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Molecular Hydrodynamics, Optics and Electro-Optics of Biological and Synthetic Polymers and Their Complexes in Solutions

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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Physics and Theory".

Deadline for manuscript submissions: closed (30 November 2022) | Viewed by 9300

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Prof. Dr. Nikolay Tsvetkov

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Department of Molecular Biophysics and Polymer Physics, Physical Faculty, St. Petersburg State University, 199034 St. Petersburg, Russia
Interests: molecular hydrodynamics, optics and electro-optics of biological and synthetic polymer and dendrimer solutions; the structure and properties of the polyelectrolyte and polymer-colloid complexes; self-assembly in polymer systems

Special Issue Information

Dear Colleagues,

This Special Issue focuses on the current state-of-the-art of physico-chemistry of polymers and their complexes in solution. The development and design of new polymer materials requires a detailed and comprehensive understanding of the fundamental relationships between the properties of macromolecules and polymer materials. Therefore, studies of macromolecules in solutions using a complex of various complementary analytical methods (including methods of hydrodynamics, optics and electro-optics, etc.) are important not only from a fundamental scientific, but also from a practical point of view. In addition, many polymers are used directly in solutions, for example, in medicine, pharmacology, organic synthesis, etc., therefore, a deep knowledge of their characteristics in solutions and the ability of these polymers to self-organization are extremely important.

The scope of the Special Issue therefore encompasses the characterization of different types of bio- and synthetic polymers as well as their complexes with other polymers and with low molecular weight agents, as well as with various nanoparticles in solutions. Articles on the study of polymers with unusual designs, such as hyper-branched and regularly branched (dendritic) systems, as well as polymer systems that can be used in drug delivery, including various polymer micelles, etc. are especially welcome. The characterization and properties of polyelectrolyte systems are also the focus of this Issue. In addition, we welcome articles proposing new methods or approaches in the study of macromolecular systems in solutions, both experimental and theoretical.

Thus, the scope of the Special Issue includes the synthesis and characterization of polymers of various polymers and their complexes in solutions using modern advanced techniques and approaches. We will be grateful to the authors who have sent their original articles, as well as analytical reviews, on the subject of the Special Issue.

Prof. Dr. Nikolay Tsvetkov
Guest Editor

Manuscript Submission Information

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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. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

structure and design of polymers in solution
polymers: biopolymers, synthetic polymers, dendrimers, polyelectrolytes
self-assembly and aggregation of polymer systems
polymer complexes, polymer micelles
conformation of polymer molecules
hydrodynamic properties
optical and electro-optical properties
analytical ultracentrifugation
viscometry/rheology
dynamic and static light scattering

Published Papers (5 papers)

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Research

17 pages, 2266 KiB

Open AccessArticle

Conformational Parameters and Hydrodynamic Behavior of Poly(2-Methyl-2-Oxazoline) in a Broad Molar Mass Range

by Alexander S. Gubarev, Alexey A. Lezov, Anna N. Podsevalnikova, Nina G. Mikusheva, Petr A. Fetin, Ivan M. Zorin, Vladimir O. Aseyev, Ondrej Sedlacek, Richard Hoogenboom and Nikolai V. Tsvetkov

Polymers 2023, 15(3), 623; https://0-doi-org.brum.beds.ac.uk/10.3390/polym15030623 - 25 Jan 2023

Cited by 3 | Viewed by 1856

Abstract

In this work, we report our results on the hydrodynamic behavior of poly(2-methyl-2-oxazoline) (PMeOx). PMeOx is gaining significant attention for use as hydrophilic polymer in pharmaceutical carriers as an alternative for the commonly used poly(ethylene glycol) (PEG), for which antibodies are found in a significant fraction of the human population. The main focus of the current study is to determine the hydrodynamic characteristics of PMeOx under physiological conditions, which serves as basis for better understanding of the use of PMeOx in pharmaceutical applications. This goal was achieved by studying PMeOx solutions in phosphate-buffered saline (PBS) as a solvent at 37 °C. This study was performed based on two series of PMeOx samples; one series is synthesized by conventional living cationic ring-opening polymerization, which is limited by the maximum chain length that can be achieved, and a second series is obtained by an alternative synthesis strategy based on acetylation of well-defined linear poly(ethylene imine) (PEI) prepared by controlled side-chain hydrolysis of a defined high molar mass of poly(2-ethyl-2-oxazoline). The combination of these two series of PMeOx allowed the determination of the Kuhn–Mark–Houwink–Sakurada equations in a broad molar mass range. For intrinsic viscosity, sedimentation and diffusion coefficients, the following expressions were obtained:

