A Review on Superhydrophobic Polymer Nanocoatings: Recent

Feb 12, 2018 - In recent years, the worldwide coating industries and scientific communities have introduced superhydrophobic coatings with exceptional...
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Cite This: Ind. Eng. Chem. Res. 2018, 57, 2727−2745

A Review on Superhydrophobic Polymer Nanocoatings: Recent Development and Applications Sonalee Das, Sudheer Kumar,* Sushanta K. Samal, Smita Mohanty, and Sanjay K. Nayak Laboratory for Advanced Research in Polymeric Materials (LARPM), Central Institute of Plastics Engineering & Technology (CIPET), B/25, CNI Complex, Patia, Bhubaneswar 751024, Odisha, India ABSTRACT: In recent years, the worldwide coating industries and scientific communities have introduced superhydrophobic coatings with exceptional water repellency for marine, automotive, and medical applications. Various research works has been devoted to creating a superhydrophobic surface. This review attempts to highlight the recent development and technical breakthrough on superhydrophobic coatings and its potential application in various fields. Moreover, emphasis has also been on providing insight regarding the recent development in superhydrophobic coatings using nanotechnology focusing both on novel preparation strategies and on investigations of their distinctive properties.

1. INTRODUCTION Recently, increasing attention has been concentrated toward the development of superhydrophobic coatings with unique structure, properties, and extended applications in the field of anti-corrosion,1−4 anti-icing,5−7 anti-fogging,8−10 self-cleaning,11−13 anti-fouling,14−16 and others sectors17−21 as depicted in Figure 1. During 2006 and 2010, the superhydrophobic surface was ranked seventh in the top 20 research fronts in material science by essential science indicators.22

Figure 2. Schematic illustrations of hydrophilic, hydrophobic, and superhydrophobic surfaces.

In recent years, there has been increased interest in fabricating superhydrophobic surfaces of microscale to nanoscale architecture. According to the literature reports, superhydrophobic coatings are present in nature. Various natural materials like lotus leaf, animal species, and their specific parts as depicted in Figure 3 exhibit superhydrophobic properties.25 It has been well established that the use of nanofillers such as nanosilica,26,27 titanium dioxide,28−30 zinc oxide,30,31 etc. can generate superhydrophobic coatings for large-scale industrial applications.32−34 By definition, superhydrophobic nanocoatings contain at least one nanoscale ingredient that plays a pivotal role in the coating properties or the morphology of the superhydrophobic coating at the nanoscale dimension.35

Figure 1. Superhydrophobic coatings market report.23

In general, wetting behavior can be classified into four different regimes on the basis of water contact angle (WCA). WCA in the range of 0° < θ < 10°, 10° < θ < 90°, 90° < θ < 150°, and 150° < θ < 180° can be termed as superhydrophilic, hydrophilic, hydrophobic, and superhydrophobic, respectively, as shown in Figure 2.24 The superhydrophobic coatings have nearly nonwetting results with easy rolling of water droplets from the surfaces. © 2018 American Chemical Society

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November 27, 2017 February 6, 2018 February 12, 2018 February 12, 2018 DOI: 10.1021/acs.iecr.7b04887 Ind. Eng. Chem. Res. 2018, 57, 2727−2745

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remarks and challenges in the field of superhydrophobic nanocoatings that needs to be addressed in the future.

