[
    {
        "id": 1,
        "chunk": "# High and long-lasting antifogging performance of silane based hydrophilic polymer coating  \n\nQian Liu , Jianbing Cui , Tatsuo Kaneko , Weifu Dong , Mingqing Chen , Jing Luo , Dongjian Shi  \n\nThe Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, Jiangsu 214122, China",
        "category": " Abstract"
    },
    {
        "id": 2,
        "chunk": "# A R T I C L E I N F O",
        "category": " Abstract"
    },
    {
        "id": 3,
        "chunk": "# A B S T R A C T  \n\nKeywords: Interfacial interaction Strong adhesion Continuous antifogging Composite coating  \n\nThe inevitable presence of fog causes a loss of light transmission in optical materials and leads to many unacceptable and serious consequences. A promising strategy for avoiding fog is to modulate the wettability of the material surface and further change the formed way of droplets. Although many works achieved high antifogging coatings, they are lack of the long-lasting antifogging at varied conditions. In this work, a high adhesion strength and persistent antifogging capability hydrophilic coating is obtained by utilizing silane coupling agents containing double bonds such as triethoxyvinylsilane (A151) and 3-(trimethoxysilyl)propyl methacrylate (KH570) with 2-acrylamido-2-methylpropanesulfonic acid (AMPS) and then compositing with poly(vinyl alcohol) (PVA). The coating composed of A151 has a relatively uniform and flat surface structure, due to weaker hydrolysis ability of A151 promoted the smooth condensation speed, compared to KH570. Thanks to the hydrophilic and hydrophobic balance properties of the A151-modulated coating network, the resultant coating exhibits good antifogging performance in the range of $0~^{\\circ}\\mathbf{C}$ to $90\\ {^\\circ}\\mathrm{C},$ , which keeps a light transmission of about $85~\\%$ . Surprisingly, the coating shows excellent adhesion $(350{-}700\\mathrm{kPa})$ to the substrate, which is significantly better than other conventional hydrophilic antifogging coatings, and the hydrophilic and hydrophobic modulation capability and the enhanced interfacial adhesion of A151 segments provide the basis of the coating for long-lasting antifogging, which would open up a new way of durable hydrophilic antifogging coatings.",
        "category": " Abstract"
    },
    {
        "id": 4,
        "chunk": "# 1. Introduction  \n\nOptical materials are wide used in a large number of visualization areas, including endoscopy [1,2], spectacle lenses [3–5], house decoration materials [6–8], windscreens [9], etc., to provide aesthetics, good observability and protection. Thus, the optical materials are required to have good optical performance in a variety of environments and operations. However, the changes in environmental parameters [10–12], or fluctuation in the temperature of the optical material [13,14], can lead to fogging on their surfaces, causing liquid droplets to block transmission of vision and reduce light transmission. The presence of fog may affect the professional judgement of doctors [15,16], shorten the visibility of eyeglasses as well as windscreens [17–19], hinder photosynthesis in plants [20], reduce the efficiency of photovoltaic conversion [21], and affect the visual evaluation and acceptance of food [22,23]. Therefore, it is an urgent necessity for development of effective antifogging strategies.  \n\nAntifogging coatings are considered to be the most promising approach to prevent fogging and significantly improve the light transmission of a substrate by eliminating visible light scattering. As a result, many researches have been devoted to creating transparent and antifogging surfaces. The main antifogging methods can be divided into active and passive antifogging. In active antifogging, the condensation of water droplets on the surface can be inhibited or even prevented by adjusting environmental parameters such as temperature, relative humidity, or air flow rate by additional wires or sensors [24–27]. In contrast, the passive antifogging utilizes surface-wetting properties, especially superhydrophobicity or superhydrophilicity, which are directly regulated by the material structures. The antifogging of the superhydrophobic surfaces is achieved by the extremely low surface energy leading to low friction coefficients between water droplets and the material surface as well as facilitating droplet migration [28]. On the other hand, hydrophilic surfaces allow droplets to diffuse