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

Deadline for manuscript submissions: closed (30 November 2017) | Viewed by 72860

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Prof. Dr. Alan Edward Tonelli

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Fiber & Polymer Science Program College of Textiles, North Carolina State University, Campus Box 8301, 2401 Research Drive, Raleigh, NC 27695-8301, USA
Interests: characterization of polymer microstructures; conformations; properties; NMR; kerr-effects; nanostructuring polymers through host–guest complex formation
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Dr. Ganesh Narayanan

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Co-Guest Editor

Department of Chemistry and The Marvin B. Dow Advanced Composites Institute, Mississippi State University, Starkville, MS 39759, USA
Interests: cyclodextrins; biomaterials; synthetic degradable polymers; analytical characterization; micro and nanofibers; orthopaedic tissue regeneration
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Dr. Alper Gurarslan

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Co-Guest Editor

Faculty of Textile Technologies and Design, Istanbul Technical University, Inonu Cad. No 65 Gumussuyu, Beyoglu, 34437 Istanbul, Turkey
Interests: polymer structure and properties; composites; flexible and stretchable electronics; 2-dimensional materials; cylodextrin; urea; biomaterials
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Special Issue Information

Dear Colleagues,

I enthusiastically invite you to contribute to a Special Issue of the open-access journal Polymers, focusing on “Host–Guest Polymer Complexes”, which I and two of my former PhD students, Drs. Alper Gurarslan and Ganesh Narayanan, are editing. We hope to include papers describing the syntheses, characterization, and use of host–guest polymer complexes, as well as factors that are important to their formation. Submissions that describe unusual and unique applications of host–guest polymer complexes using hosts other than traditional ones: cyclodextrins, cucurbiturils, urea, thiourea, cyclotriphosphazines, etc., are particularly encouraged.

I hope that you accept our invitation to make this Special Issue one that will introduce, effectively summarize, and increase interest in this important area of polymer science.

Prof. Dr. Alan Edward Tonelli
Guest Editor
Dr. Alper Gurarslan
Dr. Ganesh Narayanan
Co-Guest Editor

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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

Host Polymers
Guest Molecules
Host-Guest Polymer Complexes
Polymer Inclusion Complexes
Non-included Polymer Complexes
Formation of Polymer Complexes
Characterization of Polymer Complexes
Application of Polymer Complexes

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Published Papers (13 papers)

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Editorial

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3 pages, 179 KiB

Open AccessEditorial

Host–Guest Polymer Complexes

by Alan E. Tonelli, Ganesh Narayanan and Alper Gurarslan

Polymers 2018, 10(8), 911; https://doi.org/10.3390/polym10080911 - 13 Aug 2018

Cited by 4 | Viewed by 3525

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17 pages, 2568 KiB

Open AccessArticle

Supramolecular Hydrogel Based on pNIPAm Microgels Connected via Host–Guest Interactions

by Iurii Antoniuk, Daria Kaczmarek, Attila Kardos, Imre Varga and Catherine Amiel

Polymers 2018, 10(6), 566; https://doi.org/10.3390/polym10060566 - 23 May 2018

Cited by 33 | Viewed by 6713

Abstract

In this work, host–guest supramolecular hydrogels were prepared from poly(N-isopropylacrylamide) (pNIPAm) microgels utilizing electrostatic and host/guest self-assembly. First, pNIPAm microgels bearing a poly(acrylic acid) (pAAc) shell were coated with positively charged β-cyclodextrin polymers. Addition of adamantane-substituted dextrans (Dex-Ada) allowed us to establish interparticle connections through β-cyclodextrin-adamantane (βCD-Ada) inclusion complex formation, and thus to prepare hierarchical hydrogels. Under the conditions of hydrogel formation, close contact between the microgels was ensured. To the best of our knowledge, this is the first example of doubly crosslinked microgels prepared by noncovalent crosslinking via host–guest interactions. The prepared macrogels were studied with rheology, and fast mechanical response to temperature variation was found. Furthermore, the hydrogels exhibit fully reversible temperature-induced gel–sol transition at the physiological temperature range (37–41 °C), due to the synergetic effect between shrinking of the microgels and dissociation of βCD-Ada crosslinks at higher temperatures. This opens up attractive prospects of their potential use in biomedical applications. Full article

(This article belongs to the Special Issue Host-Guest Polymer Complexes)

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14 pages, 3972 KiB

Open AccessArticle

Reusable Xerogel Containing Quantum Dots with High Fluorescence Retention

by Xiang-Yong Liang, Lu Wang, Zhi-Yi Chang, Li-Sheng Ding, Bang-Jing Li and Sheng Zhang