3. DEVELOPMENT OF ARTIFICIAL SUPERHYDROPHOBIC POLYMER NANOCOATINGS This section deals with the recent progress in the field of superhydrophobic polymer nanocoatings using different nanofillers. In addition, this section provides detailed insight regarding the methodologies adapted and the different techniques involved in developing superhydrophobic nanocoatings. 3.1. CNT-Based Superhydrophobic Nanocoatings. Gu et al.41 prepared carbon nanotube (CNT)-based superhydrophobic hybrid membranes with fire-retardant properties by attaching 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PFDTS) onto −OH-functionalized CNTs. The PFDTS/ CNT membranes were found to be superhydrophobic with high separation oil/water efficiency under extreme conditions. De et al.42 designed superhydrophobic multiwalled carbon nanotube (MWCNT) coatings for stainless steel by the chemical vapor deposition (CVD) technique at low temperature (0.3. The coating with an MR ratio 150° and low slide angles, and (3) hydrophilic (hydrophilicity for antifogging and contamination resistance). Superhydrophilic coatings can significantly prevent fogging behavior. It was found that the condensed water droplets immediately spread flat to form a thin water layer on the substrate as compared to the dispersed droplets.90 However, three different approaches have been developed for the case of superhydrophilic surfaces to attain anti-fogging properties. First is the use of titanium dioxide (TiO2)-functionalized-based materials for antifogging properties owing to their photoinduced superhydrophilicity.91,92 The second process involves the utilization of a hydrophilic polymer to obtain superhydrophobic surface and antifogging properties.93,94 The third approach deals with the design of textured or porous surfaces which can improve the surface wettability via manipulation of roughness at various length scales.95 Watanabe et al.96 fabricated TiO2-coated glass with antifogging properties under UV illumination. Thus, a TiO2-functionalized coating can not only be employed in glass, but can also be employed for various other substrates such as polymer, metal, and ceramic materials. Gao et al.97 studied mosquito compound eyes which demonstrated superhydrophobicity and efficient protective mechanisms for sustaining clear vision in humid environments. Artificial mosquito compound eyes inspired by superhydrophobic and antifogging properties were formulated by a soft lithography approach followed by low-surface-energy fluoroalkylsilane modification. 4.4. Self-Cleaning. In the last few decades a large number of synthesis processes have been developed to prepare various self-cleaning coating materials for potential application in daily life for industry, agriculture, and military applications.98−100 At present, several self-cleaning coatings have been commercialized, for example, cement, tile, and glass in the global market. Self-cleaning materials are divided into four parts: (I) TiO2based, (II) bioinspired (lotus effect) superhydrophobic selfcleaning, (III) gecko setae-inspired dry self-cleaning, and (IV) marine organisms inspired anti-fouling self-cleaning such as shark skin and pilot whale skin. Titanium oxide is one of the most utilized functional materials which can be used to prepare self-cleaning coatings due to its unique physical and chemical properties exhibiting both photocatalytic and photoinduced superhydrophilicity.101 These unique characteristic properties are sufficient enough to induce self-cleaning properties. TiO2coated self-cleaning glass has been used in the National Opera Hall102 in China. In 2003, Japan also employed self-cleaning tiles and windows for an eco-life house.103 Cyranoski et al. prepared self-cleaning nanotiles which are both water repellent and oil -repellent.104 4.5. Anti-fouling and Anti-scaling. Anti-fouling coatings for marine application are an especially important topic in the coating fields.105,106 These marine coatings are divided into two main categories: (i) microfouling and (ii) macrofouling. In the case of microfouling, a biofilm is formed, and bacteria starts to stick, while in macrofouling larger organisms start to adhere.107 Anti-fouling coatings for ship hulls protect the exterior surface of the ships exterior as well as reduce the growth of organisms. Ships not using anti-fouling coatings leads to adherence of microorganisms onto the surface resulting in a gradual increase in fuel consumption.108−110 Figure 17 demonstrates a ship hull without an anti-fouling coating resulting in smooth of barnacles and other marine organisms on the exterior surface of the ship.

Figure 17. Anti-fouling castings of a ship hull.

Junaidi et al.47 fabricated rice husk ash (RHA) containing SiO2 anti-fouling superhydrophobic coatings prepared via chemical modification using 1H,1H,2H,2H-perfluorodecyltriethoxysilane (HDFS) and stearic acid. The results demonstrated that the commercial adhesive spray mount and HFDS (3M-HFDS) coating displayed the highest contact angle (CA) value in this work, 63% compared to the virgin 3M coatings. Conversely, 3M and stearic acid (SA)-based coating attained a higher contact angle CA, 50% compared to the virgin spray adhesive coating (3M) sample. In the antifouling test, the coating with HFDS modification could avoid the stain of kaolin slurry with dye. 4.6. Oil−Water Separation. Oil−water mixture separation is one of the most challenging research topics worldwide owing to increasing rates of industrial oily wastewater and oil spill accidents. The environmental concern and economic demands emphasize the requirement of a functionalized membrane to successfully separate oil and water.111−114 There are lots of traditional methods used for oil/water separation such as flotation, centrifugation, and filtration.115−117 However, these are very complicated operations and time-consuming processes.118 Recent years have witnessed momentous attention for fabricating polymer coatings for oil/water separation as shown in Figure 18. At present, porous superhydrophobic and superoleophilic materials containing fabrics, membrane,