rapidly into a continuous film [29,30], allowing incident light to transmit without being scattered and maintaining clarity, thereby preventing the formation of surface fog and inhibiting droplet growth to the critical size [31,32]. This process effectively avoids the pseudo-fog period, achieving efficient antifogging. Currently, some researches have used $\\mathbf{O}_{2}$ plasma etching to form nano-rough structure on the surface [33], by employed hydrophilic polymers (PEG) as hydrophilic active sites [34], or added surfactants (such as Polysorbate, Span 20 or Span 80) to achieve the purpose of antifogging [35]. Some researchers have also used the amphoteric monomer sulfobetaine to enhance the hydrophilicity, which is more conducive to the antifogging [36], or use the hydrophilic and hydrophobic components of the modulation to obtain antifogging coatings with good water resistance [37]. However, most researches on the hydrophilic antifogging coatings generally focus on the structure fabrication and the surface properties of coatings, which are obtained via the forces between the coating and the substrate including hydrogen bonding, metal coordination, and $\\pi{-}\\pi$ conjugation [38]. These weak interactions resulted in poor adhesion and instability of the coating. Therefore, considering the important influence of the capability of interfacial interactions on antifogging coatings, the utilization of stable covalent bonds to achieve strong interactions between the coating and the substrate is of great research significance.  \n\nHerein, we fabricated long-term antifogging coatings on transparent silicate glass substrates by copolymerization of triethoxyvinylsilane (A151) and 2-acrylamido-2-methylpropanesulfonic acid (AMPS) and complexation of poly(vinyl alcohol) (PVA) to form a hydrophilic/hydrophobic polymer network (denoted as PVA/P(A151-co-AMPS)). Specifically, the introduction of hydrophobic A151 not only inhibits the excessive swelling of the hydrophilic network, but also forms stable covalent interactions with the substrate and enhance the adhesion ability of the coating with hydrolysis of A151. The coating provides strong interfacial interaction $(350\\mathrm{-}700~\\mathrm{kPa})$ while effectively avoiding fog formation, and maintains high fogging transmittance $(>85\\ \\ \\%)$ within a long period over a wide range of temperatures $(0{-}90^{\\circ}\\mathbf{C})$ , with adhesion and antifogging capabilities significantly superior to those of similar products. The obtained PVA/P(A151-co-AMPS) coating paves the way for further commercial applications.",
        "category": " Introduction"
    },
    {
        "id": 5,
        "chunk": "# 2. Experimental section",
        "category": " Materials and methods"
    },
    {
        "id": 6,
        "chunk": "# 2.1. Materials  \n\nPoly (vinyl alcohol) (PVA-1799, $98\\mathrm{-}99\\mathrm{~\\}\\%$ , triethoxyvinylsilane (A151, $97~\\%]$ , 3-methacryloxypropyltrimethoxysilane (KH570, $97~\\%)$ , and initiator ammonium persulfate (APS, $98.5~\\%$ ) were purchased from Macklin. 2-Acrylamide-2-methylpropane sulfonic acid (AMPS, $98\\ \\%$ was obtained from Aladdin. All the materials and reagents were used without further purification. Glass $2.0\\ \\mathrm{mm})$ ) was purchased from Sinopharm Chemical Reagent Co., Ltd.",
        "category": " Materials and methods"
    },
    {
        "id": 7,
        "chunk": "# 2.2. Preparation of antifogging coating  \n\nAntifogging coating was prepared by thermal polymerization. Typically, PVA $(10~\\mathrm{wt\\%})$ aqueous solution was prepared by dissolved $1.0{\\mathrm{g}}$ PVA in $10{\\mathrm{g}}$ distilled water and stirred for $^{2\\mathrm{h}}$ at $95^{\\circ}\\mathrm{C}$ . $5\\mathrm{wt\\%}$ AMPS was added the above PVA solution at $60\\ {}^{\\circ}{\\bf C},$ and silane coupling agent (A151, $2\\mathrm{wt\\%}$ and the initiator APS were added sequentially after AMPS dissolved, and the reaction was continued for $^{2\\mathrm{~h~}}$ at $60~^{\\circ}\\mathrm{C}$ . Finally, the polymer solution obtained was spread uniformly on the glass surface using drip coating to obtain a coating film. The layer was further dried at $50^{\\circ}\\mathrm{C}$ for $^{2\\mathrm{h}}$ to obtain a dried polymer layer (abbr. as PVA/P $\\mathtt{\\backslash A151_{n}}\\cdot$ coAMPS)), in which n was the amount of A151. The preparation of PVA/P $\\mathrm{(KH570_{n}}$ -co-AMPS) layer was same with that of PVA/ $\\mathrm{P(A151_{n^{-}}c o^{-}}$ AMPS), just by substituted A151 as KH570.",
