Biopolymer Micro/Nanogel Particles as Smart Drug Delivery and Theranostic Systems

A special issue of Pharmaceutics (ISSN 1999-4923). This special issue belongs to the section "Drug Delivery and Controlled Release".

Deadline for manuscript submissions: closed (20 May 2023) | Viewed by 28402

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Institut des Sciences Analytiques et de Physico-Chimie pour l’Environnement et les Materiaux, UMR 5254, 64053 Pau, France
Interests: biopolymers; (bio)materials; bionanocomposites; functional polimeric materials; marine inspiration/biomimetics; valorization marine biomass; red and blue biotechnology; marine bioactive molecules; tissue engineering
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Bio-Inspired Materials Group: Functionalities & Self-Assembly, Universite de Pau et des Pays de l’Adour, E2S UPPA, 64000 Pau, France
Interests: responsive micro/nanogels; self-assembly of microgels; (transdermal) drug delivery; biopolymers; polymerization in dispersed medium

Special Issue Information

Dear Colleagues,

In recent years, micro/nanogels have become an important topic of interdisciplinary research, especially in the fields of polymer chemistry and material science focusing the efforts on their use for drug delivery and theranostic applications. In this regard, micro/nanogels can potentially revolutionize conventional therapy and diagnostic methods thanks to their incomparable chemical and physical versatility. These stem from the unique combination of their simple synthesis, large surface area, variation of their volume in response to different stimuli, and their ability to contain different types of both diagnostics and therapeutic agents in a single system.

In general, biocompatibility and even biodegradability is required for above-mentioned medical applications. In this sense, the use of biopolymers is presented an appropriate alternative to solve both issues. The diverse compositions, tunable physical behavior, and wide variety from which to choose open the possibility to develop a huge variety of biopolymer micro/nanogels suitable for different eco-friendly applications.

The aim of this Special Issue of Pharmaceutics is to present novel research and review papers on novel biopolymer-based micro/nanogels for biomedical applications such as drug delivery and theranostic. Contributions dealing with all aspects of the synthesis, characterization and (potential) applications in drug delivery and theranostics of biopolymer-based micro/nanogels are welcome. We would like to invite researchers to publish their original articles together with reviews with the aim of highlighting a general overview and future perspectives in these areas.

Dr. Susana C.M. Fernandes
Dr. Garbine Aguirre
Guest Editors

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Keywords

  • micro/nanogel
  • biopolymer
  • stimuli-responsiveness
  • biocompatibility
  • biodegradability
  • drug delivery
  • theranostics

Published Papers (13 papers)

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Editorial

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3 pages, 190 KiB  
Editorial
Biopolymer Micro/Nanogel Particles as Smart Drug Delivery and Theranostic Systems
by Susana C. M. Fernandes and Garbine Aguirre
Pharmaceutics 2023, 15(8), 2060; https://doi.org/10.3390/pharmaceutics15082060 - 31 Jul 2023
Viewed by 710
Abstract
In recent years, micro/nanogels have become an important topic of interdisciplinary research, especially in the fields of polymer chemistry and material science, with a focus on their use in drug delivery applications [...] Full article

