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Preparation and Characterization of Some Sol-Gel Modified Silica Coatings Deposited on Polyvinyl Chloride (PVC) Substrates

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Preparation and Characterization of Some Sol-Gel Modified Silica Coatings Deposited on Polyvinyl Chloride (PVC) Substrates coatings Article Preparation and Characterization of Some Sol-Gel Modified Silica Coatings Deposited on Polyvinyl Chloride (PVC) Substrates 1 1 1, 1 1 Violeta Purcar , Valentin Rădit, oiu , Alina Rădit, oiu *, Raluca Manea , Florentina Monica Raduly , Georgiana Cornelia Ispas 1, Adriana Nicoleta Frone 1 , Cristian Andi Nicolae 1 , Raluca Augusta Gabor 1, Mihai Anastasescu 2 , Hermine Stroescu 2 and Simona Căprărescu 3 1 The National Institute for Research & Development in Chemistry and Petrochemistry—ICECHIM, Splaiul Independentei No. 202, 6th District, 060021 Bucharest, Romania; [email protected] (V.P.); [email protected] (V.R.); [email protected] (R.M.); [email protected] (F.M.R.); [email protected] (G.C.I.); [email protected] (A.N.F.); [email protected] (C.A.N.); [email protected] (R.A.G.) 2 Institute of Physical Chemistry “Ilie Murgulescu” of the Romanian Academy, Splaiul Independentei No. 202, 6th District, 060021 Bucharest, Romania; [email protected] (M.A.); [email protected] (H.S.) 3 Department of Inorganic Chemistry, Physical Chemistry and Electrochemistry, Faculty of Applied Chemistry and Materials Science, University POLITEHNICA of Bucharest, Polizu Street No. 1-7, 011061 Bucharest, Romania; [email protected] * Correspondence: [email protected] Abstract: Transparent and antireflective coatings were prepared by deposition of modified silica materials onto polyvinyl chloride (PVC) substrates. These materials were obtained by the sol-gel ◦ route in acidic medium, at room temperature (25 C), using different alkoxysilanes with various functional groups (methyl, vinyl, octyl or hexadecyl). Physicochemical and microstructural properties Citation: Purcar, V.; R˘aditoiu, V.; , of resulted silica materials and of thin coatings were investigated through Fourier Transforms Infrared R˘aditoiu, A.; Manea, R.; Raduly, F.M.; , Spectroscopy (FTIR), UV-Vis spectroscopy, Thermal Gravimetric Analysis (TGA), Dynamic Mechanical Ispas, G.C.; Frone, A.N.; Nicolae, Analysis (DMA), Atomic Force Microscopy (AFM) and ellipsometric measurements. Wetting behaviors of C.A.; Gabor, R.A.; Anastasescu, M.; Stroescu, H.; et al. Preparation and the silica coatings were evaluated by measurement of static contact angle against water. FTIR spectra Characterization of Some Sol-Gel of materials confirmed the high degree of cross-linking that result from the formation of the inorganic Modified Silica Coatings Deposited backbone through the hydrolysis and polycondensation reactions together with the formation of the on Polyvinyl Chloride (PVC) organic network. These sol-gel silica coatings showed a reduction in the reflectance (10%) compared Substrates. Coatings 2021, 11, 11. with uncoated PVC substrate. AFM reveals that the films are uniform, and adherent to the substrate, https://dx.doi.org/10.3390/ but their morphology is strongly influenced by the chemical composition of the coating matrices. coatings11010011 These silica coatings can be useful for potential electronic and optical devices. Received: 30 November 2020 Keywords: sol-gel materials; PVC substrate; silica coatings; hydrophobic surface; transparency Accepted: 21 December 2020 Published: 24 December 2020 Publisher’s Note: MDPI stays neu- 1. Introduction tral with regard to jurisdictional claims in published maps and institutional Many useful synthetic and/or processing strategies have been developed to prepare affiliations. transparent hydrophobic and super-hydrophobic coatings. Coatings are mainly applied on substrates (e.g., glass, plastic or textiles) for decorative, protective or functional purposes. It was observed that, in most cases, it is a combination of these objectives [1]. Many tech- niques have been carried out to prepare hybrid coatings including plasma etching [2], Copyright: © 2020 by the authors. Li- layer-by-layer film formation [3], electrospinning [4], chemical vapor deposition (CVD) [5] censee MDPI, Basel, Switzerland. This and the sol-gel process [6]. Compared with the mentioned methods, the sol-gel process is article is an open access article distributed the most used method to produce the hybrid silica coatings because: (a) it allows the control under the terms and conditions of the of the product’s chemical composition; (b) it is attractive for coating polymers that have Creative Commons Attribution (CC BY) melting points between 150 and 300 ◦C; (c) uniform coatings can easily be fabricated by license (https://creativecommons.org/ dipping or spin coating; (d) is low cost and a cost-effectiveness technique and (e) ceramic, licenses/by/4.0/). Coatings 2021, 11, 11. https://dx.doi.org/10.3390/coatings11010011 