Graphene aerogels are the world’s lightest materials, with an unusual low density
[3633]. The combination of the hydrophobic properties of graphene sheets and low density makes the graphene aerogel a very promising candidate for oil absorption. The absorption capacity of the graphene aerogel approaches a level several hundred times greater than that of commercially available materials for environmental remediation purposes. Nowadays, using three-dimensional graphene aerogel materials for oily wastewater treatment with its complex compositions remains a great challenge owing to volume shrinkage, which results in low adsorption capacity and single-function. Ji et al.
[3734] introduced renewable Enteromorpha into the graphene aerogel using facile hydrothermal-freeze casting treatment, producing the ultralight, compression, and amphiphilic adsorbent for oil spill removal and water pollution cleanup. The results of this study show that, for clean-up of oil spills, the Enteromorpha modified graphene aerogel (EGA) showed superb adsorption capacity towards oil and organic solvents compared with pristine graphene aerogel (GA). Hence, EGA can be successfully used as an adsorbent for oil in oil/water separation processes
[3734]. Chatterjee et al.
[3835] developed a simple preparation method to synthesize aerogels with great shape retention for oil absorption application. To increase the selective oil absorption and hydrophobicity, the authors used a dip coating process to chemically modify the graphene sheets and attach it to the aerogel pore surface. Several examples were demonstrated by the authors to show the feasibility of applying the synthesized aerogel in oil spill control
[3835]. Zhan et al.
[3936] investigated the role of graphene oxide (GO) in increasing the oil absorption capacity by the aerogel materials and in decreasing the shrinkage in polyimide (PI) aerogels. The study includes grafting the GO particles with pyromellitic dianhydride (PMDA) forming GO-modified PMDA prior to reaction with 2,2′-dimethylbenzidine to form polyamic acid. The polyamic acid chains are then cross-linked using 1, 3, 5-tris (4-aminophenyl) benzene and chemically imidized using acetic anhydride and pyridine to obtain polyimide gel. The resultant aerogel specimens, obtained by supercritical drying of the gels, demonstrated great reduction of diameter shrinkage from 9.0% for unmodified monoliths to 0.8% in the presence of 5.2 wt% GO, a 9.1% reduction in surface energy compared with the unmodified aerogel, high surface area (>504 m
2/g), high porosity (>93%), and low bulk density (<0.0905 g/cm
3). These aerogels demonstrate a great increase in the hydrocarbon oil absorption capacity
[3936]. Meng et al.
[4037] synthesized a lignin-based carbon aerogel enhanced by graphene oxide (LCAGO) for the separation of oil from water. The synthesized aerogel by the authors demonstrated superhydrophobicity and good mechanical property, proving that it is capable of being used in oil/water separation. The results of the authors’ study reveal that the aerogel efficiently separated the light oil, heavy oil, and emulsified oil from water. The results of the study indicate that the material is highly effective and very practical as a water-cleaning material. In addition, the preparation process provided by the authors is energy-saving and is an efficient route for the separation and collection of oil from water with industry waste
[4037].
Recently, graphene aerogels have gained great research attention in oil/water separation processes based on their distinguishable properties. However, the over stacking of graphene oxide nanosheets (GO) results in a poor recyclability and low adsorption capacity. Kang, Cui
[4138] fabricated nitrogen-doped magnetic carbon nanospheres/graphene composite aerogels (MCNS/NGA) under weakly alkaline conditions via a one-step hydrothermal in situ electrostatic self-assembling strategy. The aerogels synthesized by the authors had super-elasticity, low density, high specific surface area, and good magnetic properties. Hence, the aerogels exhibited high adsorption capacity in the range of 187 g g
−1 to 537 g g
−1 towards various oils and organic solvents, surpassing most of the reported materials to date. Thus, the MCNS/NGA synthesized in this study are promising candidates in oil/water separation processes
[4138]. Cleaning up of crude-oil spills is considered a major environmental remediation issue and urges the fabrication of sorbents with high and stable hydrophobic and oleophilic properties. Thakkar, Pinna
[4239] synthesized aerogels with durable hydrophobicity via incorporating reduced graphene oxide (rGO) in highly porous silica matrices. The aerogels synthesized by the authors exhibited high oil selectivity and sorption. Hence, the aerogels fabricated in this study can be successfully implemented in oil/water remediation processes
[4239].
