72 lines
47 KiB
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72 lines
47 KiB
JSON
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"id": 1,
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"chunk": "# Hydrophilic nano-SiO /PVA-based coating with durable antifogging properties \n\nGuoqiang Wu, Yuling Yang, Yongtong Lei, Dapeng Fu, Yuchao Li, Yanhu Zhan, Jinming Zhen, Mouyong Teng \n\n$\\circleddash$ American Coatings Association 2020 \n\nAbstract Hydrophilic $\\mathrm{SiO}_{2}/$ poly(vinyl alcohol) (PVA) coating prepared by solution blended method showed high light transmittance and durable antifogging performance. The effects of $\\mathrm{SiO}_{2}$ content and $\\mathrm{p}\\mathrm{\\bar{H}}$ value of $\\mathrm{SiO}_{2}$ suspension on the morphology and properties of hydrophilic coating were studied by Fourier transform infrared spectroscopy, scanning electron microscopy, atomic force microscopy, contact angle test, ultraviolet visible light spectrophotometer, and antifogging test. Results showed that the PVA had good compatibility with nano- $\\mathrm{SiO}_{2}$ because of the formation of $S_{\\mathrm{i-O-C}}$ chemical bond at the interface between nano- $S\\mathrm{i}0_{2}$ and PVA. When prepared at $\\mathrm{pH}=7$ , $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coatings $\\mathbf{\\dot{SiO}}_{2}/\\mathbf{PVA}$ mass ratio of 0.8) were hydrophilic, with a water contact angle of $22.9^{\\circ}$ , and exhibited papilla-like surface features $(\\mathbf{RMS}=7.6~\\mathrm{nm}$ ). Polyethylene (PE) samples coated with this $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ film exhibited a light transmittance of up to $90\\%$ , between 560 and $700~\\mathrm{nm}$ , and remained fog-free for more than 1 month after exposure to water at $60^{\\circ}\\mathrm{C}$ (QB/T 4475-2013 standard). Water-resisting and wear-resisting tests revealed that antifogging coatings demonstrated excellent mechanical properties. \n\nKeywords Hydrophilic coating, Papilla-like structures, High transmittance, Durable antifogging",
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"category": " Abstract"
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"id": 2,
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"chunk": "# Introduction \n\nFogging occurs when water molecules condense as discrete droplets with diameters larger than $190~\\mathrm{nm}$ or half of the shortest wavelength $\\left(380\\ \\mathrm{nm}\\right)$ of visible light.1 This phenomenon is harmful to optical materials and analytical and medical instruments, such as eyeglasses,2 goggles, solar cells,3 face shields, binoculars, microscopes,4 and laparoscopes.5 Fogging is also common in agricultural greenhouses where a polymer film, such as polyethylene (PE), is used as a barrier to protect growing plants.6 The occurrence of fogging results in a number of side effects, including poor film clarity and reduced light transmittance. Several research groups have developed polymer films with antifogging performance by depositing hydrophilic coatings.7–12 An efficient way to prevent fog is to increase the surface energy that can form a hydrophilic surface for polymer films. Water drops lying on a (super)hydrophilic surface spread across it to form a transparent and continuous thin film of water. The resulting layer of water allows for the incident light to pass through it without being scattered, thus attaining the antifogging effect.13–16 \n\nSo far, two main strategies have been explored to produce antifogging coatings with water-attracting characteristics. The first strategy uses inorganic nanoparticles to create one or more layers of micron-/nanometer-scale roughness on the surface of the substrate. Various types of nanoparticles are available for the creation of surface roughness, such as $\\mathrm{TiO}_{2}$ ,8 $\\mathbf{SiO}_{2,\\dots,\\dots}^{\\phantom{-}17-19}$ faujasitic nanozeolites,20 $Z_{\\mathrm{{nO},\\l}}{}^{21}$ $\\mathbf{Z}\\mathbf{r}\\mathbf{O}_{2}$ , or ${\\bf W}{\\bf O}_{3}$ .22,23 Saxena et al.17 deposited a dendritic pattern of $\\mathrm{TiO}_{2}$ and $\\mathrm{SiO}_{2}$ on the transparent glass surface by the template method. The patterns of only $\\mathrm{SiO}_{2}$ and $\\mathrm{TiO}_{2}$ nanoparticles are attained on the glass surface after calcining the template at $450^{\\circ}\\mathrm{C}$ The surface of the glass showed superhydrophilic and antifogging performance. Chen et al.18 fabricated a multifunctional $\\mathrm{SiO}_{2}$ coating via a low-cost one-step chemical vapor deposition method. In particular, the 10-h-deposited silica nanoparticles’ thin coating surface showed the best hydrophilicity, transparency, antifogging, and self-cleaning properties. The second strategy to prepare antifogging coatings consists of depositing polymers or monomers containing hydrophilic functionalities, such as – OH or –COOH groups. For example, hydrophilic coatings have been achieved by depositing acrylic resin,24,25 silicone,26 poly(vinyl