Preparation and Application of Superhydrophobic and Robust Graphene Composites Oil/Water Separation Material†

doi:10.7503/cjcu20180332

Abstract

Abstract:

Superhydrophobic reduced graphene oxide-wrapped melamine sponge(RGO-MS) was prepared via a facile surface modification method with graphene oxide(GO) modification amphipathic melamine sponge(MS). X-ray diffraction(XRD), Raman spectra, Fourier transform infrared spectroscopy(FTIR) and scanning electron microscopy(SEM) were used to investigate the structure, morphology and component of RGO-MS. The mechanical property, hydrophobicity, oil adsorption capacity, reusability and oil/water separation efficiency of RGO-MS were also explored. The results revealed that reduced graphene oxide(RGO) coating was closely linked to MS skeleton. In addition, RGO-MS possesses outstanding adsorption capacity for floating oil and heavy oil underwater, and could maintain ultra-high adsorption capacity even after 50 adsorption-squeezing cycles which is as high as 90 % of its initial adsorption capacity. Moreover, RGO-MS exhibits extremely high separation efficiency up to 4.5×10⁶ L/(m³·h) under non-turbulent and 3×10⁶L/(m³·h) under turbulent condition water/oil system. Therefore, RGO-MS has a huge application prospect in dealing with the large-scale removal of oil and organic spillage cleanup.

Key words: Reduced graphene oxide-wrapped melamine sponge, Superhydrophobic, Adsorption capacity, Oil/water separation

CLC Number:

O648

TrendMD:

QIU Lijuan,ZHANG Ying,LIU Shuaizhuo,ZHANG Qian,ZHOU Ying. Preparation and Application of Superhydrophobic and Robust Graphene Composites Oil/Water Separation Material^†[J]. Chem. J. Chinese Universities, 2018, 39(12): 2758.

Figures/Tables 13

Fig.1 XRD patterns of MS(a) and RGO-MS(b)

Fig.2 Raman(A) and FTIR spectra(B) of MS(a), GO-MS(b) and RGO-MS(c)

Fig.3 Optical images of RGO-MS prepared with watch glasses(A) and beaker(B)

Fig.4 SEM images of MS(A, D), GO-MS(B, E) and RGO-MS(C, F) after 30 squeezing and 20 twist testsInsets: the photographs of the corresponding sponges.

Fig.5 Compressive stress-strain curves of RGO-MS with different set strain of 40%, 60%, 80%, respectively(A) and cyclic compressive stress-strain curves of RGO-MS at 60% strain(B)Insets: the process of compression text(A) and the photograph of the twisted RGO-MS(B).

Fig.6 Optical images of static water droplet on the surface of MS(A) and RGO-MS(B, C) (C) Enlarged image of static water dropcet on the surface of RGO-MS.

Fig.7 Dynamic contact angles test of water droplet on RGO-MSVolume of water droplet: (A) 4 μL; (B) 7 μL; (C) 4 μL.

Table 1 Comparison of adsorption capacity of various adsorbents

Adsorbent	Contact angle/(°)	Q_wt/(g·g^-1)	Adsorption rate/(L·h^-1)	Cycle time	Ref.
RGO-MS	163±10	62—120	18	>50	This work
PEI/RGO-Polyurethane	95.82	6.9—8.8		30	[9]
RGO	114±2	20—86		>10	[17]
GO-CNT	147.6±2	21—35	6	8	[30]
PDMS-graphene	126.6	2—8	9	5	[31]
RGO	135	100—280	<6	5	[38]
Nanodiamond- Polyurethane	150±2	3—60		10	[39]
RGO-MS	154	57—112		20	[40]

Fig.8 Adsorption capacity towards oil and organic solvents over RGO-MS(A) and recycling adsorption performance towards hexane and pump oil over RGO-MS(B)Insets in (B) are the photographs of adsorption-squeezing process over RGO-MS.

