Abstract
Modified Hummer’s method has been used in this study to synthesize graphene oxide (GO) solution that was utilized for the fabrication of three-dimensional (3D) graphene sponges and their subsequent functionalization through a low-cost and facile vapor-based surface enhancement approach. The functionalized 3D-graphene sponge is an excellent absorbent, which can remove more than 3300 wt.% of crude oil (calculated with respect to the original sorbent mass). The functionalization of the obtained graphene sponges with trichloro (1H,1H,2H,2H-perfluorooctyl)silane enhanced their wettability properties due to the super-hydrophobic nature of the resulting materials characterized by the contact angles in water greater than 150°. Furthermore, their elastic compression modulus (estimated by conducting a series of compression tests) was about 22.3 kPa. The equilibrium modeling of the oil removal process, which was performed by plotting Langmuir, Freundlich, Temkin, and Dubinin–Radushkevich isotherms, confirmed the properties of the fabricated 3D graphene sponges as exceptional absorbents for crude and diesel oil, which could be attributed to the oleophilic nature of graphene. Moreover, the obtained 3D graphene sponges could be regenerated via heat treatment, which was conducted to release the adsorbed species. After five adsorption-desorption cycles, the sorption capacity of the produced 3D graphene sponges towards crude oil reached 95% of the initial value.
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References
Bi H, Xie X, Yin K, Zhou Y, Wan S, He L, Xu F, Banhart F, Sun L, Ruoff RS (2012) Spongy graphene as a highly efficient and recyclable sorbent for oils and organic solvents. Adv Funct Mater 22:4421–4425
Bi H, Huang X, Wu X, Cao X, Tan C, Yin Z, Lu X, Sun L, Zhang H (2014a) Carbon microbelt aerogel prepared by waste paper: an efficient and recyclable sorbent for oils and organic solvents. Small 10:3544–3550
Bi H, Xie X, Yin K, Zhou Y, Wan S, Ruoff RS, Sun L (2014b) Highly enhanced performance of spongy graphene as an oil sorbent. J Mater Chem A 2:1652–1656
Chae SJ, Güneş F, Kim KK, Kim ES, Han GH, Kim SM, Shin HJ, Yoon SM, Choi JY, Park MH (2009) Synthesis of large-area graphene layers on poly-nickel substrate by chemical vapor deposition: wrinkle formation. Adv Mater 21:2328–2333
Chen X (2015) Modeling of experimental adsorption isotherm data. Information 6:14–22
Chen S, Yang R (1994) Theoretical basis for the potential-theory adsorption-isotherms-the Dubinin-Radushkevich and Dubinin-Astakhov equations. Langmuir 10:4244–4249
Chen Z, Ren W, Gao L, Liu B, Pei S, Cheng H-M (2011) Three-dimensional flexible and conductive interconnected graphene networks grown by chemical vapour deposition. Nat Mater 10:424–428
Chen J, Sheng K, Luo P, Li C, Shi G (2012) Graphene hydrogels deposited in nickel foams for high-rate electrochemical capacitors. Adv Mater 24:4569–4573
Chi C, Xu H, Zhang K, Wang Y, Zhang S, Liu X, Liu X, Zhao J, Li Y (2015) 3D hierarchical porous graphene aerogels for highly improved adsorption and recycled capacity. Mater Sci Eng B 194:62–67
Cong H-P, Ren X-C, Wang P, Yu S-H (2012) Macroscopic multifunctional graphene-based hydrogels and aerogels by a metal ion induced self-assembly process. ACS Nano 6:2693–2703
Eriksson M, Lundström I, Ekedahl L-G (1997) A model of the Temkin isotherm behavior for hydrogen adsorption at Pd–SiO 2 interfaces. J Appl Phys 82:3143–3146
Ferrari AC (2007) Raman spectroscopy of graphene and graphite: disorder, electron–phonon coupling, doping and nonadiabatic effects. Solid state communications 143:47–57
Frank I, Tanenbaum DM, van der Zande A, McEuen PL (2007): Mechanical properties of suspended graphene sheets. Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures Processing, Measurement, and Phenomena 25, 2558–2561