alcohol) (PVA),12,27–29 poly(vinyl acetate), poly(ethylene glycol),30 cellulose ester or cellulose ether,11,31 and poly(vinylpyrrolidone) (PVP).32 Lee et al.28 obtained a hydrophilic coating by hydrogen-bonding-assisted layer-by-layer assembly using PVA and poly(acrylic acid) (PAA) with excellent antifogging and frostresistant properties. Nuraje et al.2 prepared a hydrophilic surface with carboxymethyl cellulose and oligomeric chitosan on polycarbonate and glass samples, The results show that the anti-fog property is related to intermolecular hydrogen bonding and surface water film. The above-mentioned hydrophilic coatings showed excellent antifogging property; however, the fabrication steps were tedious and complex, usually requiring multistep, expensive fabrication techniques. \n\nPVA is a water-soluble polymer having the properties of good compactness, high crystallinity, strong adhesion, nontoxicity, being odorless and harmless to the human body, and good affinity for water molecules.12,16 The PVA molecule contains a large amount of hydroxyl groups and is highly hydrophilic. The addition of nano- $\\mathrm{\\cdot}\\mathrm{\\dot{SiO}}_{2}$ into PVA can improve the network structure, enhance the mechanical properties of the film, and improve its thermal stability and water resistance.33 Tong et al.34 prepared the noncharged $\\mathrm{PVA}/\\mathrm{SiO}_{2}$ hybrid films through sol–gel process for alkali recovery. The hybrid films can be potentially used to separate $\\mathrm{\\DeltaNaOH/Na_{2}W O_{4}}$ solution. Liu et al.35 reported the $\\mathrm{PVA}/\\mathrm{SiO}_{2}$ hybrid coatings via ‘‘one-step’’ hydrolysis and co-condensation, with the ability to separate oil/water immiscible mixture from highly acidic, alkaline, and salty environment. In this study, we fabricated hydrophilic nano- $\\mathrm{SiO}_{2}/$ PVA coating by solution blending method and deposited the surface on PE film by dip coating technique for the first time. The structure of hydrophilic coating was observed by SEM, AFM, and FTIR. The hydrophilic property was studied by water contact angle test. The transmittances of the coated PE were investigated. Furthermore, the antifogging property of the coated PE was also studied by the self-made antifog-measuring instrument and the mechanical properties (water-resisting and wear-resisting property) of the hydrophilic coating were also tested.",
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"category": " Introduction"
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"id": 3,
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"chunk": "# Experimental",
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"category": " Materials and methods"
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"id": 4,
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"chunk": "# Materials \n\nCorona-treated PE films with $0.1\\mathrm{mm}$ thickness were obtained from Shandong Dongda Plastic Industry $\\scriptstyle{\\mathrm{Co}}$ ., Ltd. Haq et al.36 reported that corona discharge treatment can significantly improve the wettability of the PE surface so that the hydrophilic coatings prepared in this study are expected to spread across it evenly. Poly(vinyl alcohol) (PVA, $\\bar{M}_{\\mathrm{n}}=70{,}000{-}$ 90,000, $99\\%$ hydrolyzed) was purchased from Sinopec Chongqing SVM Chemical $\\scriptstyle{\\mathrm{Co}}$ , Ltd. The colloidal silica nanoparticles Ludox N2010 $(20~\\mathrm{wt\\%}$ $\\mathrm{SiO}_{2}$ suspension, average particle size of $12\\ \\mathrm{nm}$ , and $\\mathrm{pH}$ value of 7) and Ludox SS3010 ( $(30~\\mathrm{wt\\%}$ $\\mathrm{SiO}_{2}$ suspension, average particle size of $8\\ \\mathrm{nm}$ , and $\\mathrm{pH}$ value of 10) were obtained from Shandong Peak-Tech New Material $\\mathrm{Co}$ ., Ltd. The fluorocarbon surfactant (FA-6812) was supplied by Horizon Admixtures $\\scriptstyle{\\mathrm{Co}}$ , Ltd. Deionized water was exclusively used in all aqueous solutions and rinsing procedures.",
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"category": " Materials and methods"
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"id": 5,
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"chunk": "# Preparation \n\nHydrophilic coating was deposited on PE substrates by one-step dip coating followed by solution blending method. Solution blending process is a simple and convenient method, which can be applied to fabricate various thin films.9,37,38 A brief description follows. First, PVA solution $(5~\\mathrm{wt\\%}$ in water) was mixed with Ludox (N2010, SS3010) via mechanical stirring for $^{1\\mathrm{~h~}}$ . The aforementioned solution was then diluted with deionized water followed by the addition of fluorocarbon surfactant in one thousandth to the solution in order to reduce the surface tension. Then, the PE film was immersed in the hybrid solution for $5\\mathrm{\\textbf{s}}$ Finally, the PE film was thermal-treated for $5\\mathrm{{min}}$ at $80^{\\circ}\\mathrm{C}$ to evaporate solvent. Three $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ ratios and two $\\mathrm{pH}$ values were used in this work to prepare hydrophilic coatings. The assembly of hydrophilic coating is designated as (Y$\\mathbf{PV}\\mathbf{A})_{\\mathbf{x}}$ , in which x and Y represent the mass ratio of $\\mathrm{SiO}_{2}$ to PVA and the kind of Ludox, respectively. For example, $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.8}$ means that the mass ratio of Ludox N2010 to PVA is 0.8. Table 1 lists the mass ratios of $\\mathrm{SiO}_{2}$ to PVA in the antifogging coatings.",