        "category": " Materials and methods"
    },
    {
        "id": 8,
        "chunk": "# 2.3. Measurement of antifogging performance  \n\nThe antifogging property of the sample was detected by hot steam and cold-fog conditions. Specifically, for the hot steam test, the samples were placed above a water bath at a constant temperature $(90~^{\\circ}\\mathrm{C})$ for 1 min with a distance of $1\\mathrm{cm}$ between the sample and the water surface, and then moved under ambient conditions to take a photo immediately. In order to investigate the antifogging properties of the samples, the light transmittance in the wavelength range of $400{\\scriptstyle-700}\\ \\mathrm{nm}$ was collected using a UV–Vis spectrophotometer (Shimadzu Corporation, UV-3600 PLUS). To make a comprehensive evaluation and direct comparison, we also used a test of antifogging resistance under hot steam at different temperatures $(90~^{\\circ}\\mathrm{C},70~^{\\circ}\\mathrm{C},50~^{\\circ}\\mathrm{C},30~^{\\circ}\\mathrm{C})$ and under cold condition $(0\\ ^{\\circ}\\mathbf{C})$ . In addition, a test of antifogging resistance time was also carried out (1 min, 3 min, 5 min, 7 min, $10\\mathrm{min}$ , $20\\mathrm{min}$ , $30\\mathrm{min}\\dot{}$ ).",
        "category": " Materials and methods"
    },
    {
        "id": 9,
        "chunk": "# 2.4. Wettability test  \n\nThe wettability of the sample was characterized by water contact angle (WCA) at a WCA measuring instrument (OCA15EC, Germany). The WCA was monitored on the samples with $3\\upmu\\mathrm{L}$ of droplets, and the time-related contact angle was collected every $1~\\mathrm{min}$ over a $10\\ \\mathrm{min}$ period.",
        "category": " Materials and methods"
    },
    {
        "id": 10,
        "chunk": "# 2.5. Lap shear adhesion test  \n\nThe adhesive strength of PVA/P(A151-co-AMPS) or PVA/P(KH570- co-AMPS) on glass was investigated by shear lap test according to GB/ T 7124-2008. PVA/P(A151-co-AMPS) and PVA/P(KH570-co-AMPS)) were directly coated on the glass, with an area of $1000\\ \\mathrm{mm}^{2}$ . The adherends were pressed together at $50^{\\circ}\\mathrm{C}$ for $^{2\\mathrm{h}}$ before testing. The lap shear adhesion test was carried out on a testing machine with a pressuremeasuring element of $5~\\mathrm{kN}$ and pulled apart at a speed of $5\\ \\mathrm{mm/min}$ until failure. The adhesion strength was calculated by dividing the force at breakage by the overlap area.",
        "category": " Materials and methods"
    },
    {
        "id": 11,
        "chunk": "# 2.6. Abrasion resistance, ageing resistance and water resistance test  \n\nThe abrasion resistance of PVA/P(A151-co-AMPS) was measured by pushing and pulling a coated glass continuously up and down in quartz sand with a diameter of $500~{\\upmu\\mathrm{m}}$ . The ageing resistance test was performed by exposing the coated glass to UV light at $365~\\mathrm{{nm}}$ . For water resistance, the coated glass was immersed in deionized water and then tested for anti-fog after drying. In order to assess the adhesion of the coating to the substrate, the coating immersed in deionized water was dried and then subjected to a tape peel test, where the tape was applied to the coating and then peeled off by rolling it with a $_{100~g}$ weight, and the anti-fogging properties of the coating were immediately tested. The antifogging properties of the coatings were tested after each test by placing the coated glass $1\\mathrm{cm}$ above hot water at $50^{\\circ}\\mathrm{C}$ for $10\\mathrm{min}$ .",
        "category": " Materials and methods"
    },
    {
        "id": 12,
        "chunk": "# 2.7. Characterization  \n\nThe chemical structures of the coating were characterized by the Attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR, Nicolet iS50). ATR-FTIR spectra were collected in the wavenumber range of $4000{-}400\\mathrm{cm}^{-1}$ on an instrument assisted by ATR attachments. The surface morphology of the sample was observed by optical microscopy (VHX-1000C, Hong Kong). Elemental analysis was acquired from the energy dispersive spectroscopy (EDS) device attached to the SEM (S-4800, Japan). An atomic force microscope (AFM, MuLtimode 8) was employed to exam the surface roughness of the samples. The Parallel steel plates with a diameter of $20~\\mathrm{mm}$ was selected for rheological property tests.",
        "category": " Materials and methods"
    },
    {
        "id": 13,
        "chunk": "# 3. Result and discussion",
