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

Deadline for manuscript submissions: closed (28 February 2018) | Viewed by 69667

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Prof. Dr. Enrique Lopez-Cabarcos

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Department of Chemistry in Pharmaceutical Sciences, Faculty of Pharmacy, Complutense University of Madrid, 28040 Madrid, Spain
Interests: microgels and polymer nanogels; calcium cement for bone regeneration; enzymatic biosensors

Prof. Dr. Marco Lattuada

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Department of Chemistry, Université de Fribourg, Fribourg, Switzerland
Interests: engineering of anisotropic nanoparticles; control of nanoparticles self-assembly; magnetic nanoparticles synthesis and functionalization; colloidal stability; development of mathematical models in soft-matter physics; hydrodynamic interactions in colloidal suspensions; Monte-Carlo; Brownian Dynamic and Stokesian Dynamics simulations applied to colloids; scattering techniques for particles characterization

Prof. Dr. Wuge Briscoe

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School of Chemistry, University of Bristol, Bristol BS8 1TH, UK
Interests: surface forces; friction; lubrication; lipids; liposomes; surfactants; self-assembly; coffee ring effects; nanostructured surfaces; polymer brushes; X-ray reflectivity; neutron scattering; biolubrication; bacterial membranes; nanotoxicity; deep eutectic solvents
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Special Issue Information

Dear Colleagues,

The annual European Colloid and Interface Society conference is a major event for the colloid science community, and this is the 31st conference in a series of successful meetings, of which the primary goal is to bring together all major disciplines of colloids and interfaces, enabling participants to exchange knowledge, communicate to each other the results of their recent research, and to network with colleagues for new collaborations.

ECIS 2017 (http://www.ecis2017madrid.com/) will cover fundamental and applied advances in the fields of interfaces, dispersed systems, wetting, complex fluids, micro-and nano-engineered materials, upconversion nanoparticles, ion specific effects, self-assembly of surfactants, polymers and proteins, and advances in theories and instrumentation.

The topics include, but are not limited to:

Polymer colloids
Microgels and gels
Polymers in solution
Polymer nanoparticles
Polymer gels
Self-assembly of polymers
Functionalization of surfaces with polymers

Submission window open date: 15 July 2017

Submission deadline: 28 February 2018

Prof. Dr. Enrique Lopez-Cabarcos
Prof. Dr. Marco Lattuada
Dr. Wuge Briscoe
Guest Editors

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

Polymer colloids
microgels and gels
polymers in solution
polymer nanoparticles
polymer gels
self-assembly of polymers
functionalization of surfaces with polymers

Published Papers (13 papers)

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12 pages, 2799 KiB

Open AccessArticle

Synthesis of Polypyrrole Induced by [Fe(CN)₆]³⁻ and Redox Cycling of [Fe(CN)₆]⁴⁻/[Fe(CN)₆]³⁻

by Eivydas Andriukonis, Almira Ramanaviciene and Arunas Ramanavicius

Polymers 2018, 10(7), 749; https://doi.org/10.3390/polym10070749 - 06 Jul 2018

Cited by 26 | Viewed by 4040

Abstract

Chemical synthesis of the conducting polymer polypyrrole induced by [Fe(CN)₆]³⁻ is reported. Reaction kinetics were characterized spectrophotometrically. Reaction rate was evaluated at several different pH levels in the presence of [Fe(CN)₆]³⁻ and [Fe(CN)₆]⁴⁻ ions. The formation of polypyrrole at aerobic and anaerobic conditions was evaluated. We report that at anaerobic conditions [Fe(CN)₆]⁴⁻ cannot initiate oxidative polymerization, while its oxidized form [Fe(CN)₆]³⁻ successfully initiates and maintains the pyrrole polymerization reaction. The formation of polypyrrole was also observed in the solution containing a pyrrole monomer, [Fe(CN)₆]⁴⁻ and dissolved oxygen due to re-oxidation (redox cycling) of [Fe(CN)₆]⁴⁻ into [Fe(CN)₆]³⁻ by dissolved oxygen. Experiments to determine the polymerization reaction rate were performed and showed the highest rate in the presence of 0.5 mM of [Fe(CN)₆]³⁻ at pH 9.0, while the polymerization reaction performed at pH 7.0 was determined as the slowest. This investigation opens new horizons for the application of [Fe(CN)₆]⁴⁻/[Fe(CN)₆]³⁻-based redox cycling reactions in the synthesis of the conducting polymer polypyrrole and potentially in the formation of other conducting polymers which can be formed by oxidative polymerization. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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20 pages, 1946 KiB

