key: cord-0695533-xyj8mc8g
authors: A, Jishnu; S Jayan, Jitha; Saritha, Appukuttan; A.S., Sethulekshmi; Venu, Gopika
title: Superhydrophobic graphene-based materials with self-cleaning and anticorrosion performance: An appraisal of neoteric advancement and future perspectives
date: 2020-08-15
journal: Colloids Surf A Physicochem Eng Asp
DOI: 10.1016/j.colsurfa.2020.125395
sha: 6d1277603ac47f5cea60a8c0438fd426a723d36f
doc_id: 695533
cord_uid: xyj8mc8g

Abstract Lotus like materials having superhydrophobicity is attaining greater demand due to the possibility of molding them into different high end applications. The major issue related to self-cleaning superhydrophobic surfaces is their restricted mechanical properties. The development of nanotechnology has brought many advantages in the fabrication and properties of superhydrophobic surfaces and thus it enhanced the demand of superhydrophobic surfaces. Many scientific groups have studied and reported about the superhydrophobicity exhibited by graphene and its analogous derivatives. The fabrication of the devices having properties ranging from anti-sticking and self-cleaning to anti-corrosion and low friction is made possible by the incorporation of this wonderful two-dimensional material. This review focuses on the preparation and properties of graphene based superhydrophobic coating materials with special mention to the wide range of applications rendered by them.

Composite materials with superhydrophobic traits have got extensive consideration owing to their excellent characteristic properties such as self-cleaning, hindered corrosion (1) , and application in water resistant electronic devices (2) (3) (4) . The excellent water repellent properties observed for several natural objects such as lotus leaf, butterfly wings, rice plants etc. motivated scientists towards developing materials having exceptional water repellency (5) . Superhydrophobic surfaces are those facets having a water contact angle of 150 or more (6) and these materials are prepared with sufficient surface abrasion and minimum surface energy (7) . Both industrial and domestic applications are possible with "superhydrophobic surfaces" which made them ranked 7 th in journals of material science discipline between 2006 and 2010 (8) . Superhydrophobic nanocoatings extend the area of nanotechnology and superhydrophobicity into a new dimension which has an essential role in improving the properties of coatings.

The technologies and materials in coating industry are advancing day by day to improvise the efficiency of coatings by the incorporation of cost effective and greener concepts. Undoubtedly, coating is one of the finest methods to alter the solid interface properties by paving a new protecting layer over the substrate via chemical or physical process. So the development of superhydrophobic nanocoatings are attaining more attraction due to its possible extended high end application (9) .

The surface wetting performance can be generally classified into 4 categories hydrophilic, hydrophobic, superhydrophilic and superhydrophobic according to their water contact angle (WCA). Hydrophilic and hydrophobic have their WCA within the range of 10° < θ < 90° and 90° < θ < 150° respectively. Superhydrophilic and superhydrophobic domains are of considerable interest owing to the utmost surface wetting traits having WCA differing in the stretch of 0° < θ < 10°and 150° < θ < 180° respectively. The Superhydrophobic regime is important as it experiences a perfect non wetting capability with an exceptionally elevated water contact angle that result in the rolling of water droplets easily (10) .

The work of Jiang et al. (11) on nanostructure based superhydrophobicity triggered the curiosity of scientific community and it was followed by several works on superhydrophobic nano materials. Wenzel model gives a fair explanation of the contact angle of a substrate which is in contact with a liquid. Cassie and Baxter further proposed a model which deals with J o u r n a l P r e -p r o o f heterogeneous surfaces comprising of two fractions, the former deals with solid liquid and latter with the liquid air interface. The composition of the surface together with its roughness regulate the surface dampening and the water contact angle of the surface (12, 13) . The nano-micro hierarchical roughness plays an eminent role in manipulating the characteristics of superhydrophobic nanocoatings and they are classified as inorganic, organic and inorganicorganic materials (9) .