        "category": " Results and discussion"
    },
    {
        "id": 14,
        "chunk": "# 3.1. Characterization of antifogging coatings  \n\nAs illustrated in Fig. 1, the antifogging coating was formed by casting the polymer solution on the substrate by the drip coating method and further curing at $50~^{\\circ}\\mathrm{C}_{:}$ , the thickness of the coating obtained was approximately $30~{\\upmu\\mathrm{m}}$ (Fig. S1a). During the curing process, a classical dehydration condensation reaction occurred among silane coupling agents and between silane coupling agents and glass, resulting in forming stable covalent bonds for enhancing the interfacial interaction between the coating and the substrate.  \n\n![](images/80a8492b31698799e03fb1757e090e0343fa781131095d7918b35f86745a69dc.jpg)  \nFig. 1. (a) Schematic preparation of the PVA/P(A151-co-AMPS) coating, and (b) the synthesis mechanism of P(A151-co-AMPS) coating.  \n\nChemical structures of PVA/P(A151-co-AMPS) and PVA/P(KH570- co-AMPS) were investigated by FTIR. As shown in Fig. 2a, the peaks at $1095~\\mathrm{cm}^{-1}$ and $3404~\\mathrm{cm}^{-1}$ corresponded to the stretching vibrations of $\\mathtt{C-O}$ and -OH on PVA. The absorption peaks at $1722~\\mathrm{{cm}^{-1}}$ , 1550 $\\mathsf{c m}^{-1}$ , and $1032\\mathrm{cm}^{-1}$ corresponded to the stretching vibrations of $\\scriptstyle\\mathtt{C=}0$ , ${\\tt N}\\mathrm{-H}$ , and S–O on AMPS. And the peak at $1093~\\mathrm{{cm}^{-1}}$ was the absorption peak of $s\\mathrm{i}{-}0$ in A151 and KH570, the appearance of these absorption peaks indicated the successful preparation of the coatings. As shown in Fig. 2b, the viscosity of the PVA/P(A151-co-AMPS) solution increased compared with the PVA/A151/AMPS solution, indicating the formation of P(A151-co-AMPS) network. The surface morphology of the PVA/P(A151-co-AMPS) coating was slightly different compared to the glass (Fig. S1b, c), and AFM show that the coating was differentiated from pure glass as far as roughness was concerned (Fig. 2e, f), and the morphology observation indicated the successful preparation of the coatings on the glass surface. EDS elemental mapping revealed that the polymer was uniformly coated on the surface of the glass (Fig. 2c, d), with the content of N, Si, and S elements of the coating being $71.0\\%$ , 2.2 $\\%$ , and $26.8~\\%$ , respectively (Fig. S2). Compared with PVA/P(A151-coAMPS), the surface morphology of PVA/P(KH570-co-AMPS) was rougher (Fig. S3a), and a small amount of KH570 agglomerated to form polymer particles in the Si elemental mapping (Fig. S3b). Since the hydrolysis of alkoxy group in KH570 was stronger than that of in A151, KH570 was more easily to polycondensation, and thus affected the surface morphology of the coating.  \n\n![](images/fef0e8579f372830b1a22622302ac8bbf98d0e0abbd6343bd8dc9b520de2b07b.jpg)  \nFig. 2. (a) FTIR spectra of PVA/P(A151-co-AMPS), A151, PVA/P(KH570-co-AMPS) and KH570. (b) Rheological characterization of PVA/P(A151-co-AMPS) and PVA/A151/AMPS solutions. Mapping images of (c) Si and (d) S elements. The AFM photo of (e) pure glass and (f) PVA/P(A151-co-AMPS) coating.",
        "category": " Results and discussion"
    },
    {
        "id": 15,
        "chunk": "# 3.2. Antifogging property  \n\nThe antifogging properties was tested by hot steam. The coated glass and bare glass were exposed to hot water vapor ${\\bf\\langle-90^{\\circ}C}$ 1 cm above) for 60 s. The antifogging test photographs were taken immediately after the samples were moved over the letter paper, and the antifogging performance was evaluated by the average transmittance at $400{\\-}700\\ \\mathrm{nm}$ . The effect of PVA amounts on the antifogging coating was first investigated, as shown in Fig. S4a, 2b. The coatings with $5\\ \\mathrm{wt\\%}$ PVA affected the overall performance of the antifogging coating, although it had better light transmission, the coatings had almost lost the antifogging ability (Fig. S4b), and thus $5\\ \\mathrm{wt\\%}$ PVA was not desirable for the antifogging coating. Then, the antifogging properties of the coatings with $10~\\mathrm{wt\\%}$ PVA was detected in detail.  \n\nTo understand more intuitively the effect of the silane coupling agents on the properties of the coatings, light transmission of the coatings with different amounts of A151 and their optical photo images of antifogging properties (same color as the curve of light transmittance) were investigated and shown in Fig. 3. The glasses without and with various coatings were transparent and the letters underneath were clearly visible (Fig. 3a), and the best light transmission was achieved 80 $\\%$ for the coating with $2\\mathrm{wt\\%}$ of A151 before atomization. To investigate the antifogging performance of the coatings, the transmittance and photo images were taken after the samples were placed above hot water at $90^{\\circ}\\mathrm{C}$ for $1\\mathrm{min}$ (Fig. 3b). Without the protection of the antifogging coating, water vapor formed small droplets on the bare glass, causing refraction and reflection of light, leading to a significant reduction in transmittance. For the glass with coatings, only the coating with $2\\mathrm{wt\\%}$ of A151 had no fog layer and the light transmission was ${\\sim}85~\\%$ , while the coatings with other amounts of A151 $5\\mathrm{wt\\%}$ , $10\\mathrm{\\wt{\\%}}$ ) were visibly fogged. With the low amount of A151, the coating was able to rapidly absorb the surrounding water vapor, which quickly diffused to the surface, increasing the light transmission and achieving antifogging. In the case of a large amount of A151, a large amount of hydrolyzed A151 will self-condensing and exhibit phase separation, reducing the light transmission and the coating loses its antifogging properties. For the coating PVA/P(KH570-co-AMPS), the light transmittance was weaker than that of PVA/P(A151-co-AMPS) (Fig. 3a), even with low amount of KH570, and the PVA/P(KH570-co-AMPS) coating showed lower antifogging (Fig. 3b). The possible reason was that the stronger hydrolysis of KH570 than that of A151, resulting in KH570 chains condensed together and more obvious hydrophobic effect occurred under atomization conditions. The antifogging mechanism of the coating is shown in Fig. 3c. Large number of hydrophilic groups in PVA and AMPS improve the surface energy of the composite coating, so that the fog spread uniformly on the surface to form a hydration layer, leading a high transmittance. However, for the glass without hydrophilic coating or with high hydrophobic coating, the fog condensed on the surface, grew, and finally formed water droplets, leading to obvious refraction and reflection of light, reducing the light transmittance, and therefore showing low antifogging capability.",
        "category": " Results and discussion"
    },
    {
        "id": 16,
        "chunk": "# 3.3. Wettability of coatings  \n\nTo further explored the antifogging properties of the PVA/P(A151- co-AMPS) coatings, the wettability of the coating were evaluated. The photographs of the water contact angle as a function of time and the values are shown in Fig. S5 and Fig. 4. As shown in Fig. 4a, the initial WCA of the coated glass surfaces was about $70^{\\circ}-80^{\\circ}$ , twice of that of the pure glass. As the A151 amounts in PVA/P(A151-co-AMPS) increased, the more Si-OH groups were produced by hydrolysis of the silanoxy groups, which reduced the surface energy of the coatings to be more hydrophilic and affected the initial contact angle of PVA/P(A151-coAMPS). In addition, time-dependent WCA measurements were used to further investigate the change in wettability of the coatings (Fig. 4a, b). The WCA values of all the coatings steadily decreased by approximately $35^{\\circ}$ over a 600-s time interval, while the WCA values of the pure glass decreased by approximately $17^{\\circ}$ . The WCA values indicated that the coatings absorbed a portion of the water from the water droplets in addition to the evaporation of water from the surface. Due to its beneficial absorptive capacity, the initially condensed water was immediately absorbed by the coating, leaving a fog-free surface.  \n\n![](images/3a159cc1c38f8785cc04fd2ff0c5f2c6e56d81829a26d5419a8c5be5b9926047.jpg)  \nFig. 3. Light transmittance (a) and atomized transmittance (b) of different coatings. (c) Schematic diagram of coating antifogging mechanism.  \n\n![](images/14193322e02b9decee2d2f6b181f23831190c9ac2bfc1d614f1955736d8b0ea6.jpg)  \nFig. 4. Water contact angles of PVA/P(A151-co-AMPS) with different A151 amounts at $5\\mathrm{\\wt\\%}$ (a) and $10~\\mathrm{wt\\%}$ (b) PVA.",
        "category": " Results and discussion"
    },
    {
        "id": 17,