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"category": " Materials and methods"
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"id": 6,
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"chunk": "# Characterization \n\nThe surface morphologies of the deposited coatings were examined by field emission scanning electron microscopy (FE-SEM) on a German Zeiss scanning electron microscope. Water contact angles on deposited coatings were measured at room temperature on a JC2000 contact angle measuring instrument (Shanghai Zhongchen Digital Technique Apparatus Co., Ltd). Water droplets of $2.0~\\upmu\\mathrm{L}$ were dropped carefully onto the thin-film surfaces. At least three positions were tested in order to get the average value. Atomic force microscopic (AFM) images of the deposited coatings were captured with a SPA-300HV environment controlled scanning probe microscope (Japan Seiko). The scanning frequency was $0.8\\mathrm{Hz}$ . The scanning size was $1.5~{\\upmu\\mathrm{m}}\\times1.5~{\\upmu\\mathrm{m}}$ . At least three positions were tested in order to get the average value. Transmission spectra in the wavelength range of $300{\\mathrm{-}}900\\ \\mathrm{nm}$ were recorded using a UV-3600 spectrophotometer (Shimadzu, Japan). The hybrid solution particle size and its distribution were determined with a laser particle analyzer (90Plus S/N) from Brookhaven (America). FTIR spectra of samples dispersed in KBr pellets were obtained by Nicolet IR-100 spectrometer in a spectra range of $400{\\-}4000~\\mathrm{cm}^{-1}$ . The antifogging performance of the coated PE films was tested according to the protocol defined in the QB/T 4475-2013 standard using a laboratory-made device (Fig. 1).39 The PE film was placed on the round opening (diameter of $115~\\mathrm{mm}$ ) of the instrument. The water was kept at ${}60^{\\circ}\\mathrm{C}$ in the instrument while observing and recording the surface antifogging performance of the PE film. Freeze tests were performed by placing the two PE films in the freezer at $20^{\\circ}\\mathrm{C}$ for $20~\\mathrm{min}$ . PE films were removed and then placed in the humid laboratory air. Vapor condensed on the PE film surface was observed and photographed. Reliability of the antifogging performance of the coated PE films was tested by rubbing, using a soaked sponge rotating at 50 cycles per minute for up to 20 cycles and by exposure to a continuous water scouring for $12\\mathrm{~h~}$ . \n\n<html><body><table><tr><td>Table1: Chemical antifogging layer (SiO2/PVA in mass ratio) Sample code</td><td>species for Ludox N2010 (pH = 7)</td><td>preparing LudoxSS3010</td><td>the PVA</td></tr><tr><td></td><td></td><td>(pH = 10)</td><td>(5%)</td></tr><tr><td>PVA (N2010-PVA)0.4</td><td>0 0.4</td><td>0 0</td><td>1 1</td></tr><tr><td>(N2010-PVA)0.8</td><td>0.8</td><td>0</td><td>1</td></tr><tr><td>(N2010-PVA)2</td><td>2</td><td>0</td><td>1</td></tr><tr><td>(SS3010-PVA)0.4</td><td>0</td><td>0.4</td><td>1</td></tr><tr><td>(SS3010-PVA)0.8</td><td>0</td><td>0.8</td><td>1</td></tr><tr><td>(SS3010-PVA)2</td><td>0</td><td>2</td><td>1</td></tr><tr><td>Ludox N2010</td><td>1</td><td>0</td><td>0</td></tr><tr><td></td><td></td><td></td><td></td></tr></table></body></html>",
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"category": " Materials and methods"
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},
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"id": 7,
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"chunk": "# Results and discussion",
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"category": " Results and discussion"
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"id": 8,