Silica encompassed materials are the most common choices for superhydrophobic nanocoating area. In fact, they are hydrophilic, but through chemical treatment they obtain superhydrophobicity (14, 15) . Carbonaceous materials such as carbon nanotubes, carbon nanofibers and fullerenes have gained focus in superhydrophobic nanocoatings in the recent years (9) . Inorganic and organic nanomaterials are also utilized as promising materials for enhancing the flexibility and molecular framework of these coatings (16) (17) (18) . Yuan et al. (17) developed superhydrophobic LDPE with lotus-leaf-like characteristics and contact angle in the range of 156°. A vast array of inorganic fillers could be employed for designing hybrid superhydrophobic nanocoatings. Qing et al. (19) developed ZnO/polystyrene nano composite coatings having a WCA of 158°.

Graphene, a younger cohort material, is nothing but the allotrope of carbon isolated by basic mechanical exfoliation in the earliest years of 21 st century (20) . It is a mono-atomic thin sheet of carbon arranged in a hexagonal honeycomb like crystalline lattice and it has attracted worldwide interest within no time because of fascinating properties arising from the two-dimensional structure and existence of sp 2 bonded carbon atoms (21) . Graphene is believed to have a better future for the fabrication of various carbonaceous technical devices, owing to its superior conductivities at room temperature and inertness towards corrosion (20) . Graphene was isolated in 2004 and prior to that intercalated clays and fullerenes were used as coating materials for corrosion resistance (22, 23) .

For the last few years, application of graphene and graphene-related materials are topics of increasing research interests due to many outstanding features which make them suitable for a passive layer formation that protects metals from oxidation and corrosion(24-27). The surface wettability of graphene has been discussed a lot and many efforts have been taken to control the same by modifying the surface of graphene(24). In order to reduce surface energy and increase surface roughness, a lot of methods have been employed by means of layer-by-layer assemblies (28) (29) (30) , spraying (31) , electrospinning (32, 33) , spin coating(34), electrochemical reaction and deposition (35) (36) (37) (38) , chemical vapor deposition(39)etc.

Though application of superhydrophobic nanocoatings is the main destination of all researches, the theory, materials and moulding has also fascinated the research community(9).

Self-cleaning is the most promising property of graphene coated superhydrophobic surfaces as water droplets can roll on the surface and take away the dirt sticking on the surface effectively.

J o u r n a l P r e -p r o o f Numerous artificial superhydrophobic nanocoatings with self-cleaning traits have been synthesized by different methods and are applied in diverse domains based on their applications (40) (41) (42) (43) (44) (45) . Graphene coated nano-composite materials can be effectively used in antiicing and de-icing methods (46) (47) (48) (49) and used in biosensors, biomedical implants and devices, food packaging, industrial and marine equipment (50) (51) (52) .

Graphene is an oil repellent material and hence could be used for effective separation of oil and water (53) . It also imparts anti-corrosion property to a coating system (54) . Diverse varieties of graphene, mainly single layer/bilayer graphene films, graphene oxide (GO), graphene nanoplatelets and graphene nanoribbons can be synthesized by modern techniques (55, 56) . Now a days, nanopellets of graphene are extensively used for the synthesis of composite materials via mixing with metals, ceramics and polymers to tailor the properties for various applications(57).

Graphene coatings are generally synthesized by chemical vapour deposition. Nilsson and his coworkers studied the drawbacks regarding the corrosion inhibition properties of graphene coatings on metal surfaces and concluded that graphene coated by CVD acts as corrosion inhibitor only at low gas pressures (58) . Choi and co-workers(59) synthesized graphene/nafion nanohybrids with hierarchical petal-like, porous structure and superhydrophobicity (WCA=161°) by regulating the structures with respect to the chemical composition. Lee et al. (60) presented another simple route towards the fabrication of superhydrophobic graphene surface via thermal reduction method and they obtained a transparent nano-sphere structure with excellent WCA as shown in Ngyuen and co-workers synthesized graphene-based sponges with enormous absorption capacities (165 times their own weight) there by making them apt for large-scale application(61). The increased surface roughness in nanoscale dimension was responsible for the superhydrophobicity with a CA of 161 0 (75). Table 1 

The superhydrophobicity of a surface is purely dependent on the functionalities present on the surface as well as the morphology and contact angle and hence characterization of the coating is to account the elemental change as shown in Figure 12 . In one of our studies, we have utilized the technique of EDAX to analyze the elements present in the self-assembled nano porous coreshell TiO2-GO hybrid material(86). 