Polymers 2018, 10(3), 310; https://doi.org/10.3390/polym10030310 - 13 Mar 2018

Cited by 8 | Viewed by 7418

Abstract

Although various analytical methods have been established based on quantum dots (QDs), most were conducted in solution, which is inadequate for storage/transportation and rapid analysis. Moreover, the potential environmental problems caused by abandoned QDs cannot be ignored. In this paper, a reusable xerogel containing CdTe with strong emission is established by introducing host–guest interactions between QDs and polymer matrix. This xerogel shows high QDs loading capacity without decrease or redshift in fluorescence (the maximum of loading is 50 wt % of the final xerogel), which benefits from the steric hindrance of β-cyclodextrin (βCD) molecules. Host–guest interactions immobilize QDs firmly, resulting in the excellent fluorescence retention of the xerogel. The good detecting performance and reusability mean this xerogel could be employed as a versatile analysis platform (for quantitative and qualitative analyses). In addition, the xerogel can be self-healed by the aid of water. Full article

(This article belongs to the Special Issue Host-Guest Polymer Complexes)

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10 pages, 2052 KiB

Open AccessArticle

α-Cyclodextrins Polyrotaxane Loading Silver Sulfadiazine

by Sa Liu, Chunting Zhong, Weiwei Wang, Yongguang Jia, Lin Wang and Li Ren

Polymers 2018, 10(2), 190; https://doi.org/10.3390/polym10020190 - 14 Feb 2018

Cited by 7 | Viewed by 3907

Abstract

As a drug carrier, polyrotaxane (PR) has been used for targeted delivery and sustained release of drugs, whereas silver sulfadiazine (SD-Ag) is an emerging antibiotic agent. PR was synthesized by the use of α-cyclodextrin (CD) and poly(ethylene glycol) (PEG), and a specific antibacterial material (PR-(SD-Ag)) was then prepared by loading SD-Ag onto PR with different mass ratios. The loading capacity and the encapsulation efficiency were 90% at a mass ratio of 1:1 of PR and SD-Ag. SD-Ag was released stably and slowly within 6 d in vitro, and its cumulative release reached more than 85%. The mechanism of PR loading SD-Ag might be that SD-Ag attached to the edge of α-CD through hydrogen bonding. PR-(SD-Ag) showed a higher light stability than SD-Ag and held excellent antibacterial properties against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). Full article

(This article belongs to the Special Issue Host-Guest Polymer Complexes)

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17 pages, 4964 KiB

Open AccessArticle

Preparation and Characterization of Antibacterial Polypropylene Meshes with Covalently Incorporated β-Cyclodextrins and Captured Antimicrobial Agent for Hernia Repair

by Noor Sanbhal, Ying Mao, Gang Sun, Yan Li, Mazhar Peerzada and Lu Wang

Polymers 2018, 10(1), 58; https://doi.org/10.3390/polym10010058 - 11 Jan 2018

Cited by 22 | Viewed by 4774

Abstract

Polypropylene (PP) light weight meshes are commonly used as hernioplasty implants. Nevertheless, the growth of bacteria within textile knitted mesh intersections can occur after surgical mesh implantation, causing infections. Thus, bacterial reproduction has to be stopped in the very early stage of mesh implantation. Herein, novel antimicrobial PP meshes grafted with β-CD and complexes with triclosan were prepared for mesh infection prevention. Initially, PP mesh surfaces were functionalized with suitable cold oxygen plasma. Then, hexamethylene diisocyanate (HDI) was successfully grafted on the plasma-activated PP surfaces. Afterwards, β-CD was connected with the already HDI reacted PP meshes and triclosan, serving as a model antimicrobial agent, was loaded into the cyclodextrin (CD) cavity for desired antibacterial functions. The hydrophobic interior and hydrophilic exterior of β-CD are well suited to form complexes with hydrophobic host guest molecules. Thus, the prepared PP mesh samples, CD-TCL-2 and CD-TCL-6 demonstrated excellent antibacterial properties against Staphylococcus aureus and Escherichia coli that were sustained up to 11 and 13 days, respectively. The surfaces of chemically modified PP meshes showed dramatically reduced water contact angles. Moreover, X-ray diffractometer (XRD), differential scanning calorimeter (DSC), and Thermogravimetric (TGA) evidenced that there was no significant effect of grafted hexamethylene diisocyanate (HDI) and CD on the structural and thermal properties of the PP meshes. Full article

