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Molecules
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The Progresses on Polyelectrolytes and Polyelectrolyte Complexes
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The Progresses on Polyelectrolytes and Polyelectrolyte Complexes

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Physical Chemistry".

Deadline for manuscript submissions: closed (30 November 2019) | Viewed by 19926

Special Issue Editor

Dr. Jens Smiatek

E-Mail Website
Guest Editor
Institute for Computational Physics, University of Stuttgart, 70569 Stuttgart, Germany
Interests: charged objects in solution: polyelectrolytes and ions; dynamic and structural properties of complex electrolyte solutions; molecular theories of solvation: solvation principles and thermodynamic effects; co-solute and specific ion effects and their influence on macromolecular folding equilibria
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Polyelectrolytes are ubiquitous in many technological applications as well as in biological systems. Despite their importance, however, many of their properties are poorly understood. Our lack of understanding is largely due to the charge of the polyelectrolyte, which causes long-ranging electrostatic interactions and thus considerably complicates the development of more accurate models and theories. Moreover, the presence of other components as well as the influence of external fields leads to a multitude of interesting effects and complex mechanisms that massively influence the dynamics and the structure of polyelectrolytes. Important examples here are, in particular, the formation of polyelectrolyte complexes, the dissociation properties of weak polyelectrolytes, the distribution of mobile ions in the solution, the occurrence of specific ion effects and the influence of counterions on the polyelectrolyte dynamics. This Special Issue of Molecules is intended to provide an up-to-date overview of new results and the current state of knowledge in polyelectrolyte research. The corresponding experimental, theoretical, and numerical research results can cover a broad range of topics from applications of polyelectrolytes in electrochemical energy storage systems to studies of DNA structures.

Dr. Jens Smiatek
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. Molecules 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

  • Polyelectrolyte Solutions and Polyionic Liquids
  • Polyelectrolyte Complexes and Multilayers
  • Polyelectrolyte Membranes
  • Weak and Strong Polyelectrolytes
  • Polyelectrolyte – Ion Interactions
  • Specific Ion and Additive Effects
  • Counterion Condensation
  • Biological Systems: DNA and RNA
  • Electrochemical Applications and Ion Transport Mechanisms
  • Polyelectrolyte Electrophoresis and Dynamics

Published Papers (5 papers)