Open AccessArticle

Modulation of the Catalytic Properties of Lipase B from Candida antarctica by Immobilization on Tailor-Made Magnetic Iron Oxide Nanoparticles: The Key Role of Nanocarrier Surface Engineering

by Mario Viñambres, Marco Filice and Marzia Marciello

Polymers 2018, 10(6), 615; https://doi.org/10.3390/polym10060615 - 05 Jun 2018

Cited by 18 | Viewed by 4518

Abstract

The immobilization of biocatalysts on magnetic nanomaterial surface is a very attractive alternative to achieve enzyme nanoderivatives with highly improved properties. The combination between the careful tailoring of nanocarrier surfaces and the site-specific chemical modification of biomacromolecules is a crucial parameter to finely modulate the catalytic behavior of the biocatalyst. In this work, a useful strategy to immobilize chemically aminated lipase B from Candida antarctica on magnetic iron oxide nanoparticles (IONPs) by covalent multipoint attachment or hydrophobic physical adsorption upon previous tailored engineering of nanocarriers with poly-carboxylic groups (citric acid or succinic anhydride, CALB_EDA@CA-NPs and CALB_EDA@SA-NPs respectively) or hydrophobic layer (oleic acid, CALB_EDA@OA-NPs) is described. After full characterization, the nanocatalysts have been assessed in the enantioselective kinetic resolution of racemic methyl mandelate. Depending on the immobilization strategy, each enzymatic nanoderivative permitted to selectively improve a specific property of the biocatalyst. In general, all the immobilization protocols permitted loading from good to high lipase amount (149 < immobilized lipase < 234 mg/g_Fe). The hydrophobic CALB_EDA@OA-NPs was the most active nanocatalyst, whereas the covalent CALB_EDA@CA-NPs and CALB_EDA@SA-NPs were revealed to be the most thermostable and also the most enantioselective ones in the kinetic resolution reaction (almost 90% ee R-enantiomer). A strategy to maintain all these properties in long-time storage (up to 1 month) by freeze-drying was also optimized. Therefore, the nanocarrier surface engineering is demonstrated to be a key-parameter in the design and preparation of lipase libraries with enhanced catalytic properties. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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12 pages, 20153 KiB

Open AccessArticle

Self-Organization and Swelling of Ruthenium-Metal Coordination Polymers with PTA (Metal = Ag, Au, Co)

by Benjamin Sierra-Martin, Manuel Serrano-Ruiz, Victoria García-Sakai, Franco Scalambra, Antonio Romerosa and Antonio Fernandez-Barbero

Polymers 2018, 10(5), 528; https://doi.org/10.3390/polym10050528 - 15 May 2018

Cited by 9 | Viewed by 3416

Abstract

We present the internal structure and dynamics of novel coordination polymers based on two metal-containing moieties Ru-X (X: Ag, Au, Co), bridged through the phosphine PTA (3,5,7-triaza-phosphaadamantane). X-ray scattering gives the heterometallic polymer organization. Quasi-elastic neutron scattering measurements over a broad temperature range show a transition from vibrational Debye-Waller behavior to a more dynamically active state, but with rather localized motions, coinciding with the loss of structural water at around room temperature. Light scattering reveals that the polymers self-associate to form stable micro-particles in aqueous solution with a thermally driven volume transition. This is described by the Flory theory for polymers in solution, in which the polymer solvency is calculated as a function of the temperature. Polymer self-organization is further studied by small-angle neutron scattering and electron microscopy. A polymer parallel-plane model with gaps controlled by the environmental temperature is proposed. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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14 pages, 901 KiB