        "chunk": "# 3.4. The interface strength of the coating  \n\nTo illustrate the superiority of the silane coupling agent in enhancing the adhesion strength between the coating and the glass, a lap shear test was performed as shown in Fig. 5a and the adhesion strength were obtained in Fig. 5b. Compared with PVA and PVA/PAMPS, the $\\mathbf{PVA_{10}/P}$ $(\\mathsf{A}151_{\\mathrm{n}}$ -co-AMPS) increased the interfacial adhesion by approximately 2-fold, which was attributed to the covalent condensation between A151 and the glass. With the increasing of the silane coupling agent content (Fig. 5b), the adhesion strength could increase to $700~\\mathrm{kPa}$ at $10\\ \\mathrm{wt\\%}$ A151 addition. When the silane coupling agent was KH570, the adhesion of the coating to the glass was slightly higher than that of A151 (Fig. S6, S7), probably due to the higher hydrolysis rate of KH570 increased the adhesion between the coating and the glass per unit area, as seen by the EDS elemental mapping (Fig. S3b). The uneven distribution of KH570 and the chains clustered together, which in turn affected the overall surface morphology of the coating (Fig. S3a), and the excessive roughness seriously affected the light transmission and antifogging performance of the coating (Fig. 3).  \n\nThe superiority of A151 for enhancing the adhesion of antifogging coatings was strong interfacial bonds provided by the partial hydrolysis of siloxanes on A151 to form Si-O-Si bonds with the glass, and significantly improved the adhesion strength of the coatings. The adhesive strengths of the coatings on silicate glass were higher than most of commercial glues and higher-performance polymer adhesives in the literatures [39–48], especially, the strength of the $\\mathrm{PVA_{10}}/\\mathrm{P}(\\mathrm{A}151_{10^{-}}\\mathrm{c}_{0^{-}}$ AMPS) coating was highest than that of the previous reports (Fig. 5c).  \n\n![](images/9d7386cbaf2a91a3de1d87f21048eadc8661a96dc9a161fea2cba9ecb2f0f4ef.jpg)  \nFig. 5. (a) Schematic illustration of measurement of adhesive strength based on the lap-shear test. (b) The adhesion strength of PVA/P(A151-co-AMPS) under different A151 additions at $5\\mathrm{\\wt\\%}$ and $10~\\mathrm{wt\\%}$ PVA additions. (c) Comparison of adhesion strengths of the PVA/P(A151-co-AMPS) on the glass substrate to other polymer adhesives reported in the literature. The error bars represent the standard deviation, and sample numbers, $n=3$ .",
        "category": " Results and discussion"
    },
    {
        "id": 18,
        "chunk": "# 3.5. Abrasion resistance, ageing resistance and water resistance  \n\nThe silane coupling agent A151 played two roles in this antifogging coating: exhibiting cross-linking through dehydration condensation and enhancing the adhesion strength. Considering that the practical application of the coating, the coating $\\mathrm{(PVA_{10}/P(A151_{2}}$ -co-AMPS) as an example) was subjected to abrasion tests (Fig. 6a) and ageing tests (Fig. 6b). After prolonged abrasion tests (250 cycles) and 7 days of continuous exposure to a UV source with a wavelength of $365~\\mathrm{{nm}}$ , the coating retained its good light transmission and antifogging properties. After 250 abrasion tests, the surface of the coating showed slight scratches (Fig. S8) and increased roughness (Fig. S9), but the antifogging performance was not affected, and the coating showed robust mechanical strength. The water resistance of the coatings was assessed by performing an antifog test after the samples were immersed in water for different times and dried. As shown in Fig. 6c, even after being immersed in water for $4\\mathrm{h}$ , the light transmission of the coating in the anti-fog test was still higher than ${>}85\\%$ . Due to the condensation of the coating with the glass surface to formed Si-O-Si covalent bonds, the coating was firmly bonded to the glass, resulting in the long-lasting anti-fogging performance. Additionally, the adhesion strength between the coating and the glass after $^\\textrm{\\scriptsize1h}$ of water immersion was further tested by tape peeling to assess the water resistance of the coating. The tape was fully applied to the sample and then rolled back and forth several times with a $_{100\\mathrm{~g~}}$ weight to ensure a tight fit with the coating, and finally, the tape was peeled off at a constant speed. The stability of the coating was further investigated using cycles of peeling the tape (e.g. 0, 10, 20 and 30 times). The results were shown in Fig. 5d. After 30 times of peeling, the antifogging transmittance of the coating remained stable $(85~\\%)$ . In summary, the good durability of the coatings is mainly attributed to the fact that due to the covalent bonding of the coating with the glass and the composite of the coating with PVA.",