Durability analysis of superhydrophobic surface is very important as it has an immense effect in determining the application. Mechanical durability is one of the crucial components in meeting the real-world application. The fabrication of a durable superhydrophobic material as a coating is an important aspect as it easily gets tampered by mechanical and chemical action (91) . Hierarchical nanostructures were behind this excellent superhydrophobicity (94) . In another study, it was observed that the graphene/polyurethane sponges made by dip coating method were capable of showing enhanced mechanical durability and thermal and chemical stability. The sponges also showed good elastic recovery and the test using lubricating oil confirmed the recyclability as well (95) . Superhydrophobic surfaces made by laser induction process for desalination application were capable of showing enhanced mechanical durability as well as thermal stability. Even after water jet treatment and scotch tape test, the surface maintained the superhydrophobic character. Moreover, the surfaces were capable of retaining the nature even after seven cycles of scotch test ensuring the desalination application. The surface maintained the same pattern even after the removal of the tape, but later the degradation occurred due to the failure of adhesion and it is not associated with the failure in superhydrophobicity (96) . It is observed that the topology of graphene/polypropylene surface is highly efficient to keep the water away and it forms a perfect Cassie-Baxter state. Interestingly, after abrasion, the new surfaces were having increased roughness and maintains the hydrophobicity (97) . In another study, a stretchable, robust and superhydrophobic graphene based thermoplastic polyurethane (TPU) composite with excellent mechanical durability was prepared. Knife scratch and hand rub test were carried out in order to understand the durability. The composites were capable of exhibiting superhydrophobicity even after these harsh tests and water easily rolled off from the surface. Sand paper abrasion test revealed that the surfaces were capable of maintaining the superhydrophobic behavior even after five cycles of 32.5KPa of abrasion. Moreover, at a low load of 20KPa, the surface maintained the behavior even after 450 cycles due to the tensile strength of pristine graphene, physical support of TPU to the partially embedded nanoplatelets of graphene and the elastic nature of TPU (98) . Graphene based superhydrophobic surfaces tend to show excellent mechanical durability than rGO based systems. Hence modification of rGO is usually done to increase the durability. Recently, superhydrophobic hexadecyltrimethoxysilane-grafted rGO based melamine sponges having excellent mechanical and chemical stabilities were made. These materials maintained the mechanical stability even after 40cycles .Due to the interaction between rGO and the grafted material, it shows chemical inertness as well (99) . Nanofibers of thermoplastic polyurethane (TPU) prepared via electrospinning were decorated using graphene for imparting hydrophobicity. Even after 20, 50 and 80% stretching, the fibers retained the superhydrophobicity due to the surface modification using graphene and they also maintained the superhydrophobicity in harsh chemical environment(100).

J o u r n a l P r e -p r o o f

Corrosion generally describes the damage to metal or its alloy by means of chemical or electrochemical interactive reactions that occur on the surface of the metal due to the environmental exposure. This serious problem leading to the loss of metal as scrap is a major economic issue faced throughout the world. Oiling, painting, electroplating etc. are the common methods followed to avoid this damage (101) . (109) . Reproduced with permission from springer.