Ge B, Men X, Zhu X, Zhang Z (2015) A superhydrophobic monolithic material with tunable wettability for oil and water separation. J Mater Sci 50:2365–2369
Geim AK (2009) Graphene: status and prospects. Science 324:1530–1534
Gómez-Navarro C, Weitz RT, Bittner AM, Scolari M, Mews A, Burghard M, Kern K (2007) Electronic transport properties of individual chemically reduced graphene oxide sheets. Nano Lett 7:3499–3503
Gui X, Zeng Z, Lin Z, Gan Q, Xiang R, Zhu Y, Cao A, Tang Z (2013) Magnetic and highly recyclable macroporous carbon nanotubes for spilled oil sorption and separation. ACS Appl Mater Interfaces 5:5845–5850
Hashim DP, Narayanan NT, Romo-Herrera JM, Cullen DA, Hahm MG, Lezzi P, Suttle JR, Kelkhoff D, Munoz-Sandoval E, Ganguli S (2012) Covalently bonded three-dimensional carbon nanotube solids via boron induced nanojunctions. Sci Rep 2:363
Hayase G, Kanamori K, Fukuchi M, Kaji H, Nakanishi K (2013) Facile synthesis of marshmallow-like macroporous gels usable under harsh conditions for the separation of oil and water. Angew Chem Int Ed 52:1986–1989
Johnson RD, Arnold FH (1995) The Temkin isotherm describes heterogeneous protein adsorption. Biochim Biophys Acta (BBA)-Protein Struct Mol Enzymol 1247:293–297
Lee C, Wei X, Kysar JW, Hone J (2008) Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science 321:385–388
Li X, Magnuson CW, Venugopal A, An J, Suk JW, Han B, Borysiak M, Cai W, Velamakanni A, Zhu Y (2010) Graphene films with large domain size by a two-step chemical vapor deposition process. Nano Lett 10:4328–4334
Li Y-Q, Samad YA, Polychronopoulou K, Alhassan SM, Liao K (2014) Carbon aerogel from winter melon for highly efficient and recyclable oils and organic solvents absorption. ACS Sustain Chem Eng 2:1492–1497
Liang HW, Guan QF, Chen LF, Zhu Z, Zhang WJ, Yu SH (2012) Macroscopic-scale template synthesis of robust carbonaceous nanofiber hydrogels and aerogels and their applications. Angew Chem Int Ed 51:5101–5105
Liu C, Yang J, Tang Y, Yin L, Tang H, Li C (2015) Versatile fabrication of the magnetic polymer-based graphene foam and applications for oil–water separation. Colloids Surf A Physicochem Eng Asp 468:10–16
Marcano DC, Kosynkin DV, Berlin JM, Sinitskii A, Sun Z, Slesarev A, Alemany LB, Lu W, Tour JM (2010) Improved synthesis of graphene oxide. ACS Nano 4:4806–4814
Niu Z, Chen J, Hng HH, Ma J, Chen X (2012) A leavening strategy to prepare reduced graphene oxide foams. Adv Mater 24:4144–4150
Novoselov KS (2011) Graphene: the magic of flat carbon. ECS transactiones 20:45–46
O'Donnell K 1977: Chemical and physical properties of refined petroleum products
Park S, Lee K-S, Bozoklu G, Cai W, Nguyen ST, Ruoff RS (2008) Graphene oxide papers modified by divalent ions—enhancing mechanical properties via chemical cross-linking. ACS Nano 2:572–578
Pinto ML, Mestre AS, Carvalho AP, Jo P (2010) Comparison of methods to obtain micropore size distributions of carbonaceous materials from CO2 adsorption based on the Dubinin− Radushkevich isotherm. Ind Eng Chem Res 49:4726–4730
Powell T, McKirdy D (1973) Relationship between ratio of pristane to phytane, crude oil composition and geological environment in Australia. Nature 243:37–39
Rudziński W, Jaroniec M, Sokołowski S (1974) A new isotherm equation for multilayer adsorption on heterogeneous surfaces yielding the Dubinin-Radushkevich isotherm in the submonolayer region. Phys Lett A 48:171–172
Sharif F, Roberts E (2015) Study of graphene FOAM characteristics: adsorption and electrochemical regeneration, meeting abstracts. The electrochemical. Society:1197–1197
Stankovich S, Dikin DA, Piner RD, Kohlhaas KA, Kleinhammes A, Jia Y, Wu Y, Nguyen ST, Ruoff RS (2007) Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45:1558–1565
Sun H, La P, Zhu Z, Liang W, Yang B, Zhao X, Pei C, Li A (2014) Hydrophobic carbon nanotubes for removal of oils and organics from water. J Mater Sci 49:6855–6861