[η] = 0.015 M^{0.77}

s_{0} = 0.019 M^{0.42}

and

D_{0} = 2600 M^{- 0.58}

, respectively. As a result, it can be concluded that the phosphate-buffered saline buffer at 37 °C represents a thermodynamically good solvent for PMeOx, based on the scaling indices of the equations. The conformational parameters for PMeOx chains were also determined, revealing an equilibrium rigidity or Kuhn segment length, (A) of 1.7 nm and a polymer chain diameter (d) of 0.4 nm. The obtained value for the equilibrium rigidity is very similar to the reported values for other hydrophilic polymers, such as PEG, poly(vinylpyrrolidone) and poly(2-ethyl-2-oxazoline), making PMeOx a relevant alternative to PEG. Full article

(This article belongs to the Special Issue Molecular Hydrodynamics, Optics and Electro-Optics of Biological and Synthetic Polymers and Their Complexes in Solutions)

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20 pages, 4792 KiB

Open AccessArticle

DNA Conformational Changes Induced by Its Interaction with Binuclear Platinum Complexes in Solution Indicate the Molecular Mechanism of Platinum Binding

by Nina Kasyanenko, Zhang Qiushi, Vladimir Bakulev, Petr Sokolov and Konstantin Yakovlev

Polymers 2022, 14(10), 2044; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14102044 - 17 May 2022

Cited by 3 | Viewed by 1575

Abstract

Platinum anticancer drugs inhibit the division of cancer cells through a DNA binding mechanism. The bimetallic platinum compounds have a possibility for blocking DNA replication via the cross-linking of DNA functional groups at different distances. Many compounds with metals of the platinum group have been tested for possible antitumor activity. The main target of their biological action is a DNA molecule. A combined approach to the study of the interaction of DNA with biologically active compounds of this type is proposed. The capabilities of various methods (hydrodynamic, spectral, microscopy) in obtaining information on the type of binding of coordination compounds to DNA are compared. The analysis of DNA binding with platinum binuclear compounds containing pyrazine, tetrazole, 5- methyltetrazole, 3-propanediamine as bridging ligands in a solution was carried out with the methods of circular dichroism (CD), luminescent spectroscopy (LS), low gradient viscometry (LGV), flow birefringence (FB) and atomic force microscopy (AFM). The competitive binding of different platinum compounds to DNA and the analysis of platinum attachment to DNA after protonation of its nitrogen bases simply indicates the involvement of N7 guanine in binding. Fluorescent dye DAPI was also used to recognize the location of platinum compounds in DNA grooves. DNA conformational changes recorded by variations in persistent length, polyelectrolyte swelling, DNA secondary structure, and its stability clarify the molecular mechanism of the biological activity of platinum compounds. Full article

(This article belongs to the Special Issue Molecular Hydrodynamics, Optics and Electro-Optics of Biological and Synthetic Polymers and Their Complexes in Solutions)

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16 pages, 1638 KiB

Open AccessFeature PaperArticle

Hydrodynamic Characteristics and Conformational Parameters of Ferrocene-Terpyridine-Based Polymers

by Alexander S. Gubarev, Alexey A. Lezov, Nina G. Mikusheva, Igor Perevyazko, Anna S. Senchukova, Alexandra A. Lezova, Anna N. Podsevalnikova, Vyacheslav B. Rogozhin, Marcel Enke, Andreas Winter, Ulrich S. Schubert and Nikolai V. Tsvetkov

Polymers 2022, 14(9), 1776; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14091776 - 27 Apr 2022

