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Thermal Properties and Applications of Polymers II

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

Deadline for manuscript submissions: closed (29 February 2020) | Viewed by 90206

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Prof. Dr. Xiao Hu

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Department of Physics and Astronomy, College of Science and Mathematics, Rowan University, Glassboro, NJ 08028, USA
Interests: polymer; biomaterials; biomacromolecules; regenerative medicine; drug delivery; nanotechnology
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Dear Colleagues,

Further to the success of the Special Issue of Polymers “Thermal properties and applications of polymers”, we are delighted to reopen the Special Issue, now entitled “Thermal properties and applications of polymers II”.

Over the past decades, thermal analysis has become a key analytical and characterization tool in the field of materials sciences and analytical chemistry. Specific physical and chemical properties of synthetic polymers, nanomaterials, composite materials and biomaterials with different phases and morphology can be determined through thermal analysis. Traditional thermal analysis techniques include differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), thermomechanical analysis (TMA), dynamic mechanic analysis (DMA), dielectric thermal analysis (DTEA), isothermal titration calorimetry (ITC) and heat transfer analysis (such as thermal diffusivity and thermal conductivity analysis). Some techniques such as DSC have been further developed into modulated-temperature DSC (MTDSC), pressure perturbation calorimetry (PPC), micro/nano DSC, as well as fast-scan DSC (F-DSC). These various thermal methods characterize the mechanical properties, mass, temperature, heat and/or specific heat capacity changes in the thermodynamic and kinetic transitions of different materials, such as low molecular-mass substances, amorphous and semicrystalline synthetic polymers and also biopolymers. Moreover, thermal analysis can also help quantitatively monitor the structural changes of materials during heating, cooling and isothermal measurement. In this Special Issue, we will continue to highlight the recent accomplishments of thermal analysis on polymer-based materials, and illustrate new methods developed in the field. We hope these reviews and research studies can provide a broad view of how material thermodynamic theories and methods have been used in the last decade.

Dr. Xiao Hu
Guest Editor

Keywords

Thermal analysis
Thermal diffusivity and thermal conductivity
Glass transition, crystallization, melting

Related Special Issues

Thermal Properties and Applications of Polymers III in Polymers (5 articles)
Thermal Properties and Applications of Polymers in Polymers (11 articles)

Published Papers (14 papers)

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Research

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10 pages, 3397 KiB

Open AccessArticle

Electrospun Silk-Boron Nitride Nanofibers with Tunable Structure and Properties

by Ye Xue and Xiao Hu

Polymers 2020, 12(5), 1093; https://doi.org/10.3390/polym12051093 - 11 May 2020

Cited by 6 | Viewed by 3112

Abstract

In this study, hexagonal boron nitride (h-BN) nanosheets and Bombyx mori silk fibroin (SF) proteins were combined and electrospun into BNSF nanofibers with different ratios. It was found that the surface morphology and crosslinking density of the nanofibers can be tuned through the mixing ratios. Fourier transform infrared spectroscopy study showed that pure SF electrospun fibers were dominated by random coils and they gradually became α-helical structures with increasing h-BN nanosheet content, which indicates that the structure of the nanofiber material is tunable. Thermal stability of electrospun BNSF nanofibers were largely improved by the good thermal stability of BN, and the strong interactions between BN and SF molecules were revealed by temperature modulated differential scanning calorimetry (TMDSC). With the addition of BN, the boundary water content also decreased, which may be due to the high hydrophobicity of BN. These results indicate that silk-based BN composite nanofibers can be potentially used in biomedical fields or green environmental research. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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9 pages, 8046 KiB

