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Polymers for Therapy and Diagnostics

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A special issue of Polymers (ISSN 2073-4360).

Deadline for manuscript submissions: closed (31 March 2018) | Viewed by 70873

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Special Issue Editor

Prof. Dr. Marcelo Calderón

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Guest Editor

Institute for Chemistry and Biochemistry, Freie Universität Berlin, Takustr. 3, 14195 Berlin, Germany
Interests: biocompatible FRET-based imaging systems; multifunctional polymer-drug conjugates; environmentally responsive nanogel synthesis; self-assembling amphiphiles for controlled delivery of genes

Special Issue Information

Dear Colleagues,

As Guest Editor of the Special Issue entitled “Polymers for Therapy and Diagnostics” of Polymers, is my great pleasure to invite you to contribute to this issue with your most recent results in such a fascinating field of research.

This Special Issue is an attempt to summarize the developments in the field of polymer chemistry toward the preparation of advanced materials for the treatment and diagnosis of diseases. Reviews and research articles on different aspects of therapeutics, diagnosis, theranostics, and translation are invited for this Special Issue.

The official deadline for submission is 31 March, 2018. I look forward to receiving your contribution for the “Polymers for Therapy and Diagnostics” Special Issue in Polymers.

Prof. Dr. Marcelo Calderón
Guest Editor

Manuscript Submission Information

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

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.

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

Keywords

Nanomedicine
Theranostics
Translational medicine
Structure-activity relationship
Drug delivery systems
Smart materials

Published Papers (11 papers)

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Research

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23 pages, 2646 KiB

Open AccessArticle

Bioactive and Bioadhesive Catechol Conjugated Polymers for Tissue Regeneration

by María Puertas-Bartolomé, Blanca Vázquez-Lasa and Julio San Román

Polymers 2018, 10(7), 768; https://doi.org/10.3390/polym10070768 - 13 Jul 2018

Cited by 20 | Viewed by 6498

Abstract

The effective treatment of chronic wounds constitutes one of the most common worldwide healthcare problem due to the presence of high levels of proteases, free radicals and exudates in the wound, which constantly activate the inflammatory system, avoiding tissue regeneration. In this study, we describe a multifunctional bioactive and resorbable membrane with in-built antioxidant agent catechol for the continuous quenching of free radicals as well as to control inflammatory response, helping to promote the wound-healing process. This natural polyphenol (catechol) is the key molecule responsible for the mechanism of adhesion of mussels providing also the functionalized polymer with bioadhesion in the moist environment of the human body. To reach that goal, synthesized statistical copolymers of N-vinylcaprolactam (V) and 2-hydroxyethyl methacrylate (H) have been conjugated with catechol bearing hydrocaffeic acid (HCA) molecules with high yields. The system has demonstrated good biocompatibility, a sustained antioxidant response, an anti-inflammatory effect, an ultraviolet (UV) screen, and bioadhesion to porcine skin, all of these been key features in the wound-healing process. Therefore, these novel mussel-inspired materials have an enormous potential for application and can act very positively, favoring and promoting the healing effect in chronic wounds. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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15 pages, 2908 KiB

Open AccessArticle

pH-Responsive Hybrid Hydrogels as Antibacterial and Drug Delivery Systems

by Shabnam Sattari, Abbas Dadkhah Tehrani and Mohsen Adeli

Polymers 2018, 10(6), 660; https://doi.org/10.3390/polym10060660 - 13 Jun 2018

Cited by 59 | Viewed by 6520

Abstract

This study describes the design and synthesis of organic–inorganic hybrid hydrogels based on an interpenetrating polymer network (IPN) composed of polyaspartic acid crosslinked by graphene nanosheets as the primary network and poly(acrylamide-co-acrylic acid) as the secondary network. Silver, copper oxide, and zinc oxide nanoparticles were formed within the gel matrix, and the obtained hydrogel was applied to a load and controlled release of curcumin. The loading of curcumin and the release of this drug from the gels depended on the nanoparticle’s (NP’s) content of hydrogels as well as the pH of the medium. The synthesized hydrogels showed antibacterial activity against E. coli and S. aureus bacteria. The ability of the synthesized hydrogels to incapacitate bacteria and their loading capacity and controlled release of curcumin qualify them for future therapies such as wound-dressing applications. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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13 pages, 5889 KiB

Open AccessArticle

Soy-Based Soft Matrices for Encapsulation and Delivery of Hydrophilic Compounds

by Ruvimbo Chitemere, Shane Stafslien, Long Jiang, Dean Webster and Mohiuddin Quadir

