Nanocomposite stability over time and under variations of ionic strength and pH were assessed with dynamic light scattering. The rounded shapes of nanocomposites were confirmed by scanning electron microscopy. After loading with insulin, analysis by HPLC revealed complete drug release under physiologically simulated conditions. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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20 pages, 4309 KiB

Open AccessArticle

Dual-Functioning Scaffolds for the Treatment of Spinal Cord Injury: Alginate Nanofibers Loaded with the Sigma 1 Receptor (S1R) Agonist RC-33 in Chitosan Films

by Barbara Vigani, Silvia Rossi, Giuseppina Sandri, Maria Cristina Bonferoni, Marta Rui, Simona Collina, Francesca Fagiani, Cristina Lanni and Franca Ferrari

Mar. Drugs 2020, 18(1), 21; https://doi.org/10.3390/md18010021 - 26 Dec 2019

Cited by 22 | Viewed by 3542

Abstract

The present work proposed a novel therapeutic platform with both neuroprotective and neuroregenerative potential to be used in the treatment of spinal cord injury (SCI). A dual-functioning scaffold for the delivery of the neuroprotective S1R agonist, RC-33, to be locally implanted at the site of SCI, was developed. RC-33-loaded fibers, containing alginate (ALG) and a mixture of two different grades of poly(ethylene oxide) (PEO), were prepared by electrospinning. After ionotropic cross-linking, fibers were incorporated in chitosan (CS) films to obtain a drug delivery system more flexible, easier to handle, and characterized by a controlled degradation rate. Dialysis equilibrium studies demonstrated that ALG was able to form an interaction product with the cationic RC-33 and to control RC-33 release in the physiological medium. Fibers loaded with RC-33 at the concentration corresponding to 10% of ALG maximum binding capacity were incorporated in films based on CS at two different molecular weights—low (CSL) and medium (CSM)—solubilized in acetic (AA) or glutamic (GA) acid. CSL- based scaffolds were subjected to a degradation test in order to investigate if the different CSL salification could affect the film behavior when in contact with media that mimic SCI environment. CSL AA exhibited a slower biodegradation and a good compatibility towards human neuroblastoma cell line. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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16 pages, 2547 KiB

Open AccessArticle

Sequential Delivery of Dual Growth Factors from Injectable Chitosan-Based Composite Hydrogels

by Qing Min, Jiaoyan Liu, Xiaofeng Yu, Yuchen Zhang, Jiliang Wu and Ying Wan

Mar. Drugs 2019, 17(6), 365; https://doi.org/10.3390/md17060365 - 20 Jun 2019

Cited by 25 | Viewed by 4849

Abstract

Local administration of platelet-derived growth factor-BB (PGDF-BB) and bone morphogenetic protein-2 (BMP-2) in a sequential release manner could substantially promote bone healing. To achieve this goal, a delivery system that could sustain the release of PGDF-BB and BMP-2 by way of temporal separation was developed. One type of PGDF-BB-encapsulated alginate microsphere and another type of BMP-2-encapsulated microsphere with a core-shell structure were respectively produced using emulsification methods. These two types of microspheres were then embedded into chitosan/glycerophosphate hydrogel for constructing composite gels. Some of them were found to be injectable at ambient temperature and had thermo-sensitive features near physiological temperature and pH. The optimally formulated composite gels showed the ability to control the release of PGDF-BB and BMP-2 in a sequential fashion in which PDGF-BB was released earlier than BMP-2. In vitro release patterns indicated that the release rates could be significantly regulated by varying the embedded amount of the factor-encapsulated microspheres, which can in turn mediate the temporal separation release interval between PGDF-BB and BMP-2. The released PDGF-BB and BMP-2 were detected to be bioactive based on their respective effects on Balb/c 3T3 and C2C12 cells. These results suggest that the presently developed composite gels have the potential for bone repair by synergistically utilizing the early chemotactic effect of PDGF-BB and the subsequent osteogenic and angiogenic functions of PDGF-BB and BMP-2. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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14 pages, 3138 KiB

Open AccessArticle

Edaravone-Loaded Alginate-Based Nanocomposite Hydrogel Accelerated Chronic Wound Healing in Diabetic Mice

by Ying Fan, Wen Wu, Yu Lei, Caroline Gaucher, Shuchen Pei, Jinqiang Zhang and Xuefeng Xia