Figure 18. Published research articles on oil/water separation materials each year from 2007 to 2016 (based on search result from Web science). 2739

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Figure 19. Surface modification of ormosil/PMHOS.

Recently, Wen et al.128 prepared zeolite-coated mesh films with superhydrophilic and underwater superoleophilic characteristics exhibiting gravity oil/water separation behavior, wherein water can penetrate through the film with oil retention on the film surface. Xiao et al.129 fabricated highly efficient conjugated microporous polymer-coated stainless steel and sponge for separation of oil/water and trace organic contaminants based on superhydrophobic conjugated microporous polymer-coated devices. Conjugated microporous polymers (CMPs) have been explored as a new class of porous materials that can be easily synthesized by common organic reactions such as Suzuki coupling, Sonogashira coupling, and condensation reaction. CMPs, owing to their easily adjusted surface nature, good stability, and large surface area, have gained momentous attention for their physicochemical properties. In the present work, the author reported the preparation of superhydrophobic CMPs based on an iron(III) porphyrin unit coated on stainless steel mesh for oil/water separation. The surface morphology of coated and uncoated CMPs was analyzed using scanning electron microscopy. It was observed that the surface morphology of the uncoated mesh is perfectly smooth and clear. On the other hand, the coated mesh indicated a rough surface with dendritic nanobranches of diameters between 50 and 80 nm indicating successful coating of the stainless steel with CMPs. As a consequence, water does not penetrate through the coating mesh resulting in a higher contact angle of 152°. In addition, the coated mesh floats in water, while the uncoated ones sink. It was also observed that oil can easily pass through coated mesh owing to the oleophobic characteristic of CMPs. The coatings could be easily coated on the framework of sponges to form superhydrophobic devices with rapid and efficient oil/water separation. Cho et al.130 reported the preparation of robust multifunctional superhydrophobic coatings with enhanced water/oil separation, self-cleaning, anti-corrosion, and anti-biological adhesion features. In this study, the authors used a silica ormosil suspension and siloxane polymer to prepare highly transparent and superhydrophobic nanocomposites. To further enhance the superamphiphobic properties, the hybrid nanocomposites were modified with n-alkylsilane (C8, C16), phenylsilane, and fluorosilane. The suspension on account of its good solution processability could be spin-coated on various

sponges, and meshes prepared by various chemical and physical methods have been confirmed to be promising candidates for oil/water separation.119−121 Feng et al.122 fabricated superhydrophobic/superoleophilic functional materials for oil/water mixture separation. On the basis of the lotus leaf structure, Teflon-coated mesh films with superhydrophobic and superoleophilic properties were prepared via a spray dry method for water and oil mixture separation. Based on this approach, industries could efficiently separate oil/water separation, which can be also commercialized for marine ships. Zhang et al.123 prepared nanoporous polydivinylbenzene materials by a solvothermal process exhibiting both superhydrophobicity and superoleophilicity properties. However, the nanoporous materials revealed special selectivity for several organic compounds, as compared to a conventional activated carbon absorbent. Zhang et al.124 also reported polyester textile-based superhydrophobic and superoleophilic materials prepared via chemical vapor deposition. These materials exhibited superwetting and flexibility characteristics with high oil/water separation efficiency and reusability. Recently, many authors focused on developing oil/water separation materials which can exhibit superhydrophobic and oleophilic surfaces. For instance, Varshney et al.125 synthesized novel hydrogel-coated mesh with superhydrophilicity and underwater superoleophobicity for oil/water separation. These unique materials can successfully separate water from oil/water mixtures successfully with controlled recyclability and resistant oil fouling characteristics.126 However, there is a new challenge to develop next generation materials for oil/water separation since with traditional separation technology it is very difficult to separate micrometer-scale oil droplets from water. Thus, scientists are focusing on the incorporation of stimuli-responsive polymeric materials for controlling the oil/water separation which can be a new innovation in near the future. Tu et al.127 synthesized oleophilic conical needle-like structures which can be utilized for the collection of micrometer-sized oil droplets from the water. As a result, the cone-like arrangements structure can capture micrometer-sized oil droplets and convey them toward the bottom of conical needle, with high flow and throughput. 2740