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16 pages, 2842 KiB

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Effect of Dendrigraft Generation on the Interaction between Anionic Polyelectrolytes and Dendrigraft Poly(l-Lysine)

by Feriel Meriem Lounis, Joseph Chamieh, Laurent Leclercq, Philippe Gonzalez, Jean-Christophe Rossi and Hervé Cottet

Polymers 2018, 10(1), 45; https://doi.org/10.3390/polym10010045 - 4 Jan 2018

Cited by 10 | Viewed by 3592

Abstract

In this present work, three generations of dendrigraft poly(l-Lysine) (DGL) were studied regarding their ability to interact with linear poly (acrylamide-co-2-acrylamido-2-methyl-1-propanesulfonate) (PAMAMPS) of different chemical charge densities (30% and 100%). Frontal analysis continuous capillary electrophoresis (FACCE) was successfully applied to determine binding constants and binding stoichiometries. The effect of DGL generation on the interaction was evaluated for the first three generations (G2, G3, and G4) at different ionic strengths, and the effect of ligand topology (linear PLL vs. dendrigraft DGL) on binding parameters was evaluated. An increase of the biding site constants accompanied with a decrease of the DGL-PAMAMPS (n:1) stoichiometry was observed for increasing DGL generation. The logarithm of the global binding constants decreased linearly with the logarithm of the ionic strength. This double logarithmic representation allowed determining the extent of counter-ions released from the association of DGL molecules onto one PAMAMPS chain that was compared to the total entropic reservoir constituted by the total number of condensed counter-ions before the association. Full article

(This article belongs to the Special Issue Host-Guest Polymer Complexes)

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2763 KiB

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Antibacterial Films Made of Ionic Complexes of Poly(γ-glutamic acid) and Ethyl Lauroyl Arginate

by Ana Gamarra-Montes, Beatriz Missagia, Jordi Morató and Sebastián Muñoz-Guerra

Polymers 2018, 10(1), 21; https://doi.org/10.3390/polym10010021 - 24 Dec 2017

Cited by 14 | Viewed by 6003

Abstract

The biocide agent LAE (ethyl ^αN-lauroyl l-arginate chloride) was coupled with poly(γ-glutamic acid) (PGGA) to form stable ionic complexes with LAE:PGGA ratios of 1 and 0.5. The nanostructure adopted by these complexes and its response to thermal changes were examined in detail by Differential scanning calorimetry (DSC) and X-ray diffraction (XRD) using synchrotron radiation in real time. A layered biphasic structure with LAE filling the space between the polypeptidic sheets was adopted in these complexes. The complexes were stable up to above 250 °C, non-water soluble, and were able to form consistent transparent films. The release of LAE from the complexes upon incubation in aqueous buffer was examined and found to depend on both pH and complex composition. The antibacterial activity of films made of these complexes against Gram-positive (L. monocytogenes and S. aureus) and Gram-negative (E. coli and S. enterica) bacteria was preliminary evaluated and was found to be very high against the formers and only moderate against the later. The bactericide activity displayed by the LAE·PGGA complexes was directly related with the amount of LAE that was released from the film to the environment. Full article

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3261 KiB

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pH-Responsive Host–Guest Complexation in Pillar[6]arene-Containing Polyelectrolyte Multilayer Films

by Henning Nicolas, Bin Yuan, Jiangfei Xu, Xi Zhang and Monika Schönhoff

Polymers 2017, 9(12), 719; https://doi.org/10.3390/polym9120719 - 16 Dec 2017

Cited by 11 | Viewed by 6719

Abstract

A water-soluble, anionic pillar[6]arene derivative (WP6) is applied as monomeric building block for the layer-by-layer self-assembly of thin polyelectrolyte multilayer films, and its pH-dependent host–guest properties are employed for the reversible binding and release of a methylviologen guest molecule. The alternating assembly of anionic WP6 and cationic diazo resin (DAR) is monitored in-situ by a dissipative quartz crystal microbalance (QCM-D). In solution, the formation of a stoichiometric inclusion complex of WP6 and cationic methylviologen (MV) as guest molecule is investigated by isothermal titration calorimetry and UV-vis spectroscopy, respectively, and attributed to electrostatic interactions as primary driving force of the host–guest complexation. Exposure of WP6-containing multilayers to MV solution reveals a significant decrease of the resonance frequency, confirming MV binding. Subsequent release is achieved by pH lowering, decreasing the host–guest interactions. The dissociation of the host–guest complex, release of the guest from the film, as well as full reversibility of the binding event are identified by QCM-D. In addition, UV-vis data quantify the surface coverage of the guest molecule in the film after loading and release, respectively. These findings establish the pH-responsiveness of WP6 as a novel external stimulus for the reversible guest molecule recognition in thin films. Full article