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Research

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17 pages, 3520 KiB  
Article
Comparing Zwitterionic and PEG Exteriors of Polyelectrolyte Complex Micelles
by Jeffrey M. Ting, Alexander E. Marras, Joseph D. Mitchell, Trinity R. Campagna and Matthew V. Tirrell
Molecules 2020, 25(11), 2553; https://doi.org/10.3390/molecules25112553 - 30 May 2020
Cited by 9 | Viewed by 5882
Abstract
A series of model polyelectrolyte complex micelles (PCMs) was prepared to investigate the consequences of neutral and zwitterionic chemistries and distinct charged cores on the size and stability of nanocarriers. Using aqueous reversible addition-fragmentation chain transfer (RAFT) polymerization, we synthesized a well-defined diblock [...] Read more.
A series of model polyelectrolyte complex micelles (PCMs) was prepared to investigate the consequences of neutral and zwitterionic chemistries and distinct charged cores on the size and stability of nanocarriers. Using aqueous reversible addition-fragmentation chain transfer (RAFT) polymerization, we synthesized a well-defined diblock polyelectrolyte system, poly(2-methacryloyloxyethyl phosphorylcholine methacrylate)-block-poly((vinylbenzyl) trimethylammonium) (PMPC-PVBTMA), at various neutral and charged block lengths to compare directly against PCM structure–property relationships centered on poly(ethylene glycol)-block-poly((vinylbenzyl) trimethylammonium) (PEG-PVBTMA) and poly(ethylene glycol)-block-poly(l-lysine) (PEG-PLK). After complexation with a common polyanion, poly(sodium acrylate), the resulting PCMs were characterized by dynamic light scattering (DLS) and small angle X-ray scattering (SAXS). We observed uniform assemblies of spherical micelles with a diameter ~1.5–2× larger when PMPC-PVBTMA was used compared to PEG-PLK and PEG-PVBTMA via SAXS and DLS. In addition, PEG-PLK PCMs proved most resistant to dissolution by both monovalent and divalent salt, followed by PEG-PVBTMA then PMPC-PVBTMA. All micelle systems were serum stable in 100% fetal bovine serum over the course of 8 h by time-resolved DLS, demonstrating minimal interactions with serum proteins and potential as in vivo drug delivery vehicles. This thorough study of the synthesis, assembly, and characterization of zwitterionic polymers in PCMs advances the design space for charge-driven micelle assemblies. Full article
(This article belongs to the Special Issue The Progresses on Polyelectrolytes and Polyelectrolyte Complexes)
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16 pages, 3916 KiB  
Article
PDADMAC/PSS Oligoelectrolyte Multilayers: Internal Structure and Hydration Properties at Early Growth Stages from Atomistic Simulations
by Pedro A. Sánchez, Martin Vögele, Jens Smiatek, Baofu Qiao, Marcello Sega and Christian Holm
Molecules 2020, 25(8), 1848; https://doi.org/10.3390/molecules25081848 - 17 Apr 2020
Cited by 5 | Viewed by 2714
Abstract
We analyze the internal structure and hydration properties of poly(diallyl dimethyl ammonium chloride)/poly(styrene sulfonate sodium salt) oligoelectrolyte multilayers at early stages of their layer-by-layer growth process. Our study is based on large-scale molecular dynamics simulations with atomistic resolution that we presented recently [Sánchez [...] Read more.
We analyze the internal structure and hydration properties of poly(diallyl dimethyl ammonium chloride)/poly(styrene sulfonate sodium salt) oligoelectrolyte multilayers at early stages of their layer-by-layer growth process. Our study is based on large-scale molecular dynamics simulations with atomistic resolution that we presented recently [Sánchez et al., Soft Matter 2019, 15, 9437], in which we produced the first four deposition cycles of a multilayer obtained by alternate exposure of a flat silica substrate to aqueous electrolyte solutions of such polymers at 0.1M of NaCl. In contrast to any previous work, here we perform a local structural analysis that allows us to determine the dependence of the multilayer properties on the distance to the substrate. We prove that the large accumulation of water and ions next to the substrate observed in previous overall measurements actually decreases the degree of intrinsic charge compensation, but this remains as the main mechanism within the interface region. We show that the range of influence of the substrate reaches approximately 3 nm, whereas the structure of the outer region is rather independent from the position. This detailed characterization is essential for the development of accurate mesoscale models able to reach length and time scales of technological interest. Full article
(This article belongs to the Special Issue The Progresses on Polyelectrolytes and Polyelectrolyte Complexes)
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18 pages, 3272 KiB  
Article
The Anomalous Influence of Polyelectrolyte Concentration on the Deposition and Nanostructure of Poly(ethyleneimine)/Poly(acrylic acid) Multilayers
by Martin Müller
Molecules 2019, 24(11), 2141; https://doi.org/10.3390/molecules24112141 - 06 Jun 2019
Cited by 11 | Viewed by 2860
Abstract
The deposition and nanostructure of polyelectrolyte (PEL) multilayers (PEMs) of branched poly(ethyleneimine)/poly(acrylic acid) (PEI/PAA) onto silicon substrates was studied in terms of the dependence of pH and the PEL concentration (cPEL) in the individual adsorption steps z. Both a commercial automatic [...] Read more.
The deposition and nanostructure of polyelectrolyte (PEL) multilayers (PEMs) of branched poly(ethyleneimine)/poly(acrylic acid) (PEI/PAA) onto silicon substrates was studied in terms of the dependence of pH and the PEL concentration (cPEL) in the individual adsorption steps z. Both a commercial automatic dipping device and a homebuilt automatic stream coating device (flow cell) were used. Gravimetry, SFM, transmission (TRANS) and in situ attenuated total reflection (ATR) FTIR spectroscopy were used for the quantitative determination of the adsorbed amount, thickness, chemical composition and morphology of deposited PEMs, respectively. Firstly, the combination of pH = 10 for PEI and pH = 4 for PAA, where both PEL were predominantly in the neutral state, resulted in an extraordinarily high PEM deposition, while pH combinations, where one PEL component was charged, resulted in a significantly lower PEM deposition. This was attributed to both PEL conformation effects and acid/base interactions between basic PEI and acidic PAA. Secondly, for that pH combination an exponential relationship between PEM thickness and adsorption step z was found. Thirdly, based on the results of three independent methods, the course of the deposited amount of a PEM-10 (z = 10) versus cPEL in the range 0.001 to 0.015 M at pH = 10/4 was non-monotonous showing a pronounced maximum at cPEL = 0.005 M. Analogously, for cPEL = 0.005 M a maximum of roughness and structure size was found. Fourthly, related to that finding, in situ ATR-FTIR measurements gave evidence for the release of outermost located PEI upon PAA immersion (even step) and of outermost PAA upon PEI immersion (odd step) under formation of PEL complexes in solution. These studies help us to prepare PEL-based films with a defined thickness and morphology for interaction with biofluids in the biomedical and food fields. Full article
(This article belongs to the Special Issue The Progresses on Polyelectrolytes and Polyelectrolyte Complexes)
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Review