Research

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13 pages, 1512 KiB  
Article
The Role of Crosslinker Content of Positively Charged NIPAM Nanogels on the In Vivo Toxicity in Zebrafish
by Roberta Bilardo, Federico Traldi, Caroline H. Brennan and Marina Resmini
Pharmaceutics 2023, 15(7), 1900; https://doi.org/10.3390/pharmaceutics15071900 - 07 Jul 2023
Cited by 2 | Viewed by 965
Abstract
Polymeric nanogels as drug delivery systems offer great advantages, such as high encapsulation capacity and easily tailored formulations; however, data on biocompatibility are still limited. We synthesized N-isopropylacrylamide nanogels, with crosslinker content between 5 and 20 mol%, functionalized with different positively charged [...] Read more.
Polymeric nanogels as drug delivery systems offer great advantages, such as high encapsulation capacity and easily tailored formulations; however, data on biocompatibility are still limited. We synthesized N-isopropylacrylamide nanogels, with crosslinker content between 5 and 20 mol%, functionalized with different positively charged co-monomers, and investigated the in vivo toxicity in zebrafish. Our results show that the chemical structure of the basic unit impacts the toxicity profile depending on the degree of ionization and hydrogen bonding capability. When the degree of crosslinking of the polymer was altered, from 5 mol% to 20 mol%, the distribution of the positively charged monomer 2-tert-butylaminoethyl methacrylate was significantly altered, leading to higher surface charges for the more rigid nanogels (20 mol% crosslinker), which resulted in >80% survival rate (48 h, up to 0.5 mg/mL), while the more flexible polymers (5 mol% crosslinker) led to 0% survival rate (48 h, up to 0.5 mg/mL). These data show the importance of tailoring both chemical composition and rigidity of the formulation to minimize toxicity and demonstrate that using surface charge data to guide the design of nanogels for drug delivery may be insufficient. Full article
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14 pages, 5475 KiB  
Article
Doxorubicin-Loaded Fungal-Carboxymethyl Chitosan Functionalized Polydopamine Nanoparticles for Photothermal Cancer Therapy
by Maduru Suneetha, Hyeonjin Kim and Sung Soo Han
Pharmaceutics 2023, 15(4), 1281; https://doi.org/10.3390/pharmaceutics15041281 - 19 Apr 2023
Cited by 2 | Viewed by 1217
Abstract
In this work, we synthesized doxorubicin-loaded fungal-carboxymethyl chitosan (FC) functionalized polydopamine (Dox@FCPDA) nanoparticles for improved anticancer activity via photothermal drug release. The photothermal properties revealed that the FCPDA nanoparticles with a concentration of 400 µg/mL produced a temperature of about 61.1 °C at [...] Read more.
In this work, we synthesized doxorubicin-loaded fungal-carboxymethyl chitosan (FC) functionalized polydopamine (Dox@FCPDA) nanoparticles for improved anticancer activity via photothermal drug release. The photothermal properties revealed that the FCPDA nanoparticles with a concentration of 400 µg/mL produced a temperature of about 61.1 °C at 2 W/cm2 laser illumination, which is more beneficial for cancer cells. Due to the hydrophilic FC biopolymer, the Dox was successfully encapsulated into FCPDA nanoparticles via electrostatic interactions and pi-pi stacking. The maximum drug loading and encapsulation efficiency were calculated to be 19.3% and 80.2%, respectively. The Dox@FCPDA nanoparticles exhibited improved anticancer activity on HePG2 cancer cells when exposed to an NIR laser (800 nm, 2 W/cm2). Furthermore, the Dox@FCPDA nanoparticles also improved cellular uptake with HepG2 cells. Therefore, functionalizing FC biopolymer with PDA nanoparticles is more beneficial for drug and photothermal dual therapeutic properties for cancer therapy. Full article
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26 pages, 14264 KiB  
Article
Folic Acid-Modified Ibrutinib-Loaded Silk Fibroin Nanoparticles for Cancer Cell Therapy with Over-Expressed Folate Receptor
by Marta G. Fuster, Mercedes G. Montalbán, Imane Moulefera, Gloria Víllora and David L. Kaplan
Pharmaceutics 2023, 15(4), 1186; https://doi.org/10.3390/pharmaceutics15041186 - 07 Apr 2023
Cited by 2 | Viewed by 1911
Abstract
The anticancer drug ibrutinib (IB), also known as PCI-32765, is a compound that irreversibly inhibits Bruton’s tyrosine kinase (BTK) and was initially developed as a treatment option for B-cell lineage neoplasms. Its action is not limited to B-cells, as it is expressed in [...] Read more.