(This article belongs to the Special Issue Host-Guest Polymer Complexes)

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1457 KiB

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Enhancing Stereocomplexation Ability of Polylactide by Coalescing from Its Inclusion Complex with Urea

by Ping Liu, Xiao-Tong Chen and Hai-Mu Ye

Polymers 2017, 9(11), 592; https://doi.org/10.3390/polym9110592 - 9 Nov 2017

Cited by 7 | Viewed by 3930

Abstract

In this study, polylactide/urea complexes were successfully prepared by the electrospinning method, then the host urea component was removed to obtain a coalesced poly(L-lactide) (PLLA)/poly(D-lactide) (PDLA) blend. The crystallization behavior of the coalesced PLLA/PDLA blend (c-PLLA/PDLA) was studied by a differential scanning calorimeter (DSC) and Fourier transform infrared (FTIR) spectroscopy. The c-PLLA/PDLA was found to show better crystallization ability than normal PLLA/PDLA blend (r-PLLA/PDLA). More interestingly, the c-PLLA/PDLA effectively and solely crystallized into stereocomplex crystals during the non-isothermal melt-crystallization process, and the reason was attributed to the equally-distributing state of PLLA and PDLA chains in the PLLA/PDLA/urea complex, which led to good interconnection between PLLA and PDLA chains when the urea frameworks were instantly removed. Full article

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3607 KiB

Open AccessArticle

Directional Alignment of Polyfluorene Copolymers at Patterned Solid-Liquid Interfaces

by Xiaolu Pan, Hongwei Li and Xinping Zhang

Polymers 2017, 9(8), 356; https://doi.org/10.3390/polym9080356 - 11 Aug 2017

Cited by 1 | Viewed by 5326

Abstract

Polyfluorene and its derivatives have been recognized as efficient light-emitting semiconductors. However, directional alignment of polyfluorene copolymers at a large scale has rarely been observed, in particular for the two relatively more amorphous members of poly-9,9-dioctylfluorene-co-bethiadisazole (F8BT) and poly-(9,9-dioctylfluorenyl-2,7-diyl)-co-(N,N0-diphenyl)-N,N′di(p-butyl-oxy-pheyl)-1,4-diamino-benzene) (PFB) molecules. Furthermore, the directional alignment of PFB has not been observed so far due to the triphenylamine units in its molecular structures. We present, in this work, a solution-processible method to achieve large-scale alignment of F8BT and PFB molecules into fibers as long as millimeters in a defined direction. Spin-coating the polymer film on to a glass substrate patterned by one-dimensional dielectric nano-grating structures through interference lithography and subsequent modification using 1,5-pentanediol have been used in all of the preparation procedures. Polymer fibers have been obtained in an arrangement parallel to the grating lines. The microscopic, spectroscopic, and photoconductive performances verified the formation and the quality of these directionally-aligned polymeric fibers. Full article

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5377 KiB

Open AccessArticle

Enhancement of Wound Healing in Normal and Diabetic Mice by Topical Application of Amorphous Polyphosphate. Superior Effect of a Host–Guest Composite Material Composed of Collagen (Host) and Polyphosphate (Guest)

by Werner E.G. Müller, Dinko Relkovic, Maximilian Ackermann, Shunfeng Wang, Meik Neufurth, Andrea Paravic Radicevic, Hiroshi Ushijima, Heinz-C Schröder and Xiaohong Wang

Polymers 2017, 9(7), 300; https://doi.org/10.3390/polym9070300 - 22 Jul 2017

Cited by 33 | Viewed by 6976

Abstract

The effect of polyphosphate (polyP) microparticles on wound healing was tested both in vitro and in a mice model in vivo. Two approaches were used: pure salts of polyphosphate, fabricated as amorphous microparticles (MPs, consisting of calcium and magnesium salts of polyP, “Ca–polyp-MPs” and “Mg–polyp-MPs”), and host–guest composite particles, prepared from amorphous collagen (host) and polyphosphate (guest), termed “col/polyp-MPs”. Animal experiments with polyP on healing of excisional wounds were performed using both normal mice and diabetic mice. After a healing period of 7 days “Ca–polyp-MP” significantly improved re-epithelialization in normal mice from 31% (control) to 72% (polyP microparticle-treated). Importantly, in diabetic mice, particularly the host–guest particles “col/polyp-MP”, increased the rate of re-epithelialization to ≈40% (control, 23%). In addition, those particles increased the expression of COL-I and COL-III as well as the expression the α-smooth muscle actin and the plasminogen activator inhibitor-1. We propose that “Ca–polyp-MPs”, and particularly the host–guest “col/polyp-MPs” are useful for topical treatment of wounds. Full article