Low fluidity and high viscosity heavy crude oils frequently decrease their diffusion rate into the porous adsorbents, leading to a low efficiency in oil spill removal. Hence, the photothermal effect can be used to greatly decrease the viscosity of heavy crude oil via in situ solar light heating. Luo, Wang
[4340] synthesized photothermal carbon nanotube/reduced graphene oxide (CNT/RGO) microspherical aerogels by the fabrication of graphene oxide (GO)-based microspherical aerogels with several radially orientated microchannels, followed by high-temperature reduction of the GO components and growing CNTs inside the microchannels. The results of the study show that, under 1 sun irradiation, the aerogel surface temperature quickly rose to 83 °C in 1 min, causing a rapid decrease in the viscosity of crude oil. Moreover, the optimal microspherical aerogels exhibited an excellent adsorption capacity of heavy crude oil, up to 267 g g
−1 in only 10 min, surpassing several other reported oil adsorbents
[4340]. Three-dimensional (3D) aerogels with lipophilic and hydrophobic properties have gained great attention in efficient oil spill clean-up. However, biodegradability, cost-effectiveness, and recycling are still great challenges in the application of aerogels for oil/water separation. Hu, Zhu
[4441] fabricated high biocompatibility, hydrophobic, and low cost composite aerogels via directional freezing-drying technology with the use of chitosan (CS) as the skeleton substrate, hydrophobic silicon particles/polydimethylsioxane (H-SiO
2/PDMS) as the hydrophobic modifier, and reduced graphene oxide nanosheets (rGO) as enhancements. The composite aerogel synthesized in this study demonstrated high adsorption capacity for oil, as well as good thermal and chemical stability in a harsh environment. In addition, the adsorbed oils and organic solvents can be easily extruded from aerogels owing to its excellent compressive properties
[4441]. Cleaning, collecting, and recycling oil from oil spills, specifically high viscosity crude oil, are of worldwide concern. Sun et al.
[4542] synthesized a 3D macrostructure CuFeSe
2-loaded graphene aerogel (GA-CuFeSe
2) that shows an outstanding photothermal conversion capacity, surpassing various other materials. The synthesized 3D macrostructures supported by graphene holds a versatile pore structure that allows rapid diffusion of highly viscous oils and a high corrosion resistance. The high-performance oil sorption and photothermal conversion, driven by solar power, demonstrated that this material can be efficiently applied for oil spill clean-up
[4542]. Zhang et al.
[23] developed a facile approach for a highly efficient oil/water separation process by incorporating dimethyldiallylammonium chloride acrylamide polymer (P(AM-DMDAAC)) into the graphene aerogels. The functionalized 3D graphene aerogel presented several outstanding physical properties, including low density, large specific surface area, and great hydrophobicity. The modified aerogel in this study demonstrated excellent adsorption capacity for a wide range of oils and organic solvents. The authors have also found a simple approach by changing the pH values to achieve controlled wettability transition of P(AM-DMDAAC)/graphene aerogels (PGAs). The hydrophobic PGA prepared at pH 2.03 demonstrated a superb oil/water separation performance. Thus, as an efficient and recyclable water purification material, the environmentally friendly and sustainable polymer-modified graphene aerogel has promising potential in oil/water separation
[4643].
In a severely damaged marine polluted environment, low-density and environmentally friendly aerogels have become potential materials for oil/water separation. However, several reported aerogels have the disadvantages of low oil absorption, poor flexibility, and compressibility, which hinders their application. Zhou et al.
[4744] reported an anisotropic, compressible lamellar lipophilic and hydrophobic graphene/polyvinyl alcohol/cellulose nanofiber carbon aerogel (a-GPCCA) prepared via carbonization and directional freeze-drying processes. The synthesized synthetic ultralight a-GPCCA had high porosity, reaching 99.61%, and low density (6.17 mg/cm
3). In addition, the directional freeze-drying used by the authors produced a lamellar interpenetrated three-dimensional (3D) porous structure, with a high adsorption capacity, good compressibility, and recyclability. Moreover, carbonization provided it with a high thermal stability and hydrophobic properties, resulting in a high oil/water selectivity and combustion cyclicity. Thus, the a-GPCCA fabricated in this study has promising potential in the field of the offshore oil spill treatment and domestic industrial wastewater
[4744]. Song et al.