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SA, and outstanding cell feasibility and biocompatibility suitable for preventing microleakage.

substrates. Since, the wetting behavior of the superhydrophobic surface arises from the synergistic effect of low surface energy and rough surface, the authors blended poly(methylhydroxysiloxane) (PMHOS) nanoparticles with a silica ormosil suspension to increase the surface roughness within a nanoscale as depicted in Figure 19. It was observed that the synthesized hybrid nanocomposite film exhibits a superhydrophobic surface with a contact angle of 168° and transparency of 90%. The high transmittance signifies the anti-reflective property of the ormosil film due to its low refractive indices and porous structure. In addition, the smaller particle size and better dispersibility of ormosil/PMHOS leads to reduced scattering resulting in a better anti-reflective property. This anti-reflective property can be utilized for selfcleaning applications and solar cell panels. The observed superhydrophobicity of the ormosil/PMHOS film arises due to its hierarchical surface morphology. It was also found that the superhydrophobic surface of the ormosil/PMHOS composite exhibits good nonsticking properties. This observation was attributed to the low surface energy and hierarchical surface morphology of the ormosil/PMHOS film. The prepared nanocomposites also showed an improved barrier property owing to the cross-linked structure of PMHOS. The hydroxylation and condensation of methyl and hydroxyl groups in siloxane and ormosil results in dense aggregation leading to better barrier properties. Thus, from the above findings, it was concluded that the process of fabricating simple and costeffective F-ormosil/PMHOS composites can be used for barrier, separation, optoelectronics, and other applications. 4.7. Medical. Superhydrophobic polymeric nanocoatings have been employed in the medical field for drug delivery, selfcleaning, and dental applications. Yohe et al.131 developed 3D superhydrophobic poly(ε-caprolactone) electrospun meshes containing poly(glycerol monostearate-co-ε-caprolactone) as a hydrophobic polymer dopant. This superhydrophobic mesh was used in tunable drug release activity through displacement of air to control delivery rate. The entrapped air layer within superhydrophobic meshes demonstrated long-term stability in the existence of serum, showing efficacy against cancer cells in vitro for >60 days. A high-aspect ratio TiO2 nanotest tube can also be used for self-cleaning purposes with high-sensitive immunoassays via immobilizing antibodies for diagnosis of a target antigen reported by Song et al.132 A TiO2-based immune sensor exhibits reusable and self-cleaning properties arising from the photocatalytic character of TiO2. TiO2 demonstrates an antibacterial effect owing to its unique photocatalysis and self-cleaning properties.133,134 The photocatalytic property was enhanced owing to the incorporation of sulfur into TiO2. In contrast with commercial products, the sulfur-doped TiO2 demonstrated higher photocatalysis and photoinduced superhydrophilicity. These films were found to be useful mediators for killing the bacterium Escherichia coli employing light sources generally found in UK hospitals. Similarly, Wang et al.135 also fabricated antibacterial Escherichia coli materials with photoinduced self-cleaning properties using 2,6-anthraquinone sulfonate via a layer by layer process. The superhydrophobic surface demonstrated self-cleaning properties that can reduce bacterial adhesion and also be used into coat gloves, fabrics, and general equipment. Cao et al.13 developed superhydrophobic coatings through a simple photo-cross-linked method which can be used for dental composite restoration as shown in Figure 20 a, b, and c. Superhydrophobic coatings exhibited a high contact angle, low