Open AccessArticle

Thermal Conductivity of Polyisoprene and Polybutadiene from Molecular Dynamics Simulations and Transient Measurements

by Aleksandr Vasilev, Tommy Lorenz and Cornelia Breitkopf

Polymers 2020, 12(5), 1081; https://doi.org/10.3390/polym12051081 - 09 May 2020

Cited by 17 | Viewed by 4589

Abstract

The thermal conductivities of untreated polyisoprene and polybutadiene were calculated by molecular dynamics (MD) simulations using a Green-Kubo approach between −10 °C and 50 °C at atmospheric pressure. For comparison, the thermal conductivities of untreated polyisoprene with a molecular weight of 54,000 g/mol and untreated polybutadiene with a molecular weight of 45,000 g/mol were measured by the transient hot wire method in similar conditions. The simulation results of both polymers are in good agreement with the experimental data. We observed that the MD simulations slightly overestimate the thermal conductivity due to the chosen force field description. Details are discussed in the paper. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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19 pages, 5820 KiB

Open AccessArticle

Effect of Organic Modifier and Clay Content on Non-Isothermal Cold Crystallization and Melting Behavior of Polylactide/Organovermiculite Nanocomposites

by M. Jesús Fernández and M. Dolores Fernández

Polymers 2020, 12(2), 364; https://doi.org/10.3390/polym12020364 - 07 Feb 2020

Cited by 21 | Viewed by 2353

Abstract

In clay/polymer nanocomposites, the crystallization behavior and kinetics of the polymer can be affected by the presence of clay, its content and the degree of miscibility between the clay and the polymer matrix. The effect of two different organomodified vermiculites on the non-isothermal cold crystallization and melting behavior of polylactide (PLA) was studied by differential scanning calorimetry (DSC). In the presence of vermiculites, the cold crystallization of PLA occurred earlier, particularly for the highest content of the most miscible organovermiculite with PLA. The cold crystallinity of PLA decreased at low heating rates, notably at high organoclay loadings, and increased at high heating rates, especially at low vermiculite contents. According to the crystallization half-time, crystallization rate coefficient (CRC), and crystallization rate parameter (CRP) approaches, the cold crystallization rate of PLA increased by incorporating vermiculites, with the effect being most noteworthy for the vermiculite showing better compatibility. The Mo model was successful in describing the non-isothermal cold crystallization kinetics of the PLA/vermiculite composites. The melting behavior was affected by the heating rate and the type and content of clay. The nucleating effect of the most compatible clay resulted in the less perfect crystallites. The activation energy was evaluated using the Kissinger and Takhor methods. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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11 pages, 4314 KiB

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Mechanical and Thermal Properties of All-Wood Biocomposites through Controllable Dissolution of Cellulose with Ionic Liquid

by Ke Chen, Weixin Xu, Yun Ding, Ping Xue, Pinghou Sheng, Hui Qiao, Suwei Wang and Yang Yu

Polymers 2020, 12(2), 361; https://doi.org/10.3390/polym12020361 - 06 Feb 2020

Cited by 7 | Viewed by 2513

Abstract

All-wood biocomposites were prepared with an efficient method. The ionic liquid of 1-butyl-3-methylimidazolium chloride (BMIMCl) was used to impregnate manchurian ash (MA) before hot-pressing, and the all-wood biocomposites were prepared by controllable dissolving and regenerating the cellulose in MA. The Fourier transform infrared analysis suggested that all the components of MA remained unchanged during the preparation. X-ray diffraction, thermogravimetric and scanning electron microscope analysis were carried out to study the process parameters of hot-pressing pressure and time on the crystallinity, thermal properties and microstructure of the all-wood biocomposites. The tensile strength of the prepared all-wood biocomposites reached its highest at 212.6 MPa and was increased by 239% compared with that of the original MA sample. The thermogravimetric analysis indicated that as the thermo-stability of the all-wood biocomposites increased, the mass of the residual carbon increased from 19.7% to 22.7% under a hot-pressing pressure of 10 MPa. This work provides a simple and promising pathway for the industrial application of high-performance and environmentally friendly all-wood biocomposites. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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14 pages, 3695 KiB