[4845] have successfully synthesized a grass-modified graphene aerogel (GGA) using an environmentally friendly, simple, and low-cost hydrothermal treatment. The graphene aerogel properties have been significantly enhanced by introducing the grass powder, leading to a highly efficient selective adsorption process. The results of this study show that the GGA can successfully be used in the oil/water separation of mixed solution via different manipulation methods. In addition, the GGA is capable of removing oils via adsorption, acting as a filter media dealing with oil/water mixtures, and collecting oils continuously using a peristaltic pump or gravity. This study demonstrates that the GGA is a very good and promising candidate in the oil/water separation field and spill oil clean-up for environmental remediation. Moreover, the addition of grass enhances the graphene aerogel’s oil adsorption efficiency, hydrophobicity, and mechanical property, providing a new route for high-value utilization of biomass waste
[4845]. Huang et al.
[3633] synthesized cork-like graphene aerogels via the EDA-ammonia double hydrothermal reduction method. The fabricated porous aerogels demonstrated high hydrophobicity, porosity, and excellent mechanical properties. In addition, the oil adsorption efficiency is significantly greater than that of the conventional adsorbents, with an oil adsorption capacity of 130.10 g/g for pure diesel and continuous treatment capacity of 71.67 g/g for emulsified oil in oily contaminated water. Hence, the continuous aerogel-based water treatment process is proposed in this study for graphene-based aerogels to have promising potential applications in oil spill remediation and water purification
[3633]. Chen, Li
[4946] have facilely modified an ultralight, compressive, and fire-resistant graphene aerogel via renewable lignin biomass with porous and hydrophobic skeletons. The lignin-modified graphene aerogel (LGA) in this study showed a highly efficient absorption of petroleum oils. Hence, LGA is a highly efficient, renewable, and recyclable potential candidate for applications in oil/water separation
[4946].
Low-density aerogels are very effective materials for oil absorption; however, they are limited by their low elasticity and compressibility. Mi et al.
[5047] prepared three-dimensional (3D), highly compressible, anisotropic, elastic, cellulose/graphene aerogels (CGAs) via bidirectional freeze-drying. The authors have grafted long carbon chains using the chemical vapor deposition method, forming modified cellulose/graphene aerogels (MCGA) with an enhanced superhydrophobicity. Thanks to its ultra-light weight and high surface area, MCGA holds an excellent absorption capacity of 80 to 197 times its weight, which surpasses most carbon-based aerogels and hydrophobic cellulose aerogels. Thus, MCGA is a very promising absorbent material for selective oil absorption and recovery
[5047]. In recent years, reduced graphene oxide (rGO) has attracted great attention from researchers around the world owing to its outstanding physicochemical properties and distinguishable surface chemistry. Cao et al.
[5148] developed a facile and environmentally friendly method to fabricate reduced graphene oxide/polydopamine composite aerogel modified by 1
H,1
H,2
H,2
H-perfluorodecanethiol (PFDT) and reinforced by chitosan. The aerogel synthesized by the author demonstrated high oil/water separation behavior, showing that the aerogels are very effective materials for the remediation of water from oil spill accidents
[5148]. Yu et al.
[5249] developed ultralight and nitrogen-doped graphene aerogels (UNGAS) via a hydrothermal method in the presence of graphene, L-arginine, and dopamine (DA). The synthesized UNGAS demonstrated high absorption capacity for several oils owing to low density, large surface area, and N-doping
[5249]. Cheng et al.
[5350] reported the preparation of a new type of ultralight 3D porous and highly hydrophobic graphene aerogel (GA) with melamine formaldehyde (MF) microspheres as a spacer and pore forming agent and graphene oxide as a precursor, followed by freeze-drying, hydrothermal reduction, and calcination process. The resultant calcined MF-GA (cMF-GA) exhibited a fast absorption rate and maximum sorption capacities up to 230 g/g for diesel oil. Thus, cMF-GA is a promising highly efficient and low-cost absorbent in practical applications of large-scale oil removal
[5350].