Open AccessArticle

An Accurate Estimate of the Free Energy and Phase Diagram of All-DNA Bulk Fluids

by Emanuele Locatelli and Lorenzo Rovigatti

Polymers 2018, 10(4), 447; https://doi.org/10.3390/polym10040447 - 16 Apr 2018

Cited by 4 | Viewed by 4233

Abstract

We present a numerical study in which large-scale bulk simulations of self-assembled DNA constructs have been carried out with a realistic coarse-grained model. The investigation aims at obtaining a precise, albeit numerically demanding, estimate of the free energy for such systems. We then, in turn, use these accurate results to validate a recently proposed theoretical approach that builds on a liquid-state theory, the Wertheim theory, to compute the phase diagram of all-DNA fluids. This hybrid theoretical/numerical approach, based on the lowest-order virial expansion and on a nearest-neighbor DNA model, can provide, in an undemanding way, a parameter-free thermodynamic description of DNA associating fluids that is in semi-quantitative agreement with experiments. We show that the predictions of the scheme are as accurate as those obtained with more sophisticated methods. We also demonstrate the flexibility of the approach by incorporating non-trivial additional contributions that go beyond the nearest-neighbor model to compute the DNA hybridization free energy. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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13 pages, 2597 KiB

Open AccessArticle

Novel Nano-Liposome Formulation for Dry Eyes with Components Similar to the Preocular Tear Film

by Marta Vicario-de-la-Torre, María Caballo-González, Eva Vico, Laura Morales-Fernández, Pedro Arriola-Villalobos, Beatriz De las Heras, José Manuel Benítez-del-Castillo, Manuel Guzmán, Thomas Millar, Rocío Herrero-Vanrell and Irene T. Molina-Martínez

Polymers 2018, 10(4), 425; https://doi.org/10.3390/polym10040425 - 11 Apr 2018

Cited by 28 | Viewed by 5641

Abstract

Dry eye is commonly treated with artificial tears; however, developing artificial tears similar to natural tears is difficult due to the complex nature of tears. We characterized and evaluated a novel artificial tear formulation with components similar to the lipid and aqueous constituents of natural tears. Nano-liposomes, composed in part of phosphatidylcholine, were dispersed in an aqueous solution of bioadhesive sodium hyaluronate. Liposome size, zeta potential, and physicochemical properties of the fresh and stored (4 °C) liposomal formulation were analyzed. In vitro tolerance was tested using human corneal and conjunctival cell lines by exposures of 15 min to 4 h. The tolerance of the liposomal formulation was evaluated in animals (rabbits). The average liposome size was 186.3 ± 7.0 nm, and the zeta potential was negative. The osmolarity of the formulation was 198.6 ± 1.7 mOsm, with a surface tension of 36.5 ± 0.4 mN/m and viscosity of 3.05 ± 0.02 mPa·s. Viability values in the human corneal and conjunctival cell lines were always >80%, even after liposomal formulation storage for 8 weeks. Discomfort and clinical signs after instillation in rabbit eyes were absent. The new formulation, based on phosphatidylcholine-liposomes dispersed in sodium hyaluronate has suitable components and characteristics, including high in vitro cell viability and good in vivo tolerance, to serve as a tear substitute. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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16 pages, 18984 KiB

Open AccessArticle

Active Ester Containing Surfmer for One-Stage Polymer Nanoparticle Surface Functionalization in Mini-Emulsion Polymerization

by Vanessa L. Albernaz, Monika Bach, Achim Weber, Alexander Southan and Günter E. M. Tovar