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"chunk": "# Chemical composition \n\nFigure 2 illustrates the particle size distributions of the nanocomposite solution. The average diameter of neutral Lodox N2010 was $18.7\\ \\mathrm{nm}$ , while that of the $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.4}$ composite solution was $73.5~\\mathrm{nm}$ . Such increase in the average diameter may be attributed to the encapsulation of PVA chains. As the $(\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A})$ 1 mass ratio increased to 2, the average diameter of the $(\\mathrm{N}2010–\\mathrm{PV}\\mathbf{A})_{2}$ decreased to $49.7~\\mathrm{nm}$ . This is due to the fact that PVA molecule chains can crosslink with the nano- $\\mathrm{.}\\mathrm{SiO}_{2}$ to form much denser particles.33 The average diameter of alkaline Lodox SS3010 is about $16.3\\ \\mathrm{{nm}}$ , while the diameter of $(\\mathrm{SS3010–PVA})_{0.8}$ is $68.6\\ \\mathrm{nm}$ . The neutral and alkaline Lodox showed a similar pattern with no significant difference in the solution. \n\n \nFig. 1: Diagram of fog test \n\n \nFig. 2: Particle size and distribution of nano- $S i O_{2}/P V A$ composite solution. (a) $(\\S\\S\\3010\\mathrm{-}\\mathsf{P V A})_{0.8}$ , (b) (N2010- $\\mathsf{P V}\\mathsf{A})_{0.4},$ , (c) $(\\mathsf{N}2010\\mathsf{-P V}\\mathsf{A})_{0.8},$ (d) $(\\mathsf{N}2010\\mathsf{-P V}\\mathsf{A})_{2}$ , (e) Ludox N2010, (f) Ludox SS3010 \n\nIn order to understand the interaction between the PVA and $\\mathrm{SiO}_{2}$ , the hybrid materials were analyzed by Fourier transform infrared (FTIR) spectroscopy. Figure 3 shows the FTIR spectra of PVA, $\\mathrm{SiO}_{2}$ coating, and $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coating (summarized in Table 2). The characteristic peak found around $3436~\\mathrm{cm}^{-1}$ is associated with stretching vibrations of $-\\mathrm{OH}$ , which decreased with the increase in silica content, indicating the presence of a hydrogen bond.40 The absorption peaks at 2920 and $2\\mathrm{{\\dot{8}58}}\\mathrm{{\\dot{cm}}}^{-1}$ correspond to the $\\mathrm{CH}_{3}$ asymmetric stretching and $\\mathrm{CH}_{2}$ asymmetric stretching vibrations. The peaks at $1382~\\mathrm{cm}^{-\\mathrm{f}}$ are associated with $\\mathrm{CH}_{2}$ wagging vibrations. And the peaks at 1163 and $1071~\\mathrm{cm}^{=1}$ are related to $\\mathrm{C-O}$ bond and $\\scriptstyle{\\mathrm{C-C}}$ group. The characteristic stretching vibration peak intensities of $\\mathrm{Si-O{-}S i}$ group, located at $1102~\\mathrm{{cm}^{-1}}$ and $797~\\mathrm{cm}^{-1}$ , increased gradually with the increase in $\\mathrm{SiO}_{2}$ mass fraction. The peak at $1000~\\mathrm{cm}^{-1}$ represents $\\mathrm{Si-O-C}$ vibration modes due to the overlapping vibrations of $\\mathrm{C-O}$ and $\\mathrm{Si-O}$ bonds.33,41 A similar trend was also observed by Xu et al.,42 who reported the condensation of silanol groups with the $-\\mathrm{O}\\bar{\\mathrm{H}}$ on the PVA molecule chain to form $\\mathrm{Si-O{-}(P V A){-}O{-}S i}$ crosslinks or ‘‘bridges’’. Because a lot of silanol groups had been condensed with the hydroxyls on PVA chain to form Si–O–C linkage, the vibrating intensity of Si–O–Si, Si– OH, and $\\mathrm{\\Gamma_{O-H}}$ bonds was largely weakened. \n\n \nFig. 3: Fourier transform infrared spectra of nano- $\\bullet\\mathrm{i}0_{2}/$ PVA hydrophilic coatings. (a) PVA, (b) $(\\mathsf{N}2010\\mathsf{-P V}\\mathsf{A})_{0.4},$ , (c) $(\\mathsf{N}2010\\mathrm{-}\\mathsf{P}\\mathsf{V}\\mathsf{A})_{0.8}$ , (d) $(\\mathsf{N}\\mathsf{2}\\mathbf{0}\\mathsf{1}\\mathbf{0}\\mathsf{\\mathrm{-}P}\\mathsf{V}\\mathsf{A})_{\\mathsf{2}},$ (e) Ludox N2010, (f) $(\\mathsf{S S3010-P V A})_{0.8}$ \n\nTable 2: Assignments of FTIR absorption bands of films \nPeaks for films $(\\mathsf{c m}^{-1})$ ) \n\n\n<html><body><table><tr><td>PVA</td><td>SiO2/PVA</td><td colspan=\"2\">SiO2</td></tr><tr><td>3436</td><td>3436</td><td>3436</td><td>Stretching of OH</td></tr><tr><td>2920</td><td>2920</td><td>一</td><td>Asymmetric stretching of CH3</td></tr><tr><td>2858</td><td>2858</td><td>一</td><td>Asymmetric stretching of CH2</td></tr><tr><td>1382</td><td>1382</td><td>、</td><td>CH2 wagging</td></tr><tr><td>1163</td><td>1159</td><td>一</td><td>C-O stretching</td></tr><tr><td>1071</td><td>1075</td><td>1</td><td>Stretching of C-C and bending of OH</td></tr><tr><td></td><td>一</td><td>1102</td><td>Si-O-Si</td></tr><tr><td>950</td><td>950</td><td></td><td> O-H bending out-of-plane</td></tr><tr><td>858</td><td>858</td><td>一</td><td>C-C stretching</td></tr><tr><td></td><td></td><td>797</td><td>Si-O-Si</td></tr></table></body></html>",
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"category": " Results and discussion"
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"id": 9,
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"chunk": "# Surface morphology \n\nThe SEM images of PVA, PVA/ $\\mathrm{\\SiO}_{2}$ , and $\\mathrm{SiO}_{2}$ composite coatings are displayed in Fig. 4. From Fig. 4a, it is seen that the PVA coating is smoothly coated on the PE film. For $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.4}^{-}$ , the surface of PE film is coated by silica nanoparticles with a diameter of $18\\pm5~\\mathrm{{nm}}$ , as shown in Fig. 4b. When the $\\mathrm{SiO}_{2}$ concentrations increase from $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.4}$ to $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.8}$ , the size of silica has no change, but the dispersion of $\\mathrm{SiO}_{2}$ particles is more uniform on the surface (Fig. 4c). In Fig. 4e, $\\mathrm{SiO}_{2}$ nanoparticles are evenly dispersed on the surface of PE film. The particles on the surface