The anticancer drug ibrutinib (IB), also known as PCI-32765, is a compound that irreversibly inhibits Bruton’s tyrosine kinase (BTK) and was initially developed as a treatment option for B-cell lineage neoplasms. Its action is not limited to B-cells, as it is expressed in all hematopoietic lineages and plays a crucial role in the tumor microenvironment. However, clinical trials with the drug have resulted in conflicting outcomes against solid tumors. In this study, folic acid-conjugated silk nanoparticles were used for the targeted delivery of IB to the cancer cell lines HeLa, BT-474, and SKBR3 by exploiting the overexpression of folate receptors on their surfaces. The results were compared with those of control healthy cells (EA.hy926). Cellular uptake studies confirmed total internalization of the nanoparticles functionalized by this procedure in the cancer cells after 24 h, compared to nanoparticles not functionalized with folic acid, suggesting that cellular uptake was mediated by folate receptors overexpressed in the cancer cells. The results indicate that the developed nanocarrier can be used for drug targeting applications by enhancing IB uptake in cancer cells with folate receptor overexpression. Full article
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20 pages, 3169 KiB  
Article
Degradable and Non-Degradable Chondroitin Sulfate Particles with the Controlled Antibiotic Release for Bacterial Infections
by Selin S. Suner, Mehtap Sahiner, Ramesh S. Ayyala and Nurettin Sahiner
Pharmaceutics 2022, 14(8), 1739; https://doi.org/10.3390/pharmaceutics14081739 - 20 Aug 2022
Cited by 5 | Viewed by 1708
Abstract
Non-degradable, slightly degradable, and completely degradable micro/nanoparticles derived from chondroitin sulfate (CS) were synthesized through crosslinking reactions at 50%, 40%, and 20% mole ratios, respectively. The CS particles with a 20% crosslinking ratio show total degradation within 48 h, whereas 50% CS particles [...] Read more.
Non-degradable, slightly degradable, and completely degradable micro/nanoparticles derived from chondroitin sulfate (CS) were synthesized through crosslinking reactions at 50%, 40%, and 20% mole ratios, respectively. The CS particles with a 20% crosslinking ratio show total degradation within 48 h, whereas 50% CS particles were highly stable for up to 240 h with only 7.0 ± 2.8% weight loss in physiological conditions (pH 7.4, 37 °C). Tobramycin and amikacin antibiotics were encapsulated into non-degradable CS particles with high loading at 250 g/mg for the treatment of corneal bacterial ulcers. The highest release capacity of 92 ± 2% was obtained for CS-Amikacin particles with sustainable and long-term release profiles. The antibacterial effects of CS particles loaded with 2.5 mg of antibiotic continued to render a prolonged release time of 240 h with 24 ± 2 mm inhibition zones against Pseudomonas aeruginosa. Furthermore, as a carrier, CS particles significantly improved the compatibility of the antibiotics even at high particle concentrations of 1000 g/mL with a minimum of 71 ± 7% fibroblast cell viability. In summary, the sustainable delivery of antibiotics and long-term treatment of bacterial keratitis were shown to be afforded by the design of tunable degradation ability of CS particles with improved biocompatibility for the encapsulated drugs. Full article
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23 pages, 6079 KiB  
Article
Formulation and Evaluation of Hybrid Niosomal In Situ Gel for Intravesical Co-Delivery of Curcumin and Gentamicin Sulfate
by Viliana Gugleva, Victoria Michailova, Rositsa Mihaylova, Georgi Momekov, Maya Margaritova Zaharieva, Hristo Najdenski, Petar Petrov, Stanislav Rangelov, Aleksander Forys, Barbara Trzebicka and Denitsa Momekova
Pharmaceutics 2022, 14(4), 747; https://doi.org/10.3390/pharmaceutics14040747 - 30 Mar 2022
Cited by 16 | Viewed by 2864
Abstract
The current study describes the elaboration of a hybrid drug delivery platform for an intravesical application based on curcumin/gentamicin sulfate simultaneously loaded niosomes incorporated into thermosensitive in situ gels. Series of niosomes were elaborated via the thin film hydration method, evaluating the impact [...] Read more.