Open AccessArticle

Thermal Analysis and Crystal Structure of Poly(Acrylonitrile-Co-Itaconic Acid) Copolymers Synthesized in Water

by Hailong Zhang, Ling Quan, Aijun Gao, Yuping Tong, Fengjun Shi and Lianghua Xu

Polymers 2020, 12(1), 221; https://doi.org/10.3390/polym12010221 - 16 Jan 2020

Cited by 19 | Viewed by 4507

Abstract

The composition and structure of polyacrylonitrile (PAN) precursors play an important role during thermal stabilization, which influences the properties of the resulting carbon fibers. In this paper, PAN homopolymer and PAN-itaconic (IA) copolymers with different IA contents were synthesized by aqueous phase precipitation polymerization. The effects of IA content on the structure and thermal properties were studied using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), differential scanning calorimetry (DSC), and thermogravimetric analysis (TGA). The morphology of PAN polymers showed that the average size of the PAN particles increased with the increase of IA content in the feed. The content of the IA comonomer on the copolymers was quantitatively characterized by the relative absorbance intensity (A₁₇₃₅/A₂₂₄₃) in FTIR spectrum. With the increase of IA content in the feed, PAN-IA copolymers exhibited lower degree of crystallinity and crystal size than the control PAN homopolymer. The results from DSC curves indicated that PAN-IA1.0 copolymers had lower initial exothermic temperature (192.4 °C) and velocity of evolving heat (6.33 J g⁻¹ °C⁻¹) in comparison with PAN homopolymer (T_i = 238.1 °C and ΔH/ΔT = 34.6 J g⁻¹ °C⁻¹) in an air atmosphere. TGA results suggested that PAN-IA1.0 copolymers had higher thermal stability than PAN homopolymer, which can form a ladder structure easier during thermal processing. Therefore, PAN-IA1.0 copolymers would be a suitable candidate for preparing high performance PAN based carbon fibers. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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18 pages, 5143 KiB

Open AccessArticle

Investigation on the Effect of Hyperbranched Polyester Grafted Graphene Oxide on the Crystallization Behaviors of β-Nucleated Isotactic Polypropylene

by Yansong Yu, Xi Jiang, Yiwei Fang, Jinyao Chen, Jian Kang, Ya Cao and Ming Xiang

Polymers 2019, 11(12), 1988; https://doi.org/10.3390/polym11121988 - 02 Dec 2019

Cited by 9 | Viewed by 2622

Abstract

In this article, hyperbranched polyester grafted graphene oxide (GO) was successfully prepared. X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), and transmission electron microscopy (TEM) were performed for its characterizations. On the other hand, differential scanning calorimetry (DSC) and wide-angle X-ray diffraction (WAXD) were also performed to study its influences on non-isothermal crystallization behaviors of β-nucleated isotactic polypropylene (β-iPP). The grafting ratios of hyperbranched polyester with different supermolecular structures were calculated to be 19.8–24.0 wt %, which increase with the degree of branching. The results showed that the grafting of hyperbranched polyester was advantageous in increasing the crystallization peak temperature T_p and decreasing the crystallization activation energy ΔE of β-iPP/GO composites, which contributed to the iPP’s crystallization process. Moreover, under all cooling rates (2, 5, 10, 20, 40 °C/min), crystallinities of β-iPP/GO were greatly improved after being grafted with hyperbranched polyester, because of the increase of the relative contents of α-phase α_c and the average α-crystal sizes. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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9 pages, 2134 KiB

Open AccessArticle

Ablation Behavior of Silicone Rubber-Benzoxazine-Based Composites for Ultra-High Temperature Applications

by Jinglong Gao, Zhixuan Li, Jiayi Li and Yanhui Liu

Polymers 2019, 11(11), 1844; https://doi.org/10.3390/polym11111844 - 08 Nov 2019

Cited by 10 | Viewed by 3859

Abstract

A novel type of silicon rubber composite with benzoxazine resins (BZs) and ZrO₂ was prepared. The ablative response of the composites was investigated. The results showed that the composites with BZs had superior thermal stability and higher resides compared to the pristine composites. The linear ablation rate of the composites decreased significantly with the increase in ZrO₂ content. The maximum back-face temperature of the burnt samples was no more than 100 °C for the obtained composites. Three major ablation processes were carried out simultaneously during the ablation processing. These mainly involved the carbonization of the composite, and the formation of ceramic compounds such as SiC and ZrC, as well as the shielding effect of the ablated layer, which subsequently enhanced the ablation resistance of the composites. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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21 pages, 6973 KiB