of PE film become denser with the increase in the content of neutral $\\mathrm{SiO}_{2}$ nanoparticles. However, it is found that the alkaline $\\mathrm{SiO}_{2}$ and PVA of surface structures are different from those of neutral ones and the alkaline $\\mathrm{SiO}_{2}$ nanoparticles are easily aggregated into particles with a particle size of $500\\ \\mathrm{{\\dot{n}m}}$ and dispersed on the surface unevenly (Figs. 4 f–4h). \n\nAFM was employed to disclose the surface morphology and the roughness of the coating surfaces. Figure 5 shows the AFM images of the $\\mathbf{\\bar{SiO}}_{2}/\\mathbf{PV}\\mathbf{A}$ coating surfaces with various $\\mathrm{SiO}_{2}$ concentrations and $\\mathrm{pH}$ values. As shown in Fig. 5a, the surface of PVA coating is flat with an average roughness of $4.4~\\mathrm{nm}$ . When the $\\mathrm{SiO}_{2}$ concentrations increase from (N2010- $\\mathrm{PVA})_{0.4}$ to $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.8}$ , the topographic diagrams of the two samples are similar (Figs. 5b and 5c), which agree well with the results of SEM images. The two surfaces exhibit an average roughness of $6.3~\\mathrm{{nm}}$ and $7.6~\\mathrm{nm}$ , respectively. In contrast, the average roughness of $(\\mathrm{N}2010\\mathrm{-}\\mathrm{PV}\\mathbf{A})_{2}$ decreases to $1.6\\ \\mathrm{nm}$ as shown in Fig. 5d. The $\\mathrm{SiO}_{2}$ nanoparticles accumulate layer by layer, generating holes in the surface due to the high content of $\\mathrm{SiO}_{2}$ . Figure 5e shows that the Ludox N2010 coating is in fact very smooth and dense, and many thin cracks can be noted. The roughness of $\\mathrm{SiO}_{2}$ nanoparticle coating is tested to be only $1.4~\\mathrm{nm}$ . In Fig. 5f, the nano- $\\mathrm{SiO}_{2}$ particles condense into large particles around $500\\ \\mathrm{nm}$ and the roughness reaches $8.6\\ \\mathrm{nm}$ . \n\n \nFig. 4: SEM images of PE film surface with nano- $\\mathsf{s i o}_{2}/\\mathsf{P}\\mathsf{V}\\mathsf{A}$ hydrophilic coatings. (a) PVA, (b) $(\\mathsf{N}2010\\mathsf{-P}\\mathsf{V}\\mathsf{A})_{0.4},$ (c) (N2010- $\\mathsf{P V}\\mathsf{A})_{0.8},$ , (d) $(\\mathsf{N}2010\\mathsf{-P V}\\mathsf{A})_{2}.$ , (e) Ludox N2010, (f) (SS3010-PVA)0.4, (g) (SS3010-PVA)0.8, (h) (SS3010-PVA)2 \n\nThe structural construction of natural plants and animals’ organs has provided inspiration for the wettability film designed and manufactured by humans.43,44 For example, the leaf of the lotus plant, the eyes of peacock, a nymphalid butterfly, and the fly compound eye have a well-arrayed papillae structure. In real life, there are plenty of ordered papillae arrays, which may greatly enhance the stability and wettability of various objects when coated.15 As shown in Figs. 4 and 5, the PVA coating has no obvious structure on the surface of the PE film (Supporting Information 1 shows the 3D AFM image of different specimens). With the addition of $\\mathrm{SiO}_{2}$ (Figs. 4, 5b, and 4 and 5c), the coatings $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.4}$ and $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.8}$ exhibit papilla-like nanostructures on the surface of the PE film and the coating $(\\mathrm{N}2010{\\mathrm{-}}\\mathrm{PV}\\mathrm{A})_{0.8}$ has a more regular papilla-like nanostructure on the surface of the PE film. With further increase in $\\mathrm{SiO}_{2}$ content (Figs. 4 and 5d), the voids of the coating (N2010- $\\mathrm{PVA})_{2}$ on the surface of the PE film are gradually filled and the coating $(\\mathrm{N}2010{\\mathrm{-}}\\mathrm{PV}\\mathrm{A})_{2}$ on the surface roughness is reduced from $7.6\\ \\mathrm{nm}$ [the coating (N2010- $\\mathrm{PVA})_{0.8}]$ to $1.6\\ \\mathrm{nm}$ . In Fig. 5e, the coating of $\\mathrm{SiO}_{2}$ only Ludox N2010 exhibits the minimal nanostructure on the surface of the PE film. The alkaline (SS3010- $\\mathrm{PVA})_{0.8}$ coating exhibits a convex cell structure on the surface of the PE film with the largest voids between adjacent convex cell structures (Fig. 5f). It is known that $\\mathrm{SiO}_{2}$ content and $\\mathrm{pH}$ have important influence on surface morphology.",
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"category": " Results and discussion"
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"id": 10,