        "category": " Results and discussion"
    },
    {
        "id": 19,
        "chunk": "# 3.6. Antifogging durability  \n\nThe temperature resistance employing hot steam and cold fogging were also detected. In Fig. 7a, during the initial antifogging stage (the first $1\\mathrm{min}\\mathrm{.}$ ), a slight disparity was observed in the light transmission rate of the glass coated with antifogging coating under water vapor at different temperatures. This discrepancy was attributed to the direct influence of temperature on the kinetic energy of water molecules, consequently affecting the collision frequency between water molecules and the coating surface within a given time interval. As a result, the temperature influenced the interaction between the coating and water molecules, leading to some variability in the light transmittance of the initial antifogging coating. Nonetheless, the observed light transmittance exceeded $80~\\%$ in all cases. Thus, it was believed that a successful antifogging effect was achieved when the average transmittance of the coating surpassed $80\\%$ .  \n\nThe transmittance at wavelengths of $400{\\-}700\\ \\mathrm{nm}$ at different temperatures is shown in Fig. S10, and the relationship of transmittance and temperature is summarized in Fig. 7b. The transmittance of the PVA/P (A151-co-AMPS) coated glass increased slightly at temperatures equal to or lower than $50^{\\circ}\\mathrm{C}$ with prolonged the water vapor evaporation time. This phenomenon occurred as the water molecules in contact with the coating gradually spread out, compensating for the coating surface defects and avoiding the loss of light reflection and light refraction. At the same time, the coated glass exhibited high time-independent optical transmittance $(\\sim89~\\%)$ under this condition. Conversely, at higher temperatures $70^{\\circ}\\mathrm{C}$ and $90~^{\\circ}\\mathrm{C})$ , the Brownian motion of water molecules was more intense, and the optical transmittance of the coated glass was lower than $80\\%$ at $10\\mathrm{min}$ and $5\\mathrm{min}$ , respectively, which could be attributed to the excessive water accumulation and limitation of water absorption for the coating. Overall, these findings provided valuable insights into the temperature-dependent behavior of antifogging coating and the coating was effective in preventing the formation of fog on the glass over a wide temperature range $(30\\ ^{\\circ}\\mathbf{C}\\ {\\boldsymbol{\\cdot}}90\\ ^{\\circ}\\mathbf{C})$ under hot steam conditions. The reusability of the antifogging coatings with high optical transmittance is a great challenge and is critical for practical applications. The glass with the PVA/P(A151-co-AMPS) coating was tested at $50^{\\circ}\\mathrm{C}$ for $10\\mathrm{min}$ or $20\\mathrm{min}$ over 20 cycles. As shown in Fig. 7c, the light transmission of the coating still exceeded $85\\%$ , which indicated that the coating could withstand at hot steam and repeated use under high light transmission conditions.  \n\n![](images/c7f0dbeadfe10a49a3184c9ec508b220d385fdafd35563a8e60f3cc322d6c384.jpg)  \nFig. 6. (a) Sand abrasion cycles. Inset pictures show the abrasive process and antifogging test before and after abrasion treatment. (b) UV irradiation test at $365\\mathrm{nm}$ of UV light. Inset pictures show antifogging test before and after UV irradiation treatment. (c) Transmittance of $\\mathrm{PVA_{10}}/\\mathrm{P}(\\mathrm{A}151_{2}$ -co-AMPS) in the antifogging test by immersed the coated glass in deionized water for different times and then dried. (d) Transmittances of the coated glass in antifogging tests. Tape peel test of coated glass after $^\\textrm{\\scriptsize1h}$ of deionized water immersion.  \n\n![](images/2add382451593408b13e9795fde087a0d604a49d135b514b13caad5e1c75b275.jpg)  \nFig. 7. Thermal antifogging properties and reusability of PVA/P(A151-co-AMPS) coatings on glass. a) Average transmittance of the coated glass for the first minute at different temperatures. b) Variation of transmittance of coated glass with time under water vapor at different temperatures. c) Average transmittance of coated glass slides for repeated antifogging tests $\\ensuremath{\\mathrm{?0}}\\ensuremath{\\mathrm{min}}$ and $20~\\mathrm{{min}}$ ) at the water temperature of $50~^{\\circ}\\mathrm{C}$ The coating was dried (D) at $50~^{\\circ}\\mathrm{C}$ before and after each test.  \n\nIn addition, the cold antifogging performance of the PVA/P(A151- co-AMPS) coating was evaluated by refrigerating the coated glass slide at $0^{\\circ}\\mathsf{C}$ for 1 h and then exposing it to the ambient environment $(\\sim25^{\\circ}\\mathsf C,$ $55\\mathrm{-}60\\%$ RH). The light transmission of the bare glass was only about 15 $\\%$ (Fig. 8 aI), which seriously affected the visual performance. Whereas the coated glass was unaffected in the cold condition (Fig. 8b) and still maintained the same or even higher light transmission of around $85\\%$ (Fig. 8 aIV). Remarkably, after $7200\\ \\mathrm{min}$ of refrigeration (Fig. 8c), the coated glass was still able to keep its high light transmission of ${\\sim}85~\\%$ .  \n\nAdditionally, the coated glass showed excellent reusability (Fig. 8d) even after being refrigerated for $30\\mathrm{min}$ or $60\\ \\mathrm{min}$ .  \n\nThese results suggested that the coating demonstrated excellent cold antifogging properties under both high temperature and low temperature conditions, making it suitable for a wide range of practical applications.",
        "category": " Results and discussion"
    },
    {
        "id": 20,
        "chunk": "# 4. Conclusions  \n\nIn summary, a hydrophilic antifogging coating with strong interfacial adhesion achieved long-lasting antifogging on the substrate. This coating was prepared based on the copolymerization of the hydrophobic monomer A151 and the hydrophilic monomer AMPS and then composited with PVA, resulting in an antifogging coating. Since the hydrolyzed A151 end-groups can form covalent bonds with the target surface, it showed excellent adhesion ability and avoids interfacial failure. Meanwhile, the polymerized A151 limited to some extent the excessive swelling of the coating under fogging conditions. As a result, PVA/P(A151-co-AMPS) coating maintained high light transmittance $(>85~\\%)$ under the ability of strong adhesion $(350-700~\\mathrm{kPa})$ ) for a long time $(>30\\mathrm{min}$ ) over a wide temperature range $(0{-}90^{\\circ}\\mathrm{C})$ , which had the advantages of strong adhesion ability, long antifogging time, high transparency, and reusability stability. In addition, it provides ideas for the development and design of functional antifogging coatings for the study of interfacial adhesion.  \n\n![](images/4c89b2c41b41d8fbaf4fa606ebfdb14834f05362a4cb5472d3b26fbb44d4d50b.jpg)  \nFig. 8. The cold antifogging performance of the PVA/P(A151-co-AMPS) coating. (a) Light transmittance of pure glass and coated glass before and after refrigeration at $0^{\\circ}\\mathrm{C}$ for $\\begin{array}{r}{1\\mathtt{h},}\\end{array}$ , and corresponding optical photographs (b). (c) The light transmittance of coated glass after different refrigeration times. (d) The light transmittance of the same coated glass before and after refrigeration changes with the number of refrigeration times at $0~^{\\circ}\\mathrm{C}$ .",
        "category": " Conclusions"
    },
    {
        "id": 21,
        "chunk": "# CRediT authorship contribution statement  \n\nQian Liu: Writing – review & editing, Writing – original draft, Methodology, Investigation, Formal analysis, Data curation, Conceptualization. Jianbing Cui: Validation. Tatsuo Kaneko: Supervision, Conceptualization. Weifu Dong: Conceptualization. Mingqing Chen: Validation, Supervision, Funding acquisition, Conceptualization. Jing Luo: Validation, Supervision, Investigation. Dongjian Shi: Writing – review & editing, Validation, Supervision, Methodology, Investigation, Data curation, Conceptualization.",
        "category": " Abstract"
    },
    {
        "id": 22,
        "chunk": "# Declaration of competing interest  \n\nThe authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.",
        "category": " Conclusions"
    },
    {
        "id": 23,
        "chunk": "# Data availability  \n\nData will be made available on request.",
        "category": " References"
    },
    {
        "id": 24,
        "chunk": "# Acknowledgements  \n\nThis work was supported by the National Natural Science Foundation of China (52103165, 22103029), MOE & SAFEA for the 111 Project (B13025).",
        "category": " References"
    },
    {
        "id": 25,
        "chunk": "# Appendix A. Supplementary data  \n\nSupplementary data to this article can be found online at https://doi. org/10.1016/j.porgcoat.2024.108690.",
        "category": " References"
    },
    {
        "id": 26,
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        "category": " References"
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]