Mar. Drugs 2019, 17(5), 285; https://doi.org/10.3390/md17050285 - 11 May 2019

Cited by 62 | Viewed by 6117

Abstract

Refractory wound healing is one of the most common complications of diabetes. Excessive production of reactive oxygen species (ROS) can cause chronic inflammation and thus impair cutaneous wound healing. Scavenging these ROS in wound dressing may offer effective treatment for chronic wounds. Here, a nanocomposite hydrogel based on alginate and positively charged Eudragit nanoparticles containing edaravone, an efficient free radical scavenger, was developed for maximal ROS sequestration. Eudragit nanoparticles enhanced edaravone solubility and stability breaking the limitations in application. Furthermore, loading these Eudragit nanoparticles into an alginate hydrogel increased the protection and sustained the release of edaravone. The nanocomposite hydrogel is shown to promote wound healing in a dose-dependent way. A low dose of edaravone-loaded nanocomposite hydrogel accelerated wound healing in diabetic mice. On the contrary, a high dose of edaravone might hamper the healing. Those results indicated the dual role of ROS in chronic wounds. In addition, the discovery of this work pointed out that dose could be the key factor limiting the translational application of antioxidants in wound healing. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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10 pages, 2029 KiB

Open AccessArticle

Preparation and Evaluation of Release Formulation of γ-Oryzanol/Algae Oil Self-Emulsified with Alginate Beads

by Kai-Min Yang and Po-Yuan Chiang

Mar. Drugs 2019, 17(3), 156; https://doi.org/10.3390/md17030156 - 7 Mar 2019

Cited by 17 | Viewed by 3971

Abstract

Self-emulsion improves solubility and bioavailability for γ-oryzanol/algae oil, and alginate beads can be used as controlled release carriers. In this study, self-emulsified alginate beads (SEABs) were prepared with different weight ratios of self-emulsion treatment (5%, 10%, 15%, 20%, and 30%) with alginate. We found that the microstructure with a surfactant of SEABs had a different appearance with alginate-based beads. The encapsulation of γ-oryzanol corresponded with the self-emulsion/alginate ratio, which was 98.93~60.20% with a different formulation of SEABs. During in vitro release, SEABs had the gastric protection of γ-oryzanol/algae oil, because γ-oryzanol and emulsion were not released in the simulated stomach fluid. When the SEABs were transferred to a simulation of the small intestine, they quickly began to swell and dissolve, releasing a higher content of the emulsion. We observed that the emulsion that formed had a bimodal distribution in the simulated intestinal fluid as a result of the hydrogel and emulsion droplets, leading to the formation of large aggregates. These results suggested that γ-oryzanol encapsulation within alginate beads via emulsification combined with gelation can serve as an effective controlled delivery system. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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16 pages, 3073 KiB

Open AccessArticle

Development of a Mucoadhesive and an in Situ Gelling Formulation Based on κ-Carrageenan for Application on Oral Mucosa and Esophagus Walls. II. Loading of a Bioactive Hydroalcoholic Extract

by Barbara Vigani, Silvia Rossi, Matteo Gentile, Giuseppina Sandri, Maria Cristina Bonferoni, Valeria Cavalloro, Emanuela Martino, Simona Collina and Franca Ferrari

Mar. Drugs 2019, 17(3), 153; https://doi.org/10.3390/md17030153 - 5 Mar 2019

Cited by 26 | Viewed by 3382

Abstract

The aim of the present work was to load a Hibiscus sabdariffa (HS) hydroalcoholic extract into in situ gelling formulations for the treatment of oral mucositis and esophagitis. Such formulations, selected as the most promising options in a previous work of ours, were composed by κ-carrageenan (κ-CG), a sulfated marine polymer able to gelify in presence of saliva ions, hydroxypropyl cellulose (HPC), used as mucoadhesive agent, and CaCl₂, salt able to enhance the interaction κ-CG/saliva ions. HS extract, which is rich in phytochemicals such as polyphenols, polysaccharides and organic acids, was selected due to its antioxidant and anti-inflammatory properties. For HS extraction, three different methodologies (maceration, Ultrasound Assisted Extraction (UAE) and Microwave Assisted Extraction (MAE)) were compared in terms of extraction yield and extract antioxidant activity, revealing that MAE was the best procedure. Rheological and mucoadhesive properties of HS-loaded formulations were investigated. Such formulations were characterized by a low viscosity at 25 °C, guaranteeing an easy administration, a proper in situ gelation behavior and marked elastic and mucoadhesive properties at 37 °C, functional to a protective action towards the damaged mucosa. Finally, the biocompatibility and the proliferative effect of HS-loaded formulations, as well as their antioxidant and anti-inflammatory properties, were proved in vitro on human dermal fibroblasts. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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16 pages, 3008 KiB

Open AccessArticle

Development of a Mucoadhesive and In Situ Gelling Formulation Based on κ-Carrageenan for Application on Oral Mucosa and Esophagus Walls. I. A Functional In Vitro Characterization

by Barbara Vigani, Angela Faccendini, Silvia Rossi, Giuseppina Sandri, Maria Cristina Bonferoni, Matteo Gentile and Franca Ferrari