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"chunk": "# Surface wettability \n\nEarly theoretical reports by Wenzel45 and Cassie and Baxter46 as well as other studies14,18 suggest that it is possible to significantly change water wettability on a surface by introducing roughness at the right length scale. Wenzel’s roughness equation concludes that roughened surfaces will have a large area of contact between surface and droplet. \n\n$$\n\\cos\\theta^{*}=r\\cos\\theta\n$$ \n\n \nFig. 5: AFM image of PE film surface with nano- $\\mathsf{S i O}_{2}/\\mathsf{P V}\\mathsf{A}$ hydrophilic coatings. (a) PVA, (b) $(\\mathsf{N}2010\\mathsf{-P V}\\mathsf{A})_{0.4},$ (c) (N2010- $\\mathsf{P V}\\mathsf{A})_{0.8}$ , (d) $(\\mathsf{N}2010\\mathsf{-P V}\\mathsf{A})_{2}$ , (e) Ludox N2010, (f) (SS3010-PVA)0.8 \n\nwhere $\\theta^{*}$ is the contact angle on the rough surface, $\\theta$ is the equilibrium contact angle on flat smooth surface, and $r$ is the roughness factor defined as the ratio of the actual surface area of surface to the projected area. From equation (1), for a hydrophilic surface (contact angle $\\mathit{\\Theta}<\\bar{9}0^{\\circ}$ ), the roughness will magnify the hydrophilicity and promote spreading of the droplet, whereas for a hydrophobic surface (contact angle $>$ $90^{\\circ}.$ ), the roughness will magnify the hydrophobicity and retard spreading of the droplet. \n\nThe surface wettability of composite coatings is controlled by chemical composition and morphology of composite surface. Higher hydrophilicity of a coating can be reflected by lower contact angle of water on the surface.47 To examine the hydrophilicity of the composite coating surface, water contact angle measurements were carried out, which are shown in Fig. 6. For the blank PE film, the water droplet does not spread, and the contact angle is $99.5^{\\circ}\\$ (Fig. 6a). In contrast, the PE thin film after being corona treated can improve the surface energy. From Young’s equation [equation (2)], we know that the contact angle of PE thin film surface will decrease with the increase in surface tension: \n\n$$\n\\cos\\theta=\\frac{\\gamma_{S V}-\\gamma_{S L}}{\\gamma_{L V}}\n$$ \n\nwhere $\\theta$ is the contact angle, $\\gamma_{S V}$ is the solid–gas interfacial tension, $\\gamma_{S L}$ is the solid–liquid interfacial tension, and $\\gamma_{S V}$ is the gas–liquid surface tension. The measured water contact angle decreases from $99.5^{\\circ}\\$ to $66.0^{\\circ}$ (from hydrophobic to hydrophilic, in Fig. 6b). The water droplets spread promptly out on PE film surfaces with PVA, $(\\mathrm{N}201{\\bar{0}}{\\mathrm{-}}\\mathrm{PV}{\\bar{\\mathrm{A}}})_{0.4{\\sim}2}$ , and neutral Ludox N2010 coatings (Fig. 6c, d, e, f, and g). The water contact angles change to $28.8^{\\circ}$ , $20.2^{\\circ}$ , $22.9^{\\circ}$ , $23.4^{\\circ}$ , and $23.8^{\\circ}$ at $\\mathrm{~1~s~}$ , respectively. It is found that the water contact angles of the neutral $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ composite coatings are less than those of the pure $\\mathrm{SiO}_{2}$ or PVA coating, which indicates that the structure and morphology generated by the combination of $\\mathrm{SiO}_{2}$ and PVA play a positive role in wettability. In contrast, the water contact angle on PE film with alkaline coatings exhibits the highest of all coatings at $35.5^{\\circ}$ , $29.9^{\\circ}$ and $39.0^{\\circ}$ (Fig. 6h, j, and k). Therefore, the nanoscale morphology on the surface plays a key role in spreading the water droplets.48 \n\n \nFig. 6: Water contact angle on PE film surface with nano$\\mathsf{S i O}_{2}/\\mathsf{P}\\mathsf{V}\\mathsf{A}$ hydrophilic coatings. (a) PE film, (b) PE film (after corona modification), (c) PVA, (d) $(\\mathsf{N}2010\\mathsf{-P}\\mathsf{V}\\mathsf{A})_{0.4},$ (e) (N2010-PVA) 0.8, (f) $(N2010\\mathrm{-}\\mathsf{P V}\\mathsf{A})_{2}$ , (g) Ludox N2010, (h) $(\\S\\S\\3010\\ –\\mathsf{P V A})_{0.4},$ (i) (SS3010-PVA)0.8, (j) (SS3010-PVA)2",
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"category": " Results and discussion"
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},
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{
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"id": 11,
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"chunk": "# The fogging test and optical properties \n\nIt is well known that the moisture condenses to a continuous thin film on hydrophilic or superhydrophilic surfaces, whose water contact angle is less than $4{\\bar{0}}^{\\circ}$ , in order to avoid fogging.14 As discussed above, the transparent and hydrophilic $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coating on PE film surface with a water contact angle of approximately $25^{\\circ}$ was obtained. The PE film with $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coatings was found to exhibit an excellent antifogging behavior, as shown in Fig. 7a and c. Because of the good hydrophilicity of the PE film surface containing $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coatings, it shows antifogging performance in a short time. However, the PE film surface with $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coatings shows poor antifogging property after $168\\mathrm{~h~}$ (Fig. 7d). Fogging appeared on the surface of PE film containing (SS3010-PVA) coating. PVA is gradually dissolved under the action of water vapor, resulting in the poor antifogging property of PE film surface with PVA coatings after $1\\bar{6}8\\mathrm{~h~}$ (Fig. 7d). After $720\\mathrm{{h}}$ , the photographs of PE film with $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coatings are shown in Fig. 7b. Fogging