The current study describes the elaboration of a hybrid drug delivery platform for an intravesical application based on curcumin/gentamicin sulfate simultaneously loaded niosomes incorporated into thermosensitive in situ gels. Series of niosomes were elaborated via the thin film hydration method, evaluating the impact of non-ionic surfactants’, cholesterol’s, and curcumin’s concentration. The formulation composed of equimolar ratio of Span 60, Tween 60, and 30 mol% cholesterol was selected as the optimal composition, due to the high entrapment efficiency values obtained for both drugs, and appropriate physicochemical parameters (morphology, size, PDI, and zeta potential), therefore, was further incorporated into Poloxamers (407/188) and Poloxamers and chitosan based in situ gels. The developed hybrid systems were characterized with sol to gel transition in the physiological range, suitable rheological and gelling characteristics. In addition, the formed gel structure at physiological temperatures determines the retarded dissolution of both drugs (vs. niosomal suspension) and sustained release profile. The conducted microbial studies of selected niosomal in situ gels revealed the occurrence of a synergetic effect of the two compounds when simultaneously loaded. The findings indicate that the elaborated thermosensitive niosomal in situ gels can be considered as a feasible platform for intravesical drug delivery. Full article
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16 pages, 4266 KiB  
Article
Mineralizing Gelatin Microparticles as Cell Carrier and Drug Delivery System for siRNA for Bone Tissue Engineering
by Sandra Hinkelmann, Alexandra H. Springwald, Sabine Schulze, Ute Hempel, Franziska Mitrach, Christian Wölk, Michael C. Hacker and Michaela Schulz-Siegmund
Pharmaceutics 2022, 14(3), 548; https://doi.org/10.3390/pharmaceutics14030548 - 28 Feb 2022
Cited by 5 | Viewed by 2903
Abstract
The local release of complexed siRNA from biomaterials opens precisely targeted therapeutic options. In this study, complexed siRNA was loaded to gelatin microparticles cross-linked (cGM) with an anhydride-containing oligomer (oPNMA). We aggregated these siRNA-loaded cGM with human mesenchymal stem cells (hMSC) to microtissues [...] Read more.
The local release of complexed siRNA from biomaterials opens precisely targeted therapeutic options. In this study, complexed siRNA was loaded to gelatin microparticles cross-linked (cGM) with an anhydride-containing oligomer (oPNMA). We aggregated these siRNA-loaded cGM with human mesenchymal stem cells (hMSC) to microtissues and stimulated them with osteogenic supplements. An efficient knockdown of chordin, a BMP-2 antagonist, caused a remarkably increased alkaline phosphatase (ALP) activity in the microtissues. cGM, as a component of microtissues, mineralized in a differentiation medium within 8–9 days, both in the presence and in the absence of cells. In order to investigate the effects of our pre-differentiated and chordin-silenced microtissues on bone homeostasis, we simulated in vivo conditions in an unstimulated co-culture system of hMSC and human peripheral blood mononuclear cells (hPBMC). We found enhanced ALP activity and osteoprotegerin (OPG) secretion in the model system compared to control microtissues. Our results suggest osteoanabolic effects of pre-differentiated and chordin-silenced microtissues. Full article
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15 pages, 3727 KiB  
Article
Enhanced Antimicrobial Action of Chlorhexidine Loaded in Shellac Nanoparticles with Cationic Surface Functionality
by Saba S. M. Al-Obaidy, Gillian M. Greenway and Vesselin N. Paunov
Pharmaceutics 2021, 13(9), 1389; https://doi.org/10.3390/pharmaceutics13091389 - 02 Sep 2021
Cited by 10 | Viewed by 2354
Abstract
We report on an active nanocarrier for chlorhexidine (CHX) based on sterically stabilized shellac nanoparticles (NPs) with dual surface functionalization, which greatly enhances the antimicrobial action of CHX. The fabrication process for the CHX nanocarrier is based on pH-induced co-precipitation of CHX-DG from [...] Read more.
We report on an active nanocarrier for chlorhexidine (CHX) based on sterically stabilized shellac nanoparticles (NPs) with dual surface functionalization, which greatly enhances the antimicrobial action of CHX. The fabrication process for the CHX nanocarrier is based on pH-induced co-precipitation of CHX-DG from an aqueous solution of ammonium shellac and Poloxamer 407 (P407), which serves as a steric stabilizing agent. This is followed by further surface modification with octadecyl trimethyl ammonium bromide (ODTAB) through a solvent change to yield cationic surface functionality. In this study, we assessed the encapsulation efficiency and release kinetics of the novel nanocarrier for CHX. We further examined the antimicrobial effects of the CHX nanocarriers and their individual components in order to gain better insight into how they work, to improve their design and to explore the impacts of their dual functionalization. The antimicrobial actions of CHX loaded in shellac NPs were examined on three different proxy microorganisms: a Gram-negative bacterium (E. coli), a yeast (S. cerevisiae) and a microalgae (C. reinhardtii). The antimicrobial actions of free CHX and CHX-loaded shellac NPs were compared over the