https://www.mdpi.com/journal/coatings Coatings 2021, 11, 11 2 of 13 glass, metal and polymer substrates can be easily coated [7]. Sol-gel route is considered an adequate method to produce smart and green coatings that can be suited to applications in optoelectronics, self-cleaning solar cells, photovoltaics and sensors [8,9]. Chen et al. [10] fabricated the multifunctional coating with superhydrophilic, high transparency, antireflec- tive and self-cleaning properties via a chemical vapor deposition method. They demon- strated that the antifogging and transparency properties were due to the low water contact angles and the decrease of refractive index, respectively. Lin et al. [11] realized sol-gel silica antireflective coatings with amphiphobic property and good transmittance. Gao et al. [12] fabricated antireflective superhydrophobic coatings using three silica-based sols: silica sol prepared in acidic medium, silica nanoparticle suspension prepared according to the Stöber method and mesoporous silica nanoparticle suspension, followed by chemical vapor depo- sition of 1H,1H,2H,2H-perfluorooctyltriethoxysilane. Authors obtained coatings presenting a transmittance of 95.3% at the wavelength of 630 nm. Ellis-Terrell et al. [13] reported the preparation of silica nanoparticle spray coatings on stainless steel and aluminum coupons. The results revealed that functional silica nanoparticles coating exhibited both superhydrophobic and oleophobic wetting properties (water contact angle ≥ 150◦ and oil contact angle ≥ 140◦), at lower temperatures (100 ◦C). Tasleem et al. [14] synthesized transparent hybrid silica hydrophobic coatings using the chemical surfactant trimethoxy- octylsilane and green surfactants (Nelumbo nucifera). They showed that the hybrid silica coatings displayed good transparency, low surface energy and superhydrophobic prop- erty Eshaghi immobilized the nano-hybrid coatings on polycarbonate (PC) substrates through the sol-gel method, using silica nanoparticles, 3-glycidoxypropyltrimethoxysilane (GPTMS) and perfluorooctyltrichlorosilane (PFTS) [15]. Maghrebi reports the prepara- tion of polyimide-silica hybrid films with nanostructure using the sol-gel technique by hydrolysis–polycondensation of tetraethoxysilane (TEOS) in the polyamic acid solution [16]. Wang et al. [17] obtained superhydrophobic transparent film on a glass substrate by hy- drolyzing the tetraethoxysilane (TEOS) in an acidic environment and then reacted with hexamethyldisilazane (HMDS). Islam et al. [18] reported that nanoparticle optical coating of silica and titania on polymer substrate PMMA can be prepared via a sol-gel method, at room temperature. Ortelli et al. [19] reported the preparation of organic–inorganic hybrid compositions (ceramers) through the sol-gel process, using different alkoxysilane precursors (trimethoxymethylsilane (TMEOS), (3-aminopropyl) trimethoxyalkoxysilane (APTMS) and tetraethoxysilane (TEOS)). The obtained results showed that the ceramer coatings exhibit thermal stability and water repellency properties. Fasce et al. [20] prepared the poly (ethylene oxide)/silica hybrid coatings (PEO-Si/SiO2), deposited onto a PVC substrate, obtaining coatings with uniform thickness. Al-Bataineh et al. [21] demonstrated that the polyvinyl chloride (PVC)/polystyrene (PS) hybrid films doped with silica nanopar- ticles with high transmittance (>80%) can be achieved by using the dip-coating method. Abdel-Baset et al. [22] showed that the silica nanoparticles (SiO2 NPs), synthesized by the sol-gel method, could be well dispersed on the PVC films surface in order to obtain transparent PVC-SiO2 nanocomposite films [22]. Sutar et al. [23] reported the prepara- tion of superhydrophobic coating by applying the multiple layers of PVC/SiO2 NPs on glass substrate. In the present study, the transparent and antireflective coatings were prepared by de- positing the silica materials on the plastic substrates (polyvinyl chloride (PVC)). Silica materials were synthetized via a sol-gel process, in acidic medium, at room tem- perature (25 ◦C), using different alkoxysilanes as silica sources: tetraethoxysilane (TEOS), methyltriethoxysilane (MTES), vinyltrimethoxysilane (VTMES), octyltriethoxysilane (OTES) and hexadecyltrimethoxysilane (HDTMES). This method was chosen because it is feasible for low cost, cost-effectiveness and large-scale production. Physicochemical and microstruc- tural properties of resulted silica materials and of coatings were investigated through FTIR and UV–Vis spectroscopy, TGA and DMA analysis, AFM, ellipsometric and water contact angle measurements. To our best knowledge, there are only a few studies that demonstrated the hydrophobic and antireflective properties of the silica coatings on the PVC substrate. Coatings 2021, 11, 11 3 of 13 2. Materials and Methods 2.1. Materials Tetraethoxysilane (C8H20O4Si (TEOS), 98%, Aldrich, St.
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