Polymers 2018, 10(6), 583; https://doi.org/10.3390/polym10060583 - 26 May 2018

Cited by 3 | Viewed by 3237

Abstract

A new controlled-release platform for hydrophilic compounds has been developed, utilizing citric acid-cured epoxidized sucrose soyate (ESS) as the matrix forming material. By cross-linking epoxy groups of ESS with citric acid in the presence of a hydrophilic model molecule, sodium salt of fluorescein (Sod-FS), we were able to entrap the latter homogenously within the ESS matrix. No chemical change of the entrapped active agent was evident during the fabrication process. Hydrophobicity of the matrix was found to be the rate-limiting factor for sustaining the release of the hydrophilic model compound, while inclusion of release-modifiers such as poly(ethylene glycol) (PEG) within the matrix system modulated the rate and extent of guest release. Using 5 kDa PEG at 5% w/w of the total formulation, it was possible to extend the release of the active ingredient for more than a month. In addition, the amount of modifiers in formulations also influenced the mechanical properties of the matrices, including loss and storage modulus. Mechanism of active release from ESS matrices was also evaluated using established kinetic models. Formulations composed entirely of ESS showed a non-Fickian (anomalous) release behavior while Fickian (Case I) transport was the predominant mechanism of active release from ESS systems containing different amount of PEGs. The mean dissolution time (MDT) of the hydrophilic guest molecule from within the ESS matrix was found to be a function of the molecular weight and the amount of PEG included. At the molecular level, we observed no cellular toxicities associated with ESS up to a concentration level of 10 μM. We envision that such fully bio-based matrices can find applications in compounding point-of-care, extended-release formulations of highly water-soluble active agents. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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22 pages, 4224 KiB

Open AccessArticle

Molecular Weight-Dependent Activity of Aminated Poly(α)glutamates as siRNA Nanocarriers

by Adva Krivitsky, Vadim Krivitsky, Dina Polyak, Anna Scomparin, Shay Eliyahu, Hadas Gibori, Eilam Yeini, Evgeni Pisarevsky, Rachel Blau and Ronit Satchi-Fainaro

Polymers 2018, 10(5), 548; https://doi.org/10.3390/polym10050548 - 20 May 2018

Cited by 7 | Viewed by 4471

Abstract

RNA interference (RNAi) can contribute immensely to the area of personalized medicine by its ability to target any gene of interest. Nevertheless, its clinical use is limited by lack of efficient delivery systems. Polymer therapeutics can address many of the challenges encountered by the systemic delivery of RNAi, but suffer from inherent drawbacks such as polydispersity and batch to batch heterogeneity. These characteristics may have far-reaching consequences when dealing with therapeutic applications, as both the activity and the toxicity may be dependent on the length of the polymer chain. To investigate the consequences of polymers’ heterogeneity, we have synthesized two batches of aminated poly(α)glutamate polymers (PGAamine), differing in their degree of polymerization, but not in the monomer units or their conjugation. Isothermal titration calorimetry study was conducted to define the binding affinity of these polymers with siRNA. Molecular dynamics simulation revealed that Short PGAamine:siRNA polyplexes exposed a higher amount of amine moieties to the surroundings compared to Long PGAamine. This resulted in a higher zeta potential, leading to faster degradation and diminished gene silencing. Altogether, our study highlights the importance of an adequate physico-chemical characterization to elucidate the structure–function-activity relationship, for further development of tailor-designed RNAi delivery vehicles. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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14 pages, 10233 KiB

Open AccessFeature PaperArticle

A Facile, One-Pot, Surfactant-Free Nanoprecipitation Method for the Preparation of Nanogels from Polyglycerol–Drug Conjugates that Can Be Freely Assembled for Combination Therapy Applications

by Laura I. Vossen, Stefanie Wedepohl and Marcelo Calderón

Polymers 2018, 10(4), 398; https://doi.org/10.3390/polym10040398 - 03 Apr 2018

Cited by 14 | Viewed by 6650

Abstract

A well-established strategy to treat drug resistance is the use of multiple therapeutics. Polymer-based drug delivery systems (DDS) can facilitate a simultaneous delivery of two or more drugs. In this study, we developed and synthesized a dendritic polyglycerol (PG) nanogel (NG) system that allows for free combination of different fixed ratios of active compound conjugates within a single NG particle. As a proof of concept, we synthesized NGs bearing the chemotherapeutic agent doxorubicin (DOX) and paclitaxel (PTX) in different ratios, as well as conjugated dye molecules. Our combination PG NGs were formed by simply mixing PG–drug/dye conjugates bearing free thiol groups with PG-acrylate in an inverse surfactant-free nanoprecipitation method. With this method we obtained PG-NGs in the size range of 110–165 nm with low polydispersity indices. Solubility of hydrophobic PTX was improved without the need for additional solubilizing agents such as polyethylene glycol (PEG). Interestingly, we found that our NGs made from PG-DOX conjugates have a high quenching efficiency for DOX, which could be interesting for theranostic purposes. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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11 pages, 4624 KiB