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22 pages, 1349 KiB  
Review
Theoretical and Computational Insight into Solvent and Specific Ion Effects for Polyelectrolytes: The Importance of Local Molecular Interactions
by Jens Smiatek
Molecules 2020, 25(7), 1661; https://doi.org/10.3390/molecules25071661 - 03 Apr 2020
Cited by 35 | Viewed by 3480
Abstract
Polyelectrolytes in solution show a broad plethora of interesting effects. In this short review article, we focus on recent theoretical and computational findings regarding specific ion and solvent effects and their impact on the polyelectrolyte behavior. In contrast to standard mean field descriptions, [...] Read more.
Polyelectrolytes in solution show a broad plethora of interesting effects. In this short review article, we focus on recent theoretical and computational findings regarding specific ion and solvent effects and their impact on the polyelectrolyte behavior. In contrast to standard mean field descriptions, the properties of polyelectrolytes are significantly influenced by crucial interactions with the solvent, co-solvent and ion species. The corresponding experimental and simulation results reveal a significant deviation from theoretical predictions, which also highlights the importance of charge transfer, dispersion and polarization interactions in combination with solvation mechanisms. We discuss recent theoretical and computational findings in addition to novel approaches which help broaden the applicability of simple mean field theories. Full article
(This article belongs to the Special Issue The Progresses on Polyelectrolytes and Polyelectrolyte Complexes)
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29 pages, 2709 KiB  
Review
Bioplatform Fabrication Approaches Affecting Chitosan-Based Interpolymer Complex Properties and Performance as Wound Dressings
by Hillary Mndlovu, Lisa C. du Toit, Pradeep Kumar, Yahya E. Choonara, Thashree Marimuthu, Pierre P. D. Kondiah and Viness Pillay
Molecules 2020, 25(1), 222; https://doi.org/10.3390/molecules25010222 - 06 Jan 2020
Cited by 20 | Viewed by 4533
Abstract
Chitosan can form interpolymer complexes (IPCs) with anionic polymers to form biomedical platforms (BMPs) for wound dressing/healing applications. This has resulted in its application in various BMPs such as gauze, nano/microparticles, hydrogels, scaffolds, and films. Notably, wound healing has been highlighted as a [...] Read more.
Chitosan can form interpolymer complexes (IPCs) with anionic polymers to form biomedical platforms (BMPs) for wound dressing/healing applications. This has resulted in its application in various BMPs such as gauze, nano/microparticles, hydrogels, scaffolds, and films. Notably, wound healing has been highlighted as a noteworthy application due to the remarkable physical, chemical, and mechanical properties enabled though the interaction of these polyelectrolytes. The interaction of chitosan and anionic polymers can improve the properties and performance of BMPs. To this end, the approaches employed in fabricating wound dressings was evaluated for their effect on the property–performance factors contributing to BMP suitability in wound dressing. The use of chitosan in wound dressing applications has had much attention due to its compatible biological properties. Recent advancement includes the control of the degree of crosslinking and incorporation of bioactives in an attempt to enhance the physicochemical and physicomechanical properties of wound dressing BMPs. A critical issue with polyelectrolyte-based BMPs is that their effective translation to wound dressing platforms has yet to be realised due to the unmet challenges faced when mimicking the complex and dynamic wound environment. Novel BMPs stemming from the IPCs of chitosan are discussed in this review to offer new insight into the tailoring of physical, chemical, and mechanical properties via fabrication approaches to develop effective wound dressing candidates. These BMPs may pave the way to new therapeutic developments for improved patient outcomes. Full article
(This article belongs to the Special Issue The Progresses on Polyelectrolytes and Polyelectrolyte Complexes)
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