Suni S, Kosunen A-L, Hautala M, Pasila A, Romantschuk M (2004) Use of a by-product of peat excavation, cotton grass fibre, as a sorbent for oil-spills. Mar Pollut Bull 49:916–921
Toyoda M, Inagaki M (2000) Heavy oil sorption using exfoliated graphite: new application of exfoliated graphite to protect heavy oil pollution. Carbon 38:199–210
Tran DNH, Kabiri S, Sim TR, Losic D (2015) Selective adsorption of oil-water mixtures using polydimethylsiloxane (PDMS)-graphene sponges. Environ Sci: Water Res Technol 1:298–305
Tuncaboylu DC, Okay O (2009) Preparation and characterization of single-hole macroporous organogel particles of high toughness and superfast responsivity. Eur Polym J 45:2033–2042
Upadhyay RK, Dubey A, Waghmare PR, Priyadarshini R, Roy SS (2016) Multifunctional reduced graphene oxide coated cloths for oil/water separation and antibacterial application. RSC Adv 6:62760–62767
Vlassiouk I, Regmi M, Fulvio P, Dai S, Datskos P, Eres G, Smirnov S (2011) Role of hydrogen in chemical vapor deposition growth of large single-crystal graphene. ACS Nano 5:6069–6076
Wei Q, Mather R, Fotheringham A, Yang R (2003) Evaluation of nonwoven polypropylene oil sorbents in marine oil-spill recovery. Mar Pollut Bull 46:780–783
Wei D, Liu Y, Wang Y, Zhang H, Huang L, Yu G (2009) Synthesis of N-doped graphene by chemical vapor deposition and its electrical properties. Nano Lett 9:1752–1758
Xia K, Zhan H, Gu Y (2015) Two-dimensional graphene heterojunctions: the tunable mechanical properties. Carbon 95:1061–1068
Xiao K, Deng W, Keum JK, Yoon M, Vlassiouk IV, Clark KW, Li A-P, Kravchenko II, Gu G, Payzant EA (2013) Surface-induced orientation control of CuPc molecules for the epitaxial growth of highly ordered organic crystals on graphene. J Am Chem Soc 135:3680–3687
Xu Y, Sheng K, Li C, Shi G (2010) Self-assembled graphene hydrogel via a one-step hydrothermal process. ACS Nano 4:4324–4330
Yang W, Chen G, Shi Z, Liu C-C, Zhang L, Xie G, Cheng M, Wang D, Yang R, Shi D (2013) Epitaxial growth of single-domain graphene on hexagonal boron nitride. Nat Mater 12:792–797
Yang S, Chen L, Mu L, Ma P-C (2014) Magnetic graphene foam for efficient adsorption of oil and organic solvents. J Colloid Interface Sci 430:337–344
Yang S, Chen L, Mu L, Hao B, Ma P-C (2015) Low cost carbon fiber aerogel derived from bamboo for the adsorption of oils and organic solvents with excellent performances. RSC Adv 5:38470–38478
Zhang X, Sui Z, Xu B, Yue S, Luo Y, Zhan W, Liu B (2011) Mechanically strong and highly conductive graphene aerogel and its use as electrodes for electrochemical power sources. J Mater Chem 21:6494–6497
Zhang W, Zhai X, Xiang T, Zhou M, Zang D, Gao Z, Wang C (2017) Superhydrophobic melamine sponge with excellent surface selectivity and fire retardancy for oil absorption. J Mater Sci 52:73–85
Zhao J, Ren W, Cheng H-M (2012) Graphene sponge for efficient and repeatable adsorption and desorption of water contaminations. J Mater Chem 22:20197–20202
Zhao L, Yu B, Xue F, Xie J, Zhang X, Wu R, Wang R, Hu Z, Yang S-T, Luo J (2015) Facile hydrothermal preparation of recyclable S-doped graphene sponge for cu 2+ adsorption. J Hazard Mater 286:449–456
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The authors gratefully acknowledge the financial assistance provided by the Masdar Institute of Science and Technology. The authors would also like to thank the entire team of the Masdar Institute Microscopy Suite for their contribution and support.
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Bagoole, O., Rahman, M.M., Shah, S. et al. Functionalized three-dimensional graphene sponges for highly efficient crude and diesel oil adsorption. Environ Sci Pollut Res 25, 23091–23105 (2018). https://doi.org/10.1007/s11356-018-2248-z
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DOI: https://doi.org/10.1007/s11356-018-2248-z