Polymers 2018, 10(4), 408; https://doi.org/10.3390/polym10040408 - 06 Apr 2018

Cited by 7 | Viewed by 8712

Abstract

Functional surface active monomers (surfmers) are molecules that combine the functionalities of surface activity, polymerizability, and reactive groups. This study presents an improved pathway for the synthesis of the active ester containing surfmer p-(11-acrylamido)undecanoyloxyphenyl dimethylsulfonium methyl sulfate (AUPDS). Further, the preparation of poly(methyl methacrylate) and polystyrene nanoparticles (NPs) by mini-emulsion polymerization using AUPDS is investigated, leading to NPs with active ester groups on their surface. By systematically varying reaction parameters and reagent concentrations, it was found that AUPDS feed concentrations between 2–4 mol% yielded narrowly distributed and stable spherical particles with average sizes between 83 and 134 nm for non-cross-linked NPs, and up to 163 nm for cross-linked NPs. By basic hydrolysis of the active ester groups in aqueous dispersion, the positive ζ-potential (ZP) was converted into a negative ZP and charge quantities determined by polyelectrolyte titrations before and after hydrolysis were in the same range, indicating that the active ester groups were indeed accessible in aqueous suspension. Increasing cross-linker amounts over 10 mol% also led to a decrease of ZP of NPs, probably due to internalization of the AUPDS during polymerization. In conclusion, by using optimized reaction conditions, it is possible to prepare active ester functionalized NPs in one stage using AUPDS as a surfmer in mini-emulsion polymerization. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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17 pages, 13691 KiB

Open AccessArticle

Polymerization-Driven Immobilization of dc-APGD Synthesized Gold Nanoparticles into a Quaternary Ammonium-Based Hydrogel Resulting in a Polymeric Nanocomposite with Heat-Transfer Applications

by Piotr Cyganowski, Anna Dzimitrowicz, Piotr Jamroz, Dorota Jermakowicz-Bartkowiak and Pawel Pohl

Polymers 2018, 10(4), 377; https://doi.org/10.3390/polym10040377 - 29 Mar 2018

Cited by 10 | Viewed by 4015

Abstract

A new method for the production of nanocomposites, composed of gold nanoparticles (AuNPs) and (vinylbenzyl)trimethylammonium chloride-co-N,N-methylene bisacrylamide (VBTAC-co-MBA) hydrogel, is described. Raw-AuNPs of defined optical and granulometric properties were synthesized using direct current atmospheric pressure glow discharge (dc-APGD) generated in contact with a solution of HAuCl₄. Different approaches to the polymerization-driven synthesis of Au/VBTAC-co-MBA nanocomposites were tested. It was established that homogenous dispersion of AuNPs in this new nanomaterial with was achieved in the presence of NaOH in the reaction mixture. The new nanocomposite was found to have excellent heat-transfer properties. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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17 pages, 28628 KiB

Open AccessArticle

Transport Asymmetry of Novel Bi-Layer Hybrid Perfluorinated Membranes on the Base of MF-4SC Modified by Halloysite Nanotubes with Platinum

by Anatoly Filippov, Daria Petrova, Irina Falina, Natalia Kononenko, Evgenii Ivanov, Yuri Lvov and Vladimir Vinokurov

Polymers 2018, 10(4), 366; https://doi.org/10.3390/polym10040366 - 25 Mar 2018

Cited by 19 | Viewed by 3928

Abstract

Three types of bi-layer hybrid nanocomposites on the base of perfluorinated cation-exchange membrane MF-4SC (Russian analogue of Nafion^®-117) were synthesized and characterized. It was found that two membranes possess the noticeable asymmetry of the current–voltage curve (CVC) under changing their orientation towards the applied electric field, despite the absence of asymmetry of diffusion permeability. These phenomena were explained in the frame of the “fine-porous model” expanded for bi-layer membranes. A special procedure to calculate the real values of the diffusion layers thickness and the limiting current density was proposed. Due to asymmetry effects of the current voltage curves of bi-layer hybrid membranes on the base of MF-4SC, halloysite nanotubes and platinum nanoparticles, it is prospective to assemble membrane switches (membrane relays or diodes) with predictable transport properties, founded upon the theory developed here. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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16 pages, 3027 KiB