Open AccessArticle

Preparation of a Novel Fracturing Fluid System with Excellent Elasticity and Low Friction

by Yang Zhang, Jincheng Mao, Jinzhou Zhao, Tao Xu, Anqi Du, Zhaoyang Zhang, Wenlong Zhang and Shaoyun Ma

Polymers 2019, 11(10), 1539; https://doi.org/10.3390/polym11101539 - 20 Sep 2019

Cited by 19 | Viewed by 3107

Abstract

The quaternary polymer was synthesized by radical polymerization and characterized by ¹H NMR. The tests of critical associating concentration and SEM suggest that there is a multilayered and robust network structure in the polymer solution. An excellent elasticity in the polymer solution by the first normal stress difference, viscoelasticity, and thixotropy was observed. The critical crosslinker concentration of polymer with sodium dodecyl sulfate and its interaction mechanism were investigated. According to the reaction kinetics, the supramolecular structure had the lowest activation energy, stable network structure, and greater thermal stability. Then the polymer was employed in the fracturing fluid due to its excellent elasticity using the intermolecular forces, which showed superior sand suspension capacity by dynamic sand suspension measurement. Meanwhile, a theoretical analysis was proposed as to why polymer solution has excellent suspension and drag reduction properties. Therefore, this polymer could be an alternative in many fields, especially in fracking, which is significant for the development of oil and gas resources in deep wells. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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15 pages, 4353 KiB

Open AccessArticle

Study on the Anticondensation Characteristics of Liquid Silicone Rubber Temperature-Control Coatings

by Juyi Guo, Xilin Wang, Jun Wang, Chuan Chen, Yu Liu, Weinan Fan and Zhidong Jia

Polymers 2019, 11(8), 1282; https://doi.org/10.3390/polym11081282 - 01 Aug 2019

Cited by 5 | Viewed by 3003

Abstract

Metal cabinets such as switch cabinets and ring network cabinets have the advantages of small footprints and good protection for equipment and offer neat and orderly protection. They are widely used in power systems. In a hot and humid environment, condensation can easily cause equipment to age and even cause insulation failure. Therefore, research on reliable anticondensation methods is of great significance for the safe operation of power equipment. In this study, phase change capsules with phase transition temperatures of 22 and 32 °C were used as fillers and liquid silicone rubber was used as a matrix to prepare liquid silicone rubber composites filled with phase change capsules for a temperature-control coating. Studies have shown that liquid silicone rubber coatings containing phase change capsules can significantly enhance the anticondensation performance of metal cabinets. By using a temperature-control coating on the surface where the cabinet experiences condensation, the temperature difference between the surface and the dew point is reduced, thereby slowing down the condensation rate and even preventing condensation. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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11 pages, 3939 KiB

Open AccessArticle

Preparation and Thermal Evaluation of Novel Polyimide Protective Coatings for Quartz Capillary Chromatographic Columns Operated over 320 °C for High-Temperature Gas Chromatography Analysis

by Meng-ge Huangfu, Yan Zhang, Xin-ling Zhang, Jin-gang Liu, Ying-cong Liu, Yi-dan Guo, Qing-yuan Huang and Xiu-min Zhang