The presence of organic pollutants in water is a major threat to the ecosystem. Hence oil -water separation is considered as a major solution for environmental problems. Oil water separation is a problem that is gaining momentum in the present scenario. Hence the development of oil water separating materials from superhydrophobic graphene coatings is considered very important. Conventional materials used for this process include zeolites, activated carbon, natural clays, straw, wool fibers etc. These materials exhibit low efficiency in the separation process due to their hydrophilic nature. Hence the fabrication of novel superhydrophobic materials is the need of the hour. Superhydrophobic surfaces that are oleophilic or super oleophilic can be employed to separate oil and water by concentrating oil into a semi solid phase. Tai and co-workers employed sponges for effective oil water separation (61) . GO sponges devoid of any positively charged groups exhibit the capability to adsorb anionic dyes via π-π interactions(110).

Jayaramalu et al. (111) made a biomimetic composite for oil-water separation using highly fluorinated GO and nanocrystalline zeolite imidazole framework ZIF-8 (Figure 18 ). This oil water separation is necessary to avoid the spilled oil in oceans and other water sources. Due to J o u r n a l P r e -p r o o f the self-assembly of the micro-mesoporous structure, the material was able to show a WCA of 162° with an oil CA of 0°. The sponges incorporated with these hybrid materials were able to show high absorption capacity to oils, polar and non-polar solvents. Since these sponges float over water, they can easily extract oil. Oil absorption capacity of the sponge and the hybrids are shown in Figure 19 . 

Moreover the reusability of the fabrics was confirmed by the sorption-mechanical squeezing test.

The absorption capacity was determined by simply immersing the cotton/rGO fabric in inorganic solvents and oil. The soaked fabric absorbed the oil and the absorbed oil was separated by simple squeezing and are suitable for the reuse. It was also suitable for removing oil/solvents about 40-60 times of its weight. Cao et al. (113) made anticorrosive and superhydrophobic coatings using fluorinated polydopamine/chitosan/rGO composite. By following the self-polymerization, polydopamine was anchored onto the surface of rGO. 3D structured chitosan/rGO hybrid hydrogels had oil absorption capacity 12-21 times higher than their weight. Nguyen et al. (61) used the superhydrophobic PDMS/GO sponges for oil water separation. These materials were able to absorb the spilled oil to about 54 to 165 times higher than their weight. But the absorption capacity was found to be reduced after repeated use in the case of oil. Whereas, the sponges were able to retain the absorption capacity to organic solvents even after 5 repeated cycles. Xiao et al. (114) fabricated GO/nanofiber gels for oil-water separation. Higher WCA ensures easy transport of oil into these aerogels. This can be monitored by directly immersing the material into the oil-water medium as shown in Figure 20 and absorption capacity can be evaluated from its weight. Yang et al. (115) synthesized silica incorporated GO by sol-gel process, for separating oil from water. Zhou et al. (116) used graphene/polyurethane based superhydrophobic sponge for oil-water separation. It showed an absorption efficiency of 53000 times higher than its weight due to the superhydrophobic network structure (Figure 21) . Table 2 . 

Anti-bacterial property is very effective for biosensing and biomedical applications, food packaging and for industrial as well as marine equipment manufacturing. Amine functionalized In another study, Shateri-Khalilabad and Yazdanshenas (65) (125) .Even though graphene shows excellent optical absorption, adsorption is not that much efficient, hence the incorporation of plasmonic nanoparticles together with graphene could enhance the adsorption behavior of the mask. Superhydrophobicity together with electrothermal efficiency helps the surface to remain dry and clean in the glaze ice condition (124) . The removal of surface ice can be easily done in graphene due to its highly hierarchical structure and moreover the partially embedded structure shows excellent durability against sand paper abrasion(124). The antibacterial, and mechanical robustness of functionalized and hybrid graphene based superhydrophobic materials can be exploited for making cost effective facial masks and PP kits.

Apart from medical applications, graphene based superhydrophobic materials can also be utilized for anti-icing, sensing, pollution control and self-cleaning applications. Switchable superhydrophobic graphene based surfaces can also be utilized in the development of smart materials. Thus there lies a vast prospect for graphene based superhydrophobic surfaces in the development of value added products in future.

The authors declare that they have no known competing financialinterestsor personal relationships that could have appeared to influence the work reported in this paper.

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