Open AccessArticle

Humidity-Induced Phase Transitions of Surfactants Embedded in Latex Coatings Can Drastically Alter Their Water Barrier and Mechanical Properties

by Juan F. Gonzalez-Martinez, Yana Znamenskaya Falk, Sebastian Björklund, Stefan Erkselius, Nicola Rehnberg and Javier Sotres

Polymers 2018, 10(3), 284; https://doi.org/10.3390/polym10030284 - 08 Mar 2018

Cited by 9 | Viewed by 4220

Abstract

Latex coatings are environmentally friendly i.e., they are formed from aqueous polymer dispersions, are cheap to produce and provide exceptional mechanical properties. Therefore, they are ubiquitous and can be found in a wide range of different applications such as paints and varnishes, pressure-sensitive adhesives, textiles, construction materials, paper coatings and inks. However, they also have weaknesses and their surfactant content is among them. Surfactants are often needed to stabilize polymer particles in the aqueous latex dispersions. These surfactants also form part of the coatings formed from these dispersions, and it is well-known that they can lower their performance. This work further explores this aspect and focuses on the role that embedded surfactant domains play in the response of latex coatings to humid environments. For this purpose, we made use of several experimental techniques where humidity control was implemented: quartz crystal microbalance with dissipation, atomic force microscopy and differential scanning calorimetry. By means of this multimethodological approach, we report that surfactants embedded in latex coatings can undergo humidity-induced transitions towards more hydrated and softer phases, and that this results in a drastic decrease of the mechanical and water barrier properties of the whole coatings. Subsequently, this work highlights the potential of taking into account the phase behavior of surfactants when choosing which ones to use in the synthesis of latex dispersions as this would help in predicting their performance under different environmental conditions. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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15 pages, 4696 KiB

Open AccessArticle

Hyperthermia-Triggered Gemcitabine Release from Polymer-Coated Magnetite Nanoparticles

by G. R. Iglesias, Felisa Reyes-Ortega, B. L. Checa Fernandez and Ángel V. Delgado

Polymers 2018, 10(3), 269; https://doi.org/10.3390/polym10030269 - 06 Mar 2018

Cited by 30 | Viewed by 6078

Abstract

In this work a combined, multifunctional platform, which was devised for the simultaneous application of magnetic hyperthermia and the delivery of the antitumor drug gemcitabine, is described and tested in vitro. The system consists of magnetite particles embedded in a polymer envelope, designed to make them biocompatible, thanks to the presence of poly (ethylene glycol) in the polymer shell. The commercial particles, after thorough cleaning, are provided with carboxyl terminal groups, so that at physiological pH they present negative surface charge. This was proved by electrophoresis, and makes it possible to electrostatically adsorb gemcitabine hydrochloride, which is the active drug of the resulting nanostructure. Both electrophoresis and infrared spectroscopy are used to confirm the adsorption of the drug. The gemcitabine-loaded particles are tested regarding their ability to release it while heating the surroundings by magnetic hyperthermia, in principle their chances as antitumor agents. The release, with first-order kinetics, is found to be faster when carried out in a thermostated bath at 43 °C than at 37 °C, as expected. But, the main result of this investigation is that while the particles retain their hyperthermia response, with reasonably high heating power, they release the drug faster and with zeroth-order kinetics when they are maintained at 43 °C under the action of the alternating magnetic field used for hyperthermia. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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11 pages, 2957 KiB