Figure 20. (a) Illustration of the microleakage appraisal specimen. (b) Structure of artificial restoring cavity with superhydrophobic coating. (c) Cassie−Baxter model of superhydrophobicity and superhydrophobic coating.13

4.8. Others. Superhydrophobic surfaces can also be used in other important applications, for example, automotive, marine, shielding, microfluid, sensor, and solar cells. A superhydrophobic surface exhibiting low adhesion is suitable for dropletbased microfluidic systems owing to the high mobility of liquids on such a surface. Further, Mumm et al.136 fabricated copperbased superhydrophobic surfaces which can be used in wireguided droplet microfluidic systems. Park et al.137 developed an ordered microshell array on flexible and transparent polydimethylsiloxane elastomer surfaces for solar cell applications. Golovin et al.33 designed new parameters to develop mechanical durable superhydrophobic surfaces by spray coating in the presence of different binders and fillers. Further, selfhealing SHSs were fabricated from fluorinated polyurethane elastomer and 1H,1H,2H,2H-heptadecafluorodecyl polyhedral oligomer silsequioxane (F-POSS).138

5. CONCLUSION In this review, we have given detailed insight regarding the recent progress in the synthesis of different superhydrophobic nanocoatings using various nanofillers and fabrication techniques. On the basis of the above literature findings, it is noticeable that the inclusion of nanofillers improves the superhydrophobicity of the polymer coatings. In addition, the diverse applications of the superhydrophobic polymer nanocoatings have also been discussed in brief. Investigated ZnObased polymer nanocoatings can be exclusively used for oil/ water separation and transportation application. On the other 2741