same CHX concentration range. We found that the non-coated shellac NPs loaded with CHX showed inferior action compared with free CHX due to their negative surface charge; however, the ODTAB-coated, CHX-loaded shellac NPs strongly amplified the antimicrobial action of the CHX for the tested microorganisms. The enhancement of the CHX antimicrobial action was thought to be due to the increased electrostatic adhesion between the cationic surface of the ODTAB-coated, CHX-loaded shellac NPs and the anionic surface of the cell walls of the microorganisms, ensuring direct delivery of CHX with a high concentration locally on the cell membrane. The novel CHX nanocarriers with enhanced antimicrobial action may potentially find applications in dentistry for the development of more efficient formulations against conditions such as gingivitis, periodontitis and other oral infections, as well as enabling formulations to have lower CHX concentrations. Full article
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15 pages, 2705 KiB  
Article
Tunable Polyglycerol-Based Redox-Responsive Nanogels for Efficient Cytochrome C Delivery
by Sebastian Schötz, Felix Reisbeck, Ann-Cathrin Schmitt, Mathias Dimde, Elisa Quaas, Katharina Achazi and Rainer Haag
Pharmaceutics 2021, 13(8), 1276; https://doi.org/10.3390/pharmaceutics13081276 - 17 Aug 2021
Cited by 7 | Viewed by 2223
Abstract
The sensitivity of therapeutic proteins is a challenge for their use in biomedical applications, as they are prone to degradation and opsonization, thus limiting their potential. This demands for the development of drug delivery systems shielding proteins and releasing them at the site [...] Read more.
The sensitivity of therapeutic proteins is a challenge for their use in biomedical applications, as they are prone to degradation and opsonization, thus limiting their potential. This demands for the development of drug delivery systems shielding proteins and releasing them at the site of action. Here, we describe the synthesis of novel polyglycerol-based redox-responsive nanogels and report on their potential as nanocarrier systems for the delivery of cytochrome C (CC). This system is based on an encapsulation protocol of the therapeutic protein into the polymer network. NGs were formed via inverse nanoprecipitation using inverse electron-demand Diels–Alder cyclizations (iEDDA) between methyl tetrazines and norbornenes. Coprecipitation of CC led to high encapsulation efficiencies. Applying physiological reductive conditions of l-glutathione (GSH) led to degradation of the nanogel network, releasing 80% of the loaded CC within 48 h while maintaining protein functionality. Cytotoxicity measurements revealed high potency of CC-loaded NGs for various cancer cell lines with low IC50 values (up to 30 μg·mL−1), whereas free polymer was well tolerated up to a concentration of 1.50 mg·mL−1. Confocal laser scanning microscopy (CLSM) was used to monitor internalization of free and CC-loaded NGs and demonstrate the protein cargo’s release into the cytosol. Full article
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10 pages, 2310 KiB  
Article
Property-Tuneable Microgels Fabricated by Using Flow-Focusing Microfluidic Geometry for Bioactive Agent Delivery
by Wing-Fu Lai and Wing-Tak Wong
Pharmaceutics 2021, 13(6), 787; https://doi.org/10.3390/pharmaceutics13060787 - 25 May 2021
Cited by 62 | Viewed by 2706
Abstract
Gelatine methacryloyl (GM) shows high biocompatibility and is extensively used in tissue engineering; however, few works have explored the use of GM in bioactive agent delivery. This study adopts a microfluidic approach involving the use of flow-focusing microfluidic geometry for microgel fabrication. This [...] Read more.
Gelatine methacryloyl (GM) shows high biocompatibility and is extensively used in tissue engineering; however, few works have explored the use of GM in bioactive agent delivery. This study adopts a microfluidic approach involving the use of flow-focusing microfluidic geometry for microgel fabrication. This approach generates highly monodisperse microgels whose size can be tuned by altering various fabrication conditions (including the concentration of the gel-forming solution and the flow rates of different phases). By using tetracycline hydrochloride as a model agent, the fabricated microgels enable prolonged agent release, with the encapsulation efficiency being around 30–40% depending on the concentration of the gel-forming solution. Along with their negligible cytotoxicity, our microgels show the potential to serve as carriers of bioactive agents for food and pharmaceutical applications. Full article
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Review