Open AccessArticle

Conjugate of PAMAM Dendrimer, Doxorubicin and Monoclonal Antibody—Trastuzumab: The New Approach of a Well-Known Strategy

by Monika Marcinkowska, Ewelina Sobierajska, Maciej Stanczyk, Anna Janaszewska, Arkadiusz Chworos and Barbara Klajnert-Maculewicz

Polymers 2018, 10(2), 187; https://doi.org/10.3390/polym10020187 - 14 Feb 2018

Cited by 38 | Viewed by 6041

Abstract

The strategy utilizing trastuzumab, a humanized monoclonal antibody against human epidermal growth receptor 2 (HER-2), as a therapeutic agent in HER-2 positive breast cancer therapy seems to have advantage over traditional chemotherapy, especially when given in combination with anticancer drugs. However, the effectiveness of single antibody or antibody conjugated with chemotherapeutics is still far from ideal. Antibody–dendrimer conjugates hold the potential to improve the targeting and release of active substance at the tumor site. In the present study, we developed and synthesized PAMAM dendrimer–trastuzumab conjugates carrying doxorubicin (dox) specifically to cells overexpressing HER-2. ¹HNMR, FTIR and RP-HPLC were used to characterize the products and analyze their purity. Toxicity of PAMAM–trastuzumab and PAMAM–dox–trastuzumab conjugates compared with free trastuzumab and doxorubicin towards HER-2 positive (SKBR-3) and negative (MCF-7) human breast cancer cell lines was determined using MTT assay. Furthermore, the cellular uptake and cellular localization were studied by flow cytometry and confocal microscopy, respectively. A cytotoxicity profile of above mentioned compounds indicated that conjugate PAMAM–dox–trastuzumab was more effective when compared to free drug or the conjugate PAMAM–trastuzumab. Moreover, these results reveal that trastuzumab can be used as a targeting agent in PAMAM–dox–trastuzumab conjugate. Therefore PAMAM–dox–trastuzumab conjugate might be an interesting proposition which could lead to improvements in the effectiveness of drug delivery systems for tumors that overexpress HER-2. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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16 pages, 5041 KiB

Open AccessArticle

Microencapsulation of Phosphorylated Human-Like Collagen-Calcium Chelates for Controlled Delivery and Improved Bioavailability

by Yu Mi, Zhengfang Liu, Jianjun Deng, Huan Lei, Chenhui Zhu, Daidi Fan and Xingqiang Lv

Polymers 2018, 10(2), 185; https://doi.org/10.3390/polym10020185 - 14 Feb 2018

Cited by 9 | Viewed by 3736

Abstract

The bioavailability of Phosphorylated Human-like Collagen-calcium chelates (PHLC-Ca) as calcium supplement is influenced by the extremely low pH and proteolytic enzymes in the gastrointestinal tract. This study addresses these issues by microencapsulation technology using alginate (ALG) and chitosan (CS) as wall materials. The different ratio of ALG to PHLC-Ca on microcapsules encapsulation efficiency (EE) and loading capacity (LC) was evaluated and 1:1/2 was selected as the optimal proportion. The microcapsules were micron-sized and spherical in shape. PHLC-Ca was successfully entrapped into the matrix of ALG through forming intermolecular hydrogen bonding or other interactions. The confocal laser scanning microscopy (CLSM) indicated that CS was coated on ALG microspheres. The MTT assay exhibited that CS/ALG-(PHLC-Ca) microcapsules extracts were safe to L929. The animal experiment showed that CS/ALG-(PHLC-Ca) microcapsules was superior to treating osteoporosis than PHLC-Ca. These results illustrated that the bioavailability of PHLC-Ca was improved by microencapsulated. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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25 pages, 6987 KiB

Open AccessArticle

Site-Specific DBCO Modification of DEC205 Antibody for Polymer Conjugation

by Simone Beck, Jennifer Schultze, Hans-Joachim Räder, Regina Holm, Meike Schinnerer, Matthias Barz, Kaloian Koynov and Rudolf Zentel