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Review

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3698 KiB

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Preparation and Material Application of Amylose-Polymer Inclusion Complexes by Enzymatic Polymerization Approach

by Saya Orio, Kazuya Yamamoto and Jun-ichi Kadokawa

Polymers 2017, 9(12), 729; https://doi.org/10.3390/polym9120729 - 18 Dec 2017

Cited by 19 | Viewed by 6869

Abstract

This review presents our researches on the preparation and material application of inclusion complexes that comprises an amylose host and polymeric guests through phosphorylase-catalyzed enzymatic polymerization. Amylose is a well-known polysaccharide and forms inclusion complexes with various hydrophobic small molecules. Pure amylose is produced by enzymatic polymerization by using α-d-glucose 1-phosphate as a monomer and maltooligosaccharide as a primer catalyzed by phosphorylase. We determined that a propagating chain of amylose during enzymatic polymerization wraps around hydrophobic polymers present in the reaction system to form inclusion complexes. We termed this polymerization “vine-twining polymerization” because it is similar to the way vines of a plant grow around a rod. Hierarchical structured amylosic materials, such as hydrogels and films, were fabricated by inclusion complexation through vine-twining polymerization by using copolymers covalently grafted with hydrophobic guest polymers. The enzymatically produced amyloses induced complexation with the guest polymers in the intermolecular graft copolymers, which acted as cross-linking points to form supramolecular hydrogels. By including a film-formable main-chain in the graft copolymer, a supramolecular film was obtained through hydrogelation. Supramolecular polymeric materials were successfully fabricated through vine-twining polymerization by using primer-guest conjugates. The products of vine-twining polymerization form polymeric continuums of inclusion complexes, where the enzymatically produced amylose chains elongate from the conjugates included in the guest segments of the other conjugates. Full article

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6151 KiB

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Reorganizing Polymer Chains with Cyclodextrins

by Alper Gurarslan, Abhay Joijode, Jialong Shen, Ganesh Narayanan, Gerry J. Antony, Shanshan Li, Yavuz Caydamli and Alan E. Tonelli

Polymers 2017, 9(12), 673; https://doi.org/10.3390/polym9120673 - 4 Dec 2017

Cited by 11 | Viewed by 5490

Abstract

During the past several years, we have been utilizing cyclodextrins (CDs) to nanostructure polymers into bulk samples whose chain organizations, properties, and behaviors are quite distinct from neat bulk samples obtained from their solutions and melts. We first form non-covalently bonded inclusion complexes (ICs) between CD hosts and guest polymers, where the guest chains are highly extended and separately occupy the narrow channels (~0.5–1.0 nm in diameter) formed by the columnar arrangement of CDs in the IC crystals. Careful removal of the host crystalline CD lattice from the polymer-CD-IC crystals leads to coalescence of the guest polymer chains into bulk samples, which we have repeatedly observed to behave distinctly from those produced from their solutions or melts. While amorphous polymers coalesced from their CD-ICs evidence significantly higher glass-transition temperatures, T_gs, polymers that crystallize generally show higher melting and crystallization temperatures (T_ms, T_cs), and some-times different crystalline polymorphs, when they are coalesced from their CD-ICs. Formation of CD-ICs containing two or more guest homopolymers or with block copolymers can result in coalesced samples which exhibit intimate mixing between their common homopolymer chains or between the blocks of the copolymer. On a more practically relevant level, the distinct organizations and behaviors observed for polymer samples coalesced from their CD-ICs are found to be stable to extended annealing at temperatures above their T_gs and T_ms. We believe this is a consequence of the structural organization of the crystalline polymer-CD-ICs, where the guest polymer chains included in host-IC crystals are separated and confined to occupy the narrow channels formed by the host CDs during IC crystallization. Substantial degrees of the extended and un-entangled natures of the IC-included chains are apparently retained upon coalescence, and are resistant to high temperature annealing. Following the careful removal of the host CD lattice from each randomly oriented IC crystal, the guest polymer chains now occupying a much-reduced volume may be somewhat “nematically” oriented, resulting in a collection of randomly oriented “nematic” regions of largely extended and un-entangled coalesced guest chains. The suggested randomly oriented nematic domain organization of guest polymers might explain why even at high temperatures their transformation to randomly-coiling, interpenetrated, and entangled melts might be difficult. In addition, the behaviors and uses of polymers coalesced from their CD-ICs are briefly described and summarized here, and we attempted to draw conclusions from and relationships between their behaviors and the unique chain organizations and conformations achieved upon coalescence. Full article

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