Mar. Drugs 2019, 17(2), 112; https://doi.org/10.3390/md17020112 - 12 Feb 2019

Cited by 14 | Viewed by 3190

Abstract

Oral mucositis and esophagitis represent the most frequent and clinically significant complications of cytoreductive chemotherapy and radiotherapy, which severely compromise the patient quality of life. The local application of polymeric gels could protect the injured tissues, alleviating the most painful symptoms. The present work aims at developing in situ gelling formulations for the treatment of oral mucositis and esophagitis. To reach these targets, κ-carrageenan (κ-CG) was selected as a polymer having wound healing properties and able to gelify in the presence of saliva ions, while hydroxypropyl cellulose (HPC) was used to improve the mucoadhesive properties of the formulations. CaCl₂ was identified as a salt able to enhance the interaction between κ-CG and saliva ions. Different salt and polymer concentrations were investigated in order to obtain a formulation having the following features: (i) low viscosity at room temperature to facilitate administration, (ii) marked elastic properties at 37 °C, functional to a protective action towards damaged tissues, and (iii) mucoadhesive properties. Prototypes characterized by different κ-CG, HPC, and CaCl₂ concentrations were subjected to a thorough rheological characterization and to in vitro mucoadhesion and washability tests. The overall results pointed out the ability of the developed formulations to produce a gel able to interact with saliva ions and to adhere to the biological substrates. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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12 pages, 3512 KiB

Open AccessArticle

Photo-Cured Glycol Chitosan Hydrogel for Ovarian Cancer Drug Delivery

by Hoon Hyun, Min Ho Park, Gayoung Jo, So Yeon Kim, Heung Jae Chun and Dae Hyeok Yang

Mar. Drugs 2019, 17(1), 41; https://doi.org/10.3390/md17010041 - 10 Jan 2019

Cited by 59 | Viewed by 4782

Abstract

In this study, we prepared an injectable drug delivery depot system based on a visible light-cured glycol chitosan (GC) hydrogel containing paclitaxel (PTX)-complexed beta-cyclodextrin (β-CD) (GC/CD/PTX) for ovarian cancer (OC) therapy using a tumor-bearing mouse model. The hydrogel depot system had a 23.8 Pa of storage modulus at 100 rad/s after visible light irradiation for 10 s. In addition, GC was swollen as a function of time. However, GC had no degradation with the time change. Eventually, the swollen GC matrix affected the releases of PTX and CD/PTX. GC/PTX and GC/CD/PTX exhibited a controlled release of PTX for 7 days. In addition, GC/CD/PTX had a rapid PTX release for 7 days due to improved water solubility of PTX through CD/PTX complex. In vitro cell viability tests showed that GC/CD/PTX had a lower cell viability percentage than the free PTX solution and GC/PTX. Additionally, GC/CD/PTX resulted in a superior antitumor effect against OC. Consequently, we suggest that the GC/CD system might have clinical potential for OC therapy by improving the water solubility of PTX, as PTX is included into the cavity of β-CD. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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10 pages, 2729 KiB

Open AccessArticle

Nano-in-Micro Delivery System Prepared by Co-Axial Air Flow for Oral Delivery of Conjugated Linoleic Acid

by Qian Li, Fangfang Xue, Junle Qu, Liwei Liu, Rui Hu and Chenguang Liu

Mar. Drugs 2019, 17(1), 15; https://doi.org/10.3390/md17010015 - 28 Dec 2018

Cited by 3 | Viewed by 3140

Abstract

The preparation of a nano-in-micro delivery system (NiMDS) under mild conditions without using toxic organic solvents and expensive equipment still faces challenges. In this study, we introduced the co-axial air flow method to prepare NiMDS for the oral delivery of conjugated linoleic acid (CLA). The chitosan nanoparticles were prepared using the stearic-acid-modified chitosan through self-aggregation. Then, the chitosan nanoparticles were incorporated into alginate microparticles by the co-axial air flow method. The obtained chitosan nanoparticles and NiMDS were spherical in shape with the average sizes of 221–243 nm and 130–160 μm, respectively. Compared with alginate microparticles, the hybrid particles were of fewer fragments, were bigger in size, had a higher mechanical strength, and showed a controlled release in the phosphate buffer solution (pH 1.2 or 7.4). The release kinetics study showed that encapsulating the chitosan nanoparticles into the alginate microparticles inhibited the dissolution of alginate microparticles at the initial stage. These results revealed the potential of NiMDS as an ideal oral carrier for the sustained release of CLA in the gastrointestinal environment. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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18 pages, 8464 KiB