Polymers 2018, 10(2), 141; https://doi.org/10.3390/polym10020141 - 02 Feb 2018

Cited by 13 | Viewed by 11616

Abstract

The design of multifunctional polymer-based vectors, forming pDNA vaccines, offers great potential in cancer immune therapy. The transfection of dendritic immune cells (DCs) with tumour antigen-encoding pDNA leads to an activation of the immune system to combat tumour cells. In this work, we investigated the chemical attachment of DEC205 antibodies (aDEC205) as DC-targeting structures to polyplexes of P(Lys)-b-P(HPMA). The conjugation of a synthetic block copolymer and a biomacromolecule with various functionalities (aDEC205) requires bioorthogonal techniques to avoid side reactions. Click chemistry and in particular the strain-promoted alkyne-azide cycloaddition (SPAAC) can provide the required bioorthogonality. With regard to a SPAAC of both components, we firstly synthesized two different azide-containing block copolymers, P(Lys)-b-P(HPMA)-N₃(stat) and P(Lys)-b-P(HPMA)-N₃(end), for pDNA complexation. In addition, the site-specific incorporation of ring-strained dibenzocyclooctyne (DBCO) moieties to the DEC205 antibody was achieved by an enzymatic strategy using bacterial transglutaminase (BTG). The chemical accessibility of DBCO molecules within aDEC205 as well as the accessibility of azide-functionalities on the polyplex’ surface were investigated by various SPAAC experiments and characterized by fluorescence correlation spectroscopy (FCS). Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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16 pages, 5122 KiB

Open AccessArticle

Poly(carbonate urethane)-Based Thermogels with Enhanced Drug Release Efficacy for Chemotherapeutic Applications

by Benjamin Qi Yu Chan, Hongwei Cheng, Sing Shy Liow, Qingqing Dou, Yun-Long Wu, Xian Jun Loh and Zibiao Li

Polymers 2018, 10(1), 89; https://doi.org/10.3390/polym10010089 - 18 Jan 2018

Cited by 30 | Viewed by 5547

Abstract

In this study, we report the synthesis and characterisation of a thermogelling poly(carbonate urethane) system comprising poly(ethylene glycol) (PEG), poly(propylene glycol) (PPG) and poly(polytetrahydrofuran carbonate) (PTHF carbonate). The incorporation of PTHF carbonate allowed for the control of the lower critical solution temperature (LCST) and decreased critical gelation concentration (CGC) of the thermogels significantly. In addition, the as-prepared thermogels displayed low toxicity against HepG2, L02 and HEK293T cells. Drug release studies were carried out using doxorubicin (Dox). Studies conducted using nude mice models with hepatocellular carcinoma revealed that the Dox-loaded poly(PEG/PPG/PTHF carbonate urethane) thermogels showed excellent in vivo anti-tumour performance and effectively inhibited tumour growth in the tested model. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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11 pages, 1317 KiB

Open AccessReview

Dendritic Polyglycerol Sulfate for Therapy and Diagnostics

by Nadine Rades, Kai Licha and Rainer Haag

Polymers 2018, 10(6), 595; https://doi.org/10.3390/polym10060595 - 29 May 2018

Cited by 19 | Viewed by 5645

Abstract

Dendritic polyglycerol sulfate (dPGS) has originally been investigated as an anticoagulant to potentially substitute for the natural glycosaminoglycan heparin. Compared to unfractionated heparin, dPGS possesses lower anticoagulant activity but a much higher anticomplementary effect. Since coagulation, complement activation, and inflammation are often present in the pathophysiology of numerous diseases, dPGS polymers with both anticoagulant and anticomplementary activities represent promising candidates for the development of polymeric drugs of nanosized architecture. In this review, we describe the nanomedical applications of dPGS based on its anti-inflammatory activity. Furthermore, the application of dPGS as a carrier molecule for diagnostic molecules and therapeutic drugs is reviewed, based on the ability to target tumors and localize in tumor cells. Finally, the application of dPGS for inhibition of virus infections is described. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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34 pages, 7675 KiB

Open AccessReview

Design, Synthesis and Architectures of Hybrid Nanomaterials for Therapy and Diagnosis Applications

by Micaela A. Macchione, Catalina Biglione and Miriam Strumia

Polymers 2018, 10(5), 527; https://doi.org/10.3390/polym10050527 - 14 May 2018

Cited by 59 | Viewed by 10094

Abstract

Hybrid nanomaterials based on inorganic nanoparticles and polymers are highly interesting structures since they combine synergistically the advantageous physical-chemical properties of both inorganic and polymeric components, providing superior functionality to the final material. These unique properties motivate the intensive study of these materials from a multidisciplinary view with the aim of finding novel applications in technological and biomedical fields. Choosing a specific synthetic methodology that allows for control over the surface composition and its architecture, enables not only the examination of the structure/property relationships, but, more importantly, the design of more efficient nanodevices for therapy and diagnosis in nanomedicine. The current review categorizes hybrid nanomaterials into three types of architectures: core-brush, hybrid nanogels, and core-shell. We focus on the analysis of the synthetic approaches that lead to the formation of each type of architecture. Furthermore, most recent advances in therapy and diagnosis applications and some inherent challenges of these materials are herein reviewed. Full article

(This article belongs to the Special Issue Polymers for Therapy and Diagnostics)

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