Cited by 3 | Viewed by 1752

Abstract

Nowadays, the study of metallopolymers is one of the fastest growing areas of polymer science. Metallopolymers have great potential for application in multiple technological and various biomedical processes. The macromolecules with the possibility of varying the number and type of metal ions along the entire length of the polymer chain are of particular interest. In this regard, this study presents results on two successfully synthesized homopolymers, random and block copolymers based on PMMA, containing ferrocene and terpyridine moieties in the side chain. Different architectures of copolymers may attribute interesting properties when creating complexes with various metal ions. A detailed hydrodynamic study of these structures was carried out, the consistency of hydrodynamic data was established using the concept of a hydrodynamic invariant, the absolute values of the molar masses of the studied objects were calculated, and the conformational parameters of macromolecules were determined. Using the Fixman–Stockmayer theory, the equilibrium rigidities of the studied systems were calculated and the relationship between the chemical structure and conformational characteristics was established. The studied copolymers can be attributed to the class of flexible-chain macromolecules. An increase in the equilibrium rigidity value with an increase of the side chain, which is characteristic of comb-shaped polymers, was determined. Full article

(This article belongs to the Special Issue Molecular Hydrodynamics, Optics and Electro-Optics of Biological and Synthetic Polymers and Their Complexes in Solutions)

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18 pages, 5988 KiB

Open AccessArticle

Metallo-Supramolecular Complexation Behavior of Terpyridine- and Ferrocene-Based Polymers in Solution—A Molecular Hydrodynamics Perspective

by Igor Perevyazko, Nina Mikusheva, Alexey Lezov, Alexander Gubarev, Marcel Enke, Andreas Winter, Ulrich S. Schubert and Nikolay Tsvetkov

Polymers 2022, 14(5), 944; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14050944 - 26 Feb 2022

Cited by 2 | Viewed by 1850

Abstract

The contribution deals with the synthesis of the poly(methacrylate)-based copolymers, which contain ferrocene and/or terpyridine moieties in the side chains, and the subsequent analysis of their self-assembly behavior upon supramolecular/coordination interactions with Eu³⁺ and Pd²⁺ ions in dilute solutions. Both metal ions provoke intra and inter molecular complexation that results in the formation of large supra-macromolecular assembles of different conformation/shapes. By applying complementary analytical approaches (i.e., sedimentation-diffusion analysis in the analytical ultracentrifuge, dynamic light scattering, viscosity and density measurements, morphology studies by electron microscopy), a map of possible conformational states/shapes was drawn and the corresponding fundamental hydrodynamic and macromolecular characteristics of metallo-supramolecular assemblies at various ligand-to-ion molar concentration ratios (

M / L

) in extremely dilute polymer solutions

(c [η] \approx 0.006)

were determined. It was shown that intramolecular complexation is already detected at (

L \approx 0.1

), while at

M / L > 0.5

solution/suspension precipitates. Extreme aggregation/agglomeration behavior of such dilute polymer solutions at relatively “high” metal ion content is explained from the perspective of polymer-solvent and charge interactions that will accompany the intramolecular complexation due to the coordination interactions. Full article

(This article belongs to the Special Issue Molecular Hydrodynamics, Optics and Electro-Optics of Biological and Synthetic Polymers and Their Complexes in Solutions)

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12 pages, 1826 KiB

Open AccessArticle

Conformation, Self-Organization and Thermoresponsibility of Polymethacrylate Molecular Brushes with Oligo(ethylene glycol)-block-oligo(propylene glycol) Side Chains

by Maria Simonova, Denis Kamorin, Oleg Kazantsev, Maria Nepomnyashaya and Alexander Filippov

Polymers 2021, 13(16), 2715; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13162715 - 13 Aug 2021

Cited by 9 | Viewed by 1568

Abstract

Polymethacrylic molecular brushes with oligo(ethylene glycol)-block-oligo(propylene glycol) side chains were investigated by static and dynamic light scattering and viscometry. The solvents used were acetonitrile, tetrahydrofuran, chloroform, and water. The grafted copolymers were molecularly dispersed and dissolved in tetrahydrofuran and acetonitrile. In these solvents, the molar masses of copolymers were determined. In thermodynamically good solvents, namely tetrahydrofuran and acetonitrile, investigated copolymers have a high intramolecular density and the shape of their molecules resembles a star-shaped macromolecule. In chloroform and water, the micelle-like aggregates were formed. Critical micelle concentrations decreased with the lengthening of the hydrophobic block. Molecular brushes demonstrated thermosensitive behavior in aqueous solutions. The phase separation temperatures reduced with an increase in the content of the oligo(propylene glycol) block. Full article

(This article belongs to the Special Issue Molecular Hydrodynamics, Optics and Electro-Optics of Biological and Synthetic Polymers and Their Complexes in Solutions)

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