Fig.9 Selective adsorption of RGO-MS for floating oil(pump oil)(A) and underwater heavy oil(phenixin)(B)

Fig.10 Change of non-turbulent floating oil liquid level in continuous oil-water separation process with RGO-MS at different time Time/s: (A) 0; (B) 5; (C) 10; (D) 20.

Fig.11 Change of turbulent floating oil liquid level in continuous oil-water separation process with RGO-MS at different time Time/s: (A) 0; (B) 5; (C) 20; (D) 30.

Fig.12 Change of heavy oil liquid level in continuous oil-water separation process with RGO-MS at different time

References 40

[1]	Schrope M., Nature, 2011, 472(7342), 152—154
[2]	Ivshina I.B., Kuyukina M.S., Krivoruchko A.V., Elkin A.A., Makarov S.O., Cunningham C.J., Peshkur T.A., Atlas R.M., Philp J.C., Environ. Sci.: Processes Impacts,2015, 17, 1201—1219
[3]	Dubansky B., Whitehead A., Miller J.T., Rice C.D., Galvez F., Environ. Sci. Technol.,2013, 47(10), 5074—5082
[4]	Joye S.B., Science, 2015, 349(6248), 592—593
[5]	Zahed M.A., Aziz H.A., Isa M.H., Mohajeri L., Mohajeri S., Bioresource Technol.,2010, 101(24), 9455—9460
[6]	Broje V., Keller A.A., Environ. Sci. Technol.,2006, 40(24), 7914—7918
[7]	Wan W.C., Lin Y.H., Prakash A., Zhou Y., J. Mater. Chem. A,2016, 4(48), 18687—18705
[8]	Wei Q.F., Mather R.R., Fotheringham A.F., Yang R.D., Mar. Pollut. Bull.,2003, 46(6), 780—783
[9]	Periasamy A.P., Wu W.P., Ravindranath R., Roy P., Lin G.L., Chang H.T., Mar. Pollut. Bull.,2017, 114(2), 888—895
[10]	Gupta S., Tai N.H., J. Mater. Chem. A,2016, 4(5), 1550—1565
[11]	Pham V.H., Dickerson J.H., ACS Appl. Mater. Interfaces,2014, 6(16), 14181—14188
[12]	Lei Z.W., Zhang G.Z., Deng Y.H., Wang C.Y., ACS Appl. Mater. Interfaces,2017, 9(10), 8967—8974
[13]	Yu C.L., Yu C.M., Cui L.Y., Song Z.Y., Zhao X.Y., Ma Y., Jiang L., Adv. Mater. Interfaces,2017, 4(3), 1600862
[14]	Qiu L.J., Wan W.C., Tong Z.Q., Zhang R.Y., Li L.N., Zhou Y., New J. Chem.,2018, 42, 1003—1009
[15]	Hu H., Zhao Z.B., Wan W.B., Gogotsi Y., Qiu J.S., Adv. Mater.,2013, 25(15), 2219—2223
[16]	Sun Y.R., Yang M.X., Yu F., Chen J.H., Ma J., Prog. Chem., 2015, 27(8), 1133—1146
	(孙怡然, 杨明轩, 于飞, 陈君红, 马杰. 化学进展, 2015, 27(8), 1133—1146)
[17]	Bi H.C., Xie X., Yin K.B., Zhou Y.L., Wan S., He L.B., Xu F., Banhart F., Sun L.T., Ruoff R.S., Adv. Funct. Mater.,2012, 22, 4421—4425
[18]	Xiao J.L., Zhang J.F., Lv W.Y., Song Y.H., Zheng Q., Carbon,2017, 123, 354—363
[19]	Sun H.Y., Xu Z., Gao C., Adv. Mater.,2013, 25(18), 2554—2560