Open AccessArticle

Facile and Rapid Formation of Giant Vesicles from Glass Beads

by Radu Tanasescu, Ute Mettal, Adai Colom, Aurélien Roux and Andreas Zumbuehl

Polymers 2018, 10(1), 54; https://doi.org/10.3390/polym10010054 - 09 Jan 2018

Cited by 11 | Viewed by 6407

Abstract

Giant vesicles (GVs) are widely-used model systems for biological membranes. The formulation of these vesicles, however, can be problematic and artifacts, such as degraded molecules or left-over oil, may be present in the final liposomes. The rapid formulation of a high number of artifact-free vesicles of uniform size using standard laboratory equipment is, therefore, highly desirable. Here, the gentle hydration method of glass bead-supported thin lipid films has been enhanced by adding a vortexing step. This led to the formulation of a uniform population of giant vesicles. Batches of glass beads coated with different lipids can be combined to produce vesicles of hybrid lipid compositions. This method represents a stable approach to rapidly generate giant vesicles. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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14 pages, 2445 KiB

Open AccessArticle

A Comparative Study of Poly(Azure A) Film-Modified Disposable Electrodes for Electrocatalytic Oxidation of H₂O₂: Effect of Doping Anion

by Jerónimo Agrisuelas, María-Isabel González-Sánchez, Beatriz Gómez-Monedero and Edelmira Valero

Polymers 2018, 10(1), 48; https://doi.org/10.3390/polym10010048 - 06 Jan 2018

Cited by 14 | Viewed by 5117

Abstract

In the present paper, poly(azure A) (PAA) films were electrosynthetized in the presence of different doping anions on disposable screen-printed carbon electrodes (SPCEs). The anions used included inorganic monoatomic (chloride and fluoride), inorganic polyatomic (nitrate and sulfate) and organic polyatomic (dodecyl sulfate, DS) species. The coated electrodes thus obtained were characterized by electrochemical techniques and SEM. They showed improved electrocatalytic activities towards hydrogen peroxide oxidation compared to that of a bare SPCE. In particular, the insertion of DS anions inside PAA films provided a special sensitivity to the electrocatalysis of H₂O₂, which endowed these electrodes with promising analytical features for H₂O₂ quantification. We obtained a wide linear response for H₂O₂ within a range of 5 µM to 3 mM and a limit of detection of 1.43 ± 0.10 µM (signal-to-noise ratio of 3). Furthermore, sensitivity was 72.4 ± 0.49 nA·µM⁻¹∙cm⁻² at a relatively low electrocatalytic oxidation overpotential of 0.5 V vs. Ag. The applicability of this boosted system was tested by the analysis of H₂O₂ in commercial samples of a hair lightener and an antiseptic and was corroborated by spectrophotometric methods. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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3567 KiB

Open AccessArticle

Magnetic Nanoparticles Coated with a Thermosensitive Polymer with Hyperthermia Properties

by Felisa Reyes-Ortega, Ángel V. Delgado, Elena K. Schneider, B. L. Checa Fernández and G. R. Iglesias

Polymers 2018, 10(1), 10; https://doi.org/10.3390/polym10010010 - 22 Dec 2017

Cited by 56 | Viewed by 8403

Abstract

Magnetic nanoparticles (MNPs) have been widely used to increase the efficacy of chemotherapeutics, largely through passive accumulation provided by the enhanced permeability and retention effect. Their incorporation into biopolymer coatings enables the preparation of magnetic field-responsive, biocompatible nanoparticles that are well dispersed in aqueous media. Here we describe a synthetic route to prepare functionalized, stable magnetite nanoparticles (MNPs) coated with a temperature-responsive polymer, by means of the hydrothermal method combined with an oil/water (o/w) emulsion process. The effects of both pH and temperature on the electrophoretic mobility and surface charge of these MNPs are investigated. The magnetite/polymer composition of these systems is detected by Fourier Transform Infrared Spectroscopy (FTIR) and quantified by thermogravimetric analysis. The therapeutic possibilities of the designed nanostructures as effective heating agents for magnetic hyperthermia are demonstrated, and specific absorption rates as high as 150 W/g, with 20 mT magnetic field and 205 kHz frequency, are obtained. This magnetic heating response could provide a promising nanoparticle system for combined diagnostics and cancer therapy. Full article

(This article belongs to the Special Issue Selected Papers from "ECIS 2017")

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