also occurs on the PE film surface with coatings of $(\\mathrm{N}2010{-}\\mathrm{PV}\\mathrm{A})_{0.4}$ and Ludox N2010 as shown in Fig. 7b. The coating containing silica only gradually falls off under the scour of water film for a long time, resulting in poor antifogging performance. The $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.4}$ coating shows a slightly worse antifogging performance than $(\\mathrm{N}2010–\\mathrm{PV}\\mathbf{\\bar{A}})_{0.8,\\ 2}$ coatings because it has a low nano$\\mathrm{SiO}_{2}$ content and the interaction force is small with that of PVA. The composite coating tends to swell and slide on the surface of PE film under moisture. When the distance between nano- $\\mathrm{SiO}_{2}$ particles in the surface coating of PE film is larger than $190~\\mathrm{{nm}}$ or half the shortest wavelength $(380~\\mathrm{nm})$ ) of visible light, large droplets are easily formed without the effect of nanostructures, so the antifogging performance will begin to deteriorate.1 Such phenomenon is also verified in the $(\\mathrm{SS3010–PVA})_{0.8}$ coating because it has convex cell papillae structure with the biggest air voids. In Fig. 7b, the (N2010-PVA)0.8, $_2$ coatings have chemical (formation chemical bond of silicon oxycarbon) and physical interactions (PVA molecular chain is irregular and wound around nano- $\\mathrm{SiO}_{2}$ ) in PE film surface, which finally lead to the stable and durable antifogging performance. A more aggressive fogging test was performed by placing the PE thin films into the freezer at $20^{\\circ}\\mathrm{C}$ for about $20~\\mathrm{min}$ and then moving them into humid laboratory air. As seen in Fig. 8, the blank PE films are fully fogged, whereas the PE film with $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.8}$ coating remains fog free. As a special material with more hydroxy groups, silica and PVA have been used to achieve the antifogging properties. In the research, the $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ coating surfaces are designed to form a special nanostructure, which is similar to the structure of fly compound eye (Supporting Information 2). The hydroxyl group in PVA condenses with the hydroxyl group of silica to form a gel. The gel acts as a crosslinking point in the hydrophilic coating, improving the water resistance of the PVA film. The corona modification can cause pits and oxygen-containing groups on the surface of the PE film.36,49 The thermal expansion coefficient of the PE film and nano- $\\mathrm{SiO}_{2}$ is different during the drying process, which causes the large particles of nano- $\\mathrm{\\dot{\\mathbf{SiO}_{2}}}$ to be anchored like nails on the surface of the PE film. The PVA film containing hydroxyl group exists next to the large particles of $\\mathrm{SiO}_{2}$ . The nano- $\\mathrm{SiO}_{2}$ particles play the role of nails in this case. The PVA film is nailed to the PE surface. This special structure makes the water flow easily on the surface and also reduces the scour effect of the water to the $\\mathrm{SiO}_{2}$ particles. The special nanostructure of $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ composite plays an important role in improving the stability of antifogging coatings. \n\nThe transmission spectra $(350-670~\\mathrm{nm})$ ) of $\\mathrm{SiO}_{2}/$ PVA-coated PE films are shown in Fig. 9. Clearly, in Fig. 9, the biggest transmittance of all samples reaches more than $90\\%$ in the visible light range $(400-670~\\mathrm{nm})$ . The transmittance of the coatings PVA, (N2010- $\\mathrm{PVA})_{0.4}$ , $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.8}$ , $(\\mathrm{N}2010{\\mathrm{-}}\\bar{\\mathrm{P}}\\mathrm{V}\\mathrm{A})_{2}$ , and Ludox N2010 shows a trend of decreasing first and then increasing with the addition of silica, which has a negative correlation with the roughness of the surface of the coatings. The coatings $\\mathbf{\\bar{(N2010-PVA)}_{0.8}}$ and (SS3010-PVA) $_{0.8}$ have large roughness (7.6 and $8.6\\ \\mathrm{nm}$ ), and the transmittance of the surfaces is lowered. In Fig. 9, the disadvantage is that the $(\\mathrm{N}2010{-}\\mathrm{PV}\\mathrm{A})_{0.8}$ hydrophilic coating with good antifogging performance slightly decreases the light transmittance of the PE film, but the biggest transmittance still exceeds $90\\%$ $(350-670~\\mathrm{nm}$ ). \n\n \nFig. 7: Fogging test image on PE film surface with nano-SiO2/PVA hydrophilic coatings (a) nano-SiO2/PVA $(\\mathsf{p H}=7)$ after 0.5 h, (b) nano-SiO2/PVA ( $\\left[\\mathsf{p H}=7\\right)$ after $720\\ h$ , (c) nano-SiO2/PVA $\\left[\\mathsf{p}\\mathsf{H}=\\mathsf{10}\\right]$ after $\\pmb{0.5}\\hbar$ , (d) nano-SiO $\\mathsf{\\pmb{\\mathscr{2}}}^{\\prime}\\mathsf{P}\\mathsf{V}\\mathsf{A}$ $\\left\\langle\\mathsf{p}\\mathsf{H}=1\\mathsf{0}\\right\\rangle$ ) after 168 h \n\n \nFig. 8: Freeze tests. Fogging response being removed from 2 $\\mathsf{\\pmb{20}}^{\\circ}\\mathsf{\\pmb{C}}$ freezer to humid laboratory environment. (a) PE film uncoated, (b) PE film with $(\\mathsf{N2010-P V A})_{0.8}$ coating",