Polymers 2019, 11(6), 946; https://doi.org/10.3390/polym11060946 - 01 Jun 2019

Cited by 9 | Viewed by 2943

Abstract

Protection of intrinsically brittle quartz chromatographic columns (CCs) from breakage or property deterioration in gas chromatography (GC) analysis has become an important research topic regarding high-temperature GC techniques. Polyimide (PI) has proved to be the most suitable protective coating for quartz CCs. In the current research, a series of novel high-temperature-resistant PI coatings for quartz CCs operated over 320 °C have been successfully prepared. For this purpose, the aromatic diamine with a rigid skeleton structure 2-(4-aminophenyl)-5-aminobenzimidazole (APBI) was copolymerized with two aromatic dianhydrides—3,3’,4,4’-benzophenotetracarboxylic acid dianhydride (BTDA) and 4,4’-oxydiphthalic anhydride (ODPA)—and an aromatic diamine with flexible ether linkages—4,4’-oxydianiline (ODA)—by a two-step polymerization procedure via soluble poly(amic acid) (PAA) precursors, followed by thermal imidization at elevated temperatures. The developed PI coatings exhibited good comprehensive properties, including glass transition temperatures (T_g) as high as 346.9 °C, measured by dynamic mechanical analysis (DMA), and coefficients of linear thermal expansion (CTEs) as low as 24.6 × 10⁻⁶/K in the range of 50–300 °C. In addition, the PI coatings exhibited good adhesion to the fused quartz capillary columns. No cracking, delamination, warpage, or other failures occurred during the 100-cycle thermal shock test in the range of 25–320 °C. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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13 pages, 2914 KiB

Open AccessArticle

Crosslinking Effect on Thermal Conductivity of Electrospun Poly(acrylic acid) Nanofibers

by Yeongcheol Park, Suyeong Lee, Sung Soo Ha, Bernard Alunda, Do Young Noh, Yong Joong Lee, Sangwon Kim and Jae Hun Seol

Polymers 2019, 11(5), 858; https://doi.org/10.3390/polym11050858 - 10 May 2019

Cited by 18 | Viewed by 8057

Abstract

The thermal conductivity (k) of poly(acrylic acid) (PAA) nanofibers, which were electrospun at various electrospinning voltages, was measured using suspended microdevices. While the thermal conductivities of the as-spun PAA nanofibers varied depending on the electrospinning voltages, the most pronounced 3.1-fold increase in thermal conductivity in comparison to that of bulk PAA was observed at the electrospinning voltage of 14 kV. On the other hand, a reduction in the thermal conductivity of the nanofibers was observed when the as-spun nanofibers were either thermally annealed at the glass transition temperature of PAA or thermally crosslinked. It is notable that the thermal conductivity of crosslinked PAA nanofibers was comparable to that of crosslinked bulk PAA. Polarized Raman spectroscopy and Fourier transform infrared spectroscopy verified that the k enhancement via electrospinning and the k reduction by the thermal treatments could be attributed to the conformational changes between gauche and trans states, which may be further related to the orientation of molecular chains. In contrast, hydrogen bonds did not contribute significantly to the k enhancement. Additionally, the suppression of k observed for the crosslinked PAA nanofibers might result from the shortening of single molecular chains via crosslinking. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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14 pages, 6646 KiB

Open AccessArticle

Thermal Analysis of Crystallization and Phase Transition in Novel Polyethylene Glycol Grafted Butene-1 Copolymers

by Chuanbin An, Yulian Li, Yahui Lou, Dongpo Song, Bin Wang, Li Pan, Zhe Ma and Yuesheng Li

Polymers 2019, 11(5), 837; https://doi.org/10.3390/polym11050837 - 08 May 2019

Cited by 9 | Viewed by 4283

Abstract

Copolymerization is an effective strategy to regulate the molecular structure and tune crystalline structures. In this work, novel butene-1 copolymers with different polyethylene glycol (PEG) grafts (number-average molecular weight M_n = 750, 2000, and 4000 g/mol) were synthesized, for the first time introducing long-chain grafts to the polybutene-1 main chain. For these PEG-grafted copolymers, crystallization, melting, and phase transition behaviors were explored using differential scanning calorimetry. With respect to the linear homopolymer, the incorporation of a trimethylsilyl group decreases the cooling crystallization temperature (T_c), whereas the presence of the long PEG grafts unexpectedly elevates T_c. For isothermal crystallization, a critical temperature was found at 70 °C, below which all polyethylene glycol-grafted butene-1 (PB-PEG) copolymers have faster crystallization kinetics than polybutene-1 (PB). The subsequent melting process shows that for the identical crystallization temperature, generated PB-PEG crystallites always have lower melting temperatures than that of PB. Moreover, the II-I phase transition behavior of copolymers is also dependent on the length of PEG grafts. When form II, obtained from isothermal crystallization at 60 °C, was annealed at 25 °C, PB-PEG-750, with the shortest PEG grafts of M_n = 750 g/mol, could have the faster transition rate than PB. However, PB-PEG-750 exhibits a negative correlation between transition rate and crystallization temperature. Differently, in PB-PEG copolymers with PEG grafts M_n = 2000 and 4000 g/mol, transition rates rise with elevating crystallization temperature, which is similar with homopolymer PB. Therefore, the grafting of the PEG side chain provides the available method to tune phase transition without sacrificing crystallization capability in butene-1 copolymers. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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18 pages, 3396 KiB