Open AccessArticle

Folate Receptor-Targeted and GSH-Responsive Carboxymethyl Chitosan Nanoparticles Containing Covalently Entrapped 6-Mercaptopurine for Enhanced Intracellular Drug Delivery in Leukemia

by Xuan Wei, Jianhong Liao, Zahra Davoudi, Hua Zheng, Jingru Chen, Dan Li, Xiong Xiong, Yihua Yin, Xiuxiang Yu, Jinghui Xiong and Qun Wang

Mar. Drugs 2018, 16(11), 439; https://doi.org/10.3390/md16110439 - 8 Nov 2018

Cited by 98 | Viewed by 6923

Abstract

For enhanced intracellular accumulation of 6-mercaptopurine (6-MP) in leukemia, a folate receptor-targeted and glutathione (GSH)-responsive polymeric prodrug nanoparticle was made. The nanoparticles were prepared by conjugating 6-MP to carboxymethyl chitosan via a GSH-sensitive carbonyl vinyl sulfide linkage, ultrasonic self-assembly and surface decoration with folate. The TEM graphs shows that the as-synthesized nanoparticles are spherical with a particle size of 170~220 nm. In vitro drug release of nanoparticles demonstrated acceptable stability in PBS containing 20 μM GSH at pH 7.4. However, the cumulative drug release rate of the samples containing 20 mM and 10 mM GSH medium reached 78.9% and 64.8%, respectively, in pH 5.0 at 20 h. This indicated that this nano-sized system is highly sensitive to GSH. The inhibition ratio of folate-modified nanoparticles compared to unmodified nanoparticles was higher in cancer cells (human promyelocytic leukemia cells, HL-60) while their cytotoxicity was lower in normal cells (mouse fibroblast cell lines, L929). Furthermore, in vitro cancer cell incubation studies confirmed that folate-modified nanoparticles therapeutics were significantly more effective than unmodified nanoparticles therapeutics. Our results suggest that folate receptor-targeting and GSH-stimulation can significantly elevate tumour intracellular drug release. Therefore, folate-modified nanoparticles containing chemoradiotherapy is a potential treatment for leukemia therapy. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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Review

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21 pages, 1761 KiB

Open AccessReview

Recent Advances in Chitosan-Based Carriers for Gene Delivery

by Ye Cao, Yang Fei Tan, Yee Shan Wong, Melvin Wen Jie Liew and Subbu Venkatraman

Mar. Drugs 2019, 17(6), 381; https://doi.org/10.3390/md17060381 - 25 Jun 2019

Cited by 255 | Viewed by 9802

Abstract

Approximately 4000 diseases are associated with malfunctioning genes in a particular cell type. Gene-based therapy provides a platform to modify the disease-causing genes expression at the cellular level to treat pathological conditions. However, gene delivery is challenging as these therapeutic genes need to overcome several physiological and intracellular barriers in order, to reach the target cells. Over the years, efforts have been dedicated to develop efficient gene delivery vectors to overcome these systemic barriers. Chitosan, a versatile polysaccharide, is an attractive non-viral vector material for gene delivery mainly due to its cationic nature, biodegradability and biocompatibility. The present review discusses the design factors that are critical for efficient gene delivery/transfection and highlights the recent progress of gene therapy using chitosan-based carriers. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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23 pages, 2175 KiB

Open AccessReview

Chitosan-Based In Situ Gels for Ocular Delivery of Therapeutics: A State-of-the-Art Review

by Teodora Irimia, Cristina-Elena Dinu-Pîrvu, Mihaela Violeta Ghica, Dumitru Lupuleasa, Daniela-Lucia Muntean, Denisa Ioana Udeanu and Lăcrămioara Popa

Mar. Drugs 2018, 16(10), 373; https://doi.org/10.3390/md16100373 - 9 Oct 2018

Cited by 108 | Viewed by 8477

Abstract

Ocular in situ gels are a promising alternative to overcome drawbacks of conventional eye drops because they associate the advantages of solutions such as accuracy and reproducibility of dosing, or ease of administration with prolonged contact time of ointments. Chitosan is a natural polymer suitable for use in ophthalmic formulations due to its biocompatibility, biodegradability, mucoadhesive character, antibacterial and antifungal properties, permeation enhancement and corneal wound healing effects. The combination of chitosan, pH-sensitive polymer, with other stimuli-responsive polymers leads to increased mechanical strength of formulations and an improved therapeutic effect due to prolonged ocular contact time. This review describes in situ gelling systems resulting from the association of chitosan with various stimuli-responsive polymers with emphasis on the mechanism of gel formation and application in ophthalmology. It also comprises the main techniques for evaluation of chitosan in situ gels, along with requirements of safety and ocular tolerability. Full article

(This article belongs to the Special Issue Marine Biopolymers and Drug Delivery)

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