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"category": " Results and discussion"
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},
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{
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"id": 12,
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"chunk": "# The mechanical properties \n\nFor the purpose of actual application, the mechanical properties (water-resisting and wear-resisting property) of $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ hydrophilic coating must be considered. It was preliminarily assessed by the impact of a water scour. In this study, the water flowed out for $12\\mathrm{~h~}$ on $(\\mathrm{N}2010–\\mathrm{PV}\\mathrm{A})_{0.8}$ coating surface. When water drop was in contact with the hydrophilic coating, it immediately spread out on the surface (Supporting Information 3). These water scour tests were repeated three times. After the water flushing test of the coating, the properties of the coating were analyzed (Fig. 10a). The SEM image showed that nano- $\\mathrm{SiO}_{2}$ was still present on the surface of PE films. The contact angle on the surface of PE film increased from $22.9^{\\circ}$ to $44.2^{\\circ}$ , it still remained hydrophilicity. Subsequently, the thin film was washed for up to 20 cycles using a sponge at a speed of 50 cycles per minute. If the hydrophilic coating was not washed off, it was believed to have good washability and could endure practical washing. After washing, the SEM image of PE thin film became smooth (Fig. 10b), and it also maintained a low water contact angle $(37.8^{\\circ})$ and good antifogging property. Therefore, the current hydrophilic coating showed good mechanical properties. \n\n \nFig. 9: Transmission spectra of PE film with nano- $\\bullet\\mathrm{i}0_{2}/$ PVA hydrophilic coatings. (a) Blank PE film, (b) PVA, (c) $(\\mathsf{N}2010\\mathrm{-}\\mathsf{P}\\mathsf{V}\\mathsf{A})_{0.4}$ , (d) $(\\mathsf{N}2010{\\circ}\\mathsf{P}\\mathsf{V}\\mathsf{A})_{0.8}$ , (e) $(N2010\\ –\\mathsf{P V A})_{2}$ , (f) Ludox N2010, (g) $(\\Im\\Im3010\\mathrm{-}\\mathsf{P V A})_{0.8}$",
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"category": " Results and discussion"
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},
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{
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"id": 13,
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"chunk": "# Conclusions \n\nIn summary, the hydrophilic coating of $\\mathrm{SiO}_{2}/\\mathrm{PV}\\mathrm{A}$ with high light transmittance and durable antifogging properties was prepared by solution blending method with simple and low-cost one-step dipping technique. The influence of different $\\mathrm{SiO}_{2}$ contents and $\\mathrm{\\pH}$ on the hydrophilic coating was discussed. Dynamic laser particle and Fourier transform infrared spectra data showed that the $\\mathrm{SiO}_{2}$ particles interacted with PVA molecular chain by forming a small amount of $_{\\mathrm{Si-O-C}}$ chemical bonds. The chemical structure can improve the strength and water resistance of the hydrophilic coating. SEM and AFM images of PE film containing $(\\mathrm{N}201\\bar{0}{\\cdot}\\mathrm{PV}\\mathrm{A})_{0.8}$ coating showed that $\\mathrm{SiO}_{2}$ nanoparticles were dispersed in PVA with good compatibility, forming a uniform papilla-like structure. The large roughness $(7.6~\\mathrm{nm})$ had a magnifying effect on the hydrophilicity of the coating, which decreased the contact angle from $99.5^{\\circ}\\$ to $22.9^{\\circ}$ . The maximum transmittance of the PE film with SiO2/PVA coatings between 560 and $700~\\mathrm{nm}$ was over $90\\%$ . The antifogging time was more than 1 month under $60^{\\circ}\\mathrm{C}$ by QB/T 4475-2013 standard. The water-resisting and wearresisting property tests showed that the current hydrophilic coating showed good mechanical properties. The current approach was facile, effective, and low cost, and had applications in the fields of eyeglasses, mirrors, face shields, camera lens, greenhouse claddings, and medical instruments. \n\n \nFig. 10: SEM images of PE film (N2010-PVA)0.8 coating (a) after 12-h water scour test, (b) after 20-cycle wear test. Insert shows a water contact angle image and fogging test image on corresponding PE film surface \n\nAcknowledgments This work was supported by the Natural Science Foundation of Shandong Province (Grant Numbers ZR2019MB053; ZR2017MEM001; and R2019MEE018)",
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"category": " Conclusions"
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},
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{
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"id": 14,
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"category": " References"
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