Open AccessArticle

Preparation of a Hydrophobic-Associating Polymer with Ultra-High Salt Resistance Using Synergistic Effect

by Yang Zhang, Jincheng Mao, Jinzhou Zhao, Xiaojiang Yang, Tao Xu, Chong Lin, Jinhua Mao, Hongzhong Tan, Zhaoyang Zhang, Bo Yang and Shaoyun Ma

Polymers 2019, 11(4), 626; https://doi.org/10.3390/polym11040626 - 04 Apr 2019

Cited by 30 | Viewed by 4511

Abstract

Polymer, SRP-2-1, was synthesized by micellar polymerization and characterized by ¹H NMR. Salt tolerance and viscoelasticity tests verified that the salt resistance of SRP-2-1 was promoted by the synergistic effects of oxyethylene groups, sulfonate, and hydrophobic chains. It is suggested that the structure of SRP-2-1 became more compact with increasing salinity. Furthermore, a mechanism is proposed as to why SRP-2-1 solution has excellent salt-resistance properties. The experimental results indicate that, because of the good shear resistance properties, the polymer SRP-2-1 could be used as an alternative in many fields, for instance in fracturing fluids, enhanced oil recovery, and sewage treatment. Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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21 pages, 3864 KiB

Open AccessReview

Application of Differential Scanning Calorimetry (DSC) and Modulated Differential Scanning Calorimetry (MDSC) in Food and Drug Industries

by César Leyva-Porras, Pedro Cruz-Alcantar, Vicente Espinosa-Solís, Eduardo Martínez-Guerra, Claudia I. Piñón-Balderrama, Isaac Compean Martínez and María Z. Saavedra-Leos

Polymers 2020, 12(1), 5; https://doi.org/10.3390/polym12010005 - 18 Dec 2019

Cited by 113 | Viewed by 40030

Abstract

Phase transition issues in the field of foods and drugs have significantly influenced these industries and consequently attracted the attention of scientists and engineers. The study of thermodynamic parameters such as the glass transition temperature (Tg), melting temperature (Tm), crystallization temperature (Tc), enthalpy (H), and heat capacity (Cp) may provide important information that can be used in the development of new products and improvement of those already in the market. The techniques most commonly employed for characterizing phase transitions are thermogravimetric analysis (TGA), dynamic mechanical analysis (DMA), thermomechanical analysis (TMA), and differential scanning calorimetry (DSC). Among these techniques, DSC is preferred because it allows the detection of transitions in a wide range of temperatures (−90 to 550 °C) and ease in the quantitative and qualitative analysis of the transitions. However, the standard DSC still presents some limitations that may reduce the accuracy and precision of measurements. The modulated differential scanning calorimetry (MDSC) has overcome some of these issues by employing sinusoidally modulated heating rates, which are used to determine the heat capacity. Another variant of the MDSC is the supercooling MDSC (SMDSC). SMDSC allows the detection of more complex thermal events such as solid–solid (Ts-s) transitions, liquid–liquid (Tl-l) transitions, and vitrification and devitrification temperatures (Tv and Tdv, respectively), which are typically found at the supercooling temperatures (Tco). The main advantage of MDSC relies on the accurate detection of complex transitions and the possibility of distinguishing reversible events (dependent on the heat capacity) from non-reversible events (dependent on kinetics). Full article

(This article belongs to the Special Issue Thermal Properties and Applications of Polymers II)

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