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(9) Howarter, J. A.; Youngblood, J. P. Self-cleaning and anti-fog surfaces via stimuli-responsive polymer brushes. Adv. Mater. 2007, 19, 3838−3843. (10) Gan, W. Y.; Lam, S. W.; Chiang, K.; Amal, R.; Zhao, H.; Brungs, M. P. Novel TiO2 thin film with non-uv activated superwetting and antifogging behaviours. J. Mater. Chem. 2007, 17, 952−954. (11) Latthe, S. S.; Terashima, C.; Nakata, K.; Sakai, M.; Fujishima, A. Development of sol−gel processed semi-transparent and self-cleaning superhydrophobic coatings. J. Mater. Chem. A 2014, 2, 5548−5553. (12) Nakajima, A.; Hashimoto, K.; Watanabe, T.; Takai, K.; Yamauchi, G.; Fujishima, A. Transparent superhydrophobic thin films with self-cleaning properties. Langmuir 2000, 16, 7044−7047. (13) Ganesh, V. A.; Raut, H. K.; Nair, A. S.; Ramakrishna, S. A review on self-cleaning coatings. J. Mater. Chem. 2011, 21, 16304−16322. (14) Banerjee, I.; Pangule, R. C.; Kane, R. S. Antifouling coatings: recent developments in the design of surfaces that prevent fouling by proteins, bacteria, and marine organisms. Adv. Mater. 2011, 23, 690− 718. (15) Chambers, L. D.; Stokes, K. R.; Walsh, F. C.; Wood, R. J. Modern approaches to marine antifouling coatings. Surf. Coat. Technol. 2006, 201, 3642−3652. (16) Hellio, C.; Yebra, D., Eds.; Advances in Marine Antifouling Coatings and Technologies; Woodheads Publishing Elsevier, 2009; pp 577−622. (17) Xue, Z.; Cao, Y.; Liu, N.; Feng, L.; Jiang, L. Special wettable materials for oil/water separation. J. Mater. Chem. A 2014, 2, 2445− 2460. (18) Zheng, Y.; Bai, H.; Huang, Z.; Tian, X.; Nie, F. Q.; Zhao, Y.; Jiang, L.; Zhai, J. Directional water collection on wetted spider silk. Nature 2010, 463, 640−643. (19) Ball, P. Engineering shark skin and other solutions. Nature 1999, 400, 507−509. (20) Li, Y.; Zhang, Z.; Wang, M.; Men, X.; Xue, Q. Environmentally safe, substrate-independent and repairable nanoporous coatings: largescale preparation, high transparency and antifouling properties. J. Mater. Chem. A 2017, 5, 20277−20288. (21) Zhang, S.; Yang, Y.; Gao, B.; Li, Y. C.; Liu, Z. Superhydrophobic controlled-release fertilizers coated with bio-based polymers with organosilicon and nano-silica modifications. J. Mater. Chem. A 2017, 5, 19943−19953. (22) Adams, J.; Pendlebury, D. Global Research Report: Materials Science and Technology; Thomson Reuters Science Watch, 2011. (23) Hydrophobic Coating Market Size & Forecast by Property (Anti-Microbial, Anti-Icing/Wetting, Anti-Fouling, Anti-Corrosion, Self-Cleaning), by Application (Aerospace, Automotive, Construction, Medical, Optical), by Region and Trend Analysis from 2014 To 2025, 2016. Grand View Research. http://www.grandviewresearch.com/ industry-analysis/hydrophobic-coating-market (accessed February 2018). (24) Marmur, A. Hydro-hygro-oleo-omni-phobic terminology of wettability classification. Soft Matter 2012, 8, 6867−6870. (25) Gao, X.; Jiang, L. Biophysics: water-repellent legs of water striders. Nature 2004, 432, 36−36. (26) Shang, H. M.; Wang, Y.; Limmer, S. J.; Chou, T. P.; Takahashi, K.; Cao, G. Z. Optically transparent superhydrophobic silica-based films. Thin Solid Films 2005, 472, 37−43. (27) Bravo, J.; Zhai, L.; Wu, Z.; Cohen, R. E.; Rubner, M. F. Transparent superhydrophobic films based on silica nanoparticles. Langmuir 2007, 23, 7293−7298. (28) Lai, Y.; Tang, Y.; Gong, J.; Gong, D.; Chi, L.; Lin, C.; Chen, Z. Transparent superhydrophobic/superhydrophilic TiO2-based coatings for self-cleaning and anti-fogging. J. Mater. Chem. 2012, 22, 7420− 7426. (29) Zhang, X.; Jin, M.; Liu, Z.; Nishimoto, S.; Saito, H.; Murakami, T.; Fujishima, A. Preparation and photocatalytic wettability conversion of TiO2-based superhydrophobic surfaces. Langmuir 2006, 22, 9477− 9479.

hand, clay-based polymer nanocoatings exhibited superior antiwetting properties with good self-cleaning ability. Both CNT and silica-based polymer exhibited superior chemical resistance properties in both acidic and alkaline solutions. Moreover, the different fabrication techniques involved in developing the superhydrophobic polymer nanocoatings would enable researchers to understand the mechanism and the practical concepts for attaining better properties in the future. Although remarkable advancements have been carried out in the past two decades in superhydrophobic polymer nanocoatings, a number of challenges still need addressed for large-scale industrial application. The current era demands the fabrication of green, ecofriendly, superhydrophobic polymer nanocoatings with low volatile organic emission (VOCs), longer shelf life, and good adhesion strength. The technologies involved in designing and fabricating superhydrophobic polymer nanocoatings should be cheaper to be more productive on a large scale. In addition, a new theoretical model also needs to be developed apart from Cassie and Wenzel to gain deep insight regarding the mechanism of superhydrophobicity.39,40 Thus, it can be claimed that with ever increasing interest and scientific focus in this area much development could be attained to lead to large-scale production and industrial commercialization.

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AUTHOR INFORMATION

Corresponding Author

*E-mail: [email protected]. Fax: +91-6742743863. Tel: +91-674-2742852. ORCID

Sudheer Kumar: 0000-0002-8944-0728 Notes

The authors declare no competing financial interest.

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ACKNOWLEDGMENTS The authors are thankful to the Department of Chemicals and Petrochemicals, Government of India, for the financial support of this research work.

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