Jump to: Editorial, Research

33 pages, 5353 KiB  
Review
Biopolymer-Based Nanogel Approach in Drug Delivery: Basic Concept and Current Developments
by Ebru Altuntaş, Burcu Özkan, Sevgi Güngör and Yıldız Özsoy
Pharmaceutics 2023, 15(6), 1644; https://doi.org/10.3390/pharmaceutics15061644 - 02 Jun 2023
Cited by 12 | Viewed by 2268
Abstract
Due to their increased surface area, extent of swelling and active substance-loading capacity and flexibility, nanogels made from natural and synthetic polymers have gained significant interest in scientific and industrial areas. In particular, the customized design and implementation of nontoxic, biocompatible, and biodegradable [...] Read more.
Due to their increased surface area, extent of swelling and active substance-loading capacity and flexibility, nanogels made from natural and synthetic polymers have gained significant interest in scientific and industrial areas. In particular, the customized design and implementation of nontoxic, biocompatible, and biodegradable micro/nano carriers makes their usage very feasible for a range of biomedical applications, including drug delivery, tissue engineering, and bioimaging. The design and application methodologies of nanogels are outlined in this review. Additionally, the most recent advancements in nanogel biomedical applications are discussed, with particular emphasis on applications for the delivery of drugs and biomolecules. Full article
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54 pages, 8011 KiB  
Review
Natural Gums in Drug-Loaded Micro- and Nanogels
by Anna Froelich, Emilia Jakubowska, Barbara Jadach, Piotr Gadziński and Tomasz Osmałek
Pharmaceutics 2023, 15(3), 759; https://doi.org/10.3390/pharmaceutics15030759 - 24 Feb 2023
Cited by 10 | Viewed by 2576
Abstract
Gums are polysaccharide compounds obtained from natural sources, such as plants, algae and bacteria. Because of their excellent biocompatibility and biodegradability, as well as their ability to swell and their sensitivity to degradation by the colon microbiome, they are regarded as interesting potential [...] Read more.
Gums are polysaccharide compounds obtained from natural sources, such as plants, algae and bacteria. Because of their excellent biocompatibility and biodegradability, as well as their ability to swell and their sensitivity to degradation by the colon microbiome, they are regarded as interesting potential drug carriers. In order to obtain properties differing from the original compounds, blends with other polymers and chemical modifications are usually applied. Gums and gum-derived compounds can be applied in the form of macroscopic hydrogels or can be formulated into particulate systems that can deliver the drugs via different administration routes. In this review, we present and summarize the most recent studies regarding micro- and nanoparticles obtained with the use of gums extensively investigated in pharmaceutical technology, their derivatives and blends with other polymers. This review focuses on the most important aspects of micro- and nanoparticulate systems formulation and their application as drug carriers, as well as the challenges related to these formulations. Full article
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26 pages, 1633 KiB  
Review
Thermoresponsive Chitosan-Grafted-Poly(N-vinylcaprolactam) Microgels via Ionotropic Gelation for Oncological Applications
by Lorenzo Marsili, Michele Dal Bo, Federico Berti and Giuseppe Toffoli
Pharmaceutics 2021, 13(10), 1654; https://doi.org/10.3390/pharmaceutics13101654 - 11 Oct 2021
Cited by 11 | Viewed by 2341
Abstract
Microgels can be considered soft, porous and deformable particles with an internal gel structure swollen by a solvent and an average size between 100 and 1000 nm. Due to their biocompatibility, colloidal stability, their unique dynamicity and the permeability of their architecture, they [...] Read more.
Microgels can be considered soft, porous and deformable particles with an internal gel structure swollen by a solvent and an average size between 100 and 1000 nm. Due to their biocompatibility, colloidal stability, their unique dynamicity and the permeability of their architecture, they are emerging as important candidates for drug delivery systems, sensing and biocatalysis. In clinical applications, the research on responsive microgels is aimed at the development of “smart” delivery systems that undergo a critical change in conformation and size in reaction to a change in environmental conditions (temperature, magnetic fields, pH, concentration gradient). Recent achievements in biodegradable polymer fabrication have resulted in new appealing strategies, including the combination of synthetic and natural-origin polymers with inorganic nanoparticles, as well as the possibility of controlling drug release remotely. In this review, we provide a literature review on the use of dual and multi-responsive chitosan-grafted-poly-(N-vinylcaprolactam) (CP) microgels in drug delivery and oncological applications. Full article
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