[20]	Chen Z.X., Lu H.B., Chem. J. Chinese Universities,2013, 34(9), 2020—2033
	(陈仲欣, 卢红斌. 高等学校化学学报, 2013, 34(9), 2020—2033)
[21]	Wang Z.T., Xiao C.F., Zhao J., Hu X., Xu N.K., Chem. J. Chinese Universities,2014, 35(11), 2410—2417
	(王子涛, 肖长发, 赵健, 胡霄, 徐乃库. 高等学校化学学报, 2014, 35(11), 2410—2417)
[22]	Zhu H.G., Chen D.Y., An W., Li N.J., Xu Q.F., Li H., He J.H., Lu J.M., Small,2015, 11(39), 5222—5229
[23]	Stolz A., Floch S.L., Reinert L., Ramos S. M.M., Tuaillon-Combes J., Soneda Y., Chaudet P., Baillis D., Blanchard N., Duclaux L., San-Miguel A., Carbon,2016, 107, 198—208
[24]	Dong X.C., Chen J., Ma Y.W., Wang J., Chan-Park M.B., Liu X.M., Wang L.H., Huang W., Chen P., Chem. Commun.,2012, 48(86), 10660—10662
[25]	Ji C.H., Zhang K., Li L., Chen X.X., Hu J.L., Yan D.Y., Xiao G.Y., He X.H., J. Mater. Chem. A,2017, 5(22), 11263—11270
[26]	Li R., Chen C.B., Li J., Xu L.M., Xiao G.Y., Yan D.Y., J. Mater. Chem. A,2014, 2(9), 3057—3064
[27]	Cong H.P., Ren X.C., Wang P., Yu S.H., ACS Nano,2012, 6(3), 2693—2703
[28]	Wan W.C., Zhang F., Yu S., Zhang R.Y., Zhou Y., New J. Chem.,2016, 40(4), 3040—3046
[29]	Wan W.C., Zhang R.Y., Li W., Liu H., Lin Y.H., Li L.N., Zhou Y., Environ. Sci.: Nano,2016, 3, 107—113
[30]	Kabiri S., Tran D. N.H., Altalhi T., Losic D., Carbon,2014, 80, 523—533
[31]	Tran D. N.H., Kabiri S., Sim T.R., Losic D., Environ. Sci.: Water Res. Technol.,2015, 1, 298—305
[32]	Yang D.X., Velamakanni A., Bozoklu G., Park S., Stoller M., Piner R.D., Stankovich S., Jung I., Field D.A., Ventrice C.A., Ruoff R.S., Carbon,2009, 47(1), 145—152
[33]	Ge J., Shi L.A., Wang Y.C., Zhao H.Y., Yao H.B., Zhu Y.B., Zhang Y., Zhu H.W., Wu H. A, Yu S. H., Nat. Nanotechnol.,2017, 12, 434—440
[34]	Stankovich S., Dikin D.A., Piner R.D., Kohlhaas K.A., Kleinhammes A., Jia Y.Y., Wu Y., Nguyen S.T., Ruoff R.S., Carbon,2007, 45(7), 1558—1565
[35]	Zhang J.L., Yang H.J., Shen G.X., Cheng P., Zhang J.Y., Guo S.W., Chem. Commun.,2010, 46, 1112—1114
[36]	Yao H.B., Huang G., Cui C.H., Wang X.H., Yu S.H., Adv. Mater.,2011, 23(32), 3643—3647
[37]	Kuang J., Liu L.Q., Gao Y., Zhou D., Chen Z., Han B.H., Zhang Z., Nanoscale,2013, 5(24), 12171—12177
[38]	He Y.L., Li J.H., Luo K., Li L.F., Chen J.B., Li J.Y., Ind. Eng. Chem. Res.,2016, 55(13), 3775—3781
[39]	Cao N., Yang B., Barras A., Szunerits S., Boukherroub R., Chem. Eng. J.,2017, 307, 319—325
[40]	Song S., Yang H., Su C.P., Jiang Z.B., Lu Z., Chem. Eng. J.,2016, 306, 504—511