Reduced graphene oxide/metal oxide nanoparticles composite membranes for highly efficient molecular separation

doi:10.1016/j.jmst.2018.05.008

Abstract

Abstract:

Graphene oxide (GO) membranes play an important role in various nanofiltration applications including desalination, water purification, gas separation, and pervaporation. However, it is still very challenging to achieve both high separation efficiency and good water permeance at the same time. Here, we synthesized two kinds of GO-based composite membranes i.e. reduced GO (rGO)@MoO₂ and rGO@WO₃ by in-situ growth of metal nanoparticles on the surface of GO sheets. They show a high separation efficiency of ～100% for various organic dyes such as rhodamine B, methylene blue and evans blue, along with a water permeance over 125 L m^-2 h^-1 bar^-1. The high water permeance and rejection efficiency open up the possibility for the real applications of our GO composite membranes in water purification and wastewater treatment. Furthermore, this composite strategy can be readily extended to the fabrication of other ultrathin molecular sieving membranes for a wide range of molecular separation applications.

Key words: Graphene oxide, Composite, Membranes, Separation, Permeance

Khalid Hussain Thebo, Xitang Qian, Qinwei Wei, Qing Zhang, Hui-Ming Cheng, Wencai Ren. Reduced graphene oxide/metal oxide nanoparticles composite membranes for highly efficient molecular separation[J]. J. Mater. Sci. Technol., 2018, 34(9): 1481-1486.

Figures/Tables 4

Fig. 1. Structure characterization of rGO@metal oxide nanoparticles composite membranes. (a, b) Top-view SEM images of rGO@MoO2 (a) and rGO@WO3 (b) composite membrane. (c, d) Cross-sectional SEM images of rGO@MoO2 (c) and rGO@WO3 (d) composite membrane. (e, f) Raman spectra (e) and XRD patterns (f) of GO, rGO@MoO2, and rGO@WO3 membrane.

Fig. 2. Chemical composition and bonding characterization of rGO@metal oxide nanoparticles composite membranes. (a-c) C 1s XPS spectra of GO (a), rGO@MoO2 (b), and rGO@WO3 membranes (c). (d) FTIR spectra of GO, rGO@MoO2, and rGO@WO3 composite membranes.

Fig. 3. Permeance and separation performance of rGO@metal oxide composite membranes. (a, b) Permeance and rejection to different organic dyes of rGO@MoO2 (a) and rGO@WO3 (b) composite membranes at a trans-membrane pressure of 1.0 bar. (c, d) UV-vis absorption spectra of the feed, permeate and retentate of RB after filtration by rGO@MoO2 (c) and rGO@WO3 (d) composite membranes. The insets show the photos of the feed and permeate solutions.

Table 1 Water permeance and separation performance of rGO@metal oxide nanoparticles composite membranes to various dye molecules at 25 °C.

Dyes	MW (g mol^-1)	Charge	rGO@MoO₂ membrane (800 nm)		rGO@WO₃ membrane (1000 nm)
Dyes	MW (g mol^-1)	Charge	Permeance (L m^-2 h^-1 bar^-1)	Rejection (%)	Permeance (L m^-2 h^-1 bar^-1)	Rejection (%)
RB	479.0	+	145	100	140	100
MLB	373.0	+	145	100	140	100
FA	585.53	-	150	95	160	98
MB	799.8	-	180	90	180	85
EB	960.0	-	125	100	130	100

References

[1]	L. Wang, M.S.H.Boutilier, P.R. Kidambi, D. Jang, N.G. Hadji-constantinou, R. Karnik, Nat. Nanotechnol., 12(2017), pp. 509-522
[2]	J.R. Werber, C.O. Osuji, M. Elimelech, Nat. Rev. Mater. (2016), p. 16018
[3]	Q. Wang, N. Li, B. Bolto, M. Hoang, Z. Xie, Desalination, 387(2016), pp. 46-60
[4]	G. Liu, W. Jin, N. Xu, Chem. Soc. Rev., 44(2015), pp. 5016-5030
[5]	A.W. Mohammad, Y.H. Teow, W.L. Ang, Y.T. Chung, N. Hilal, Desalination, 356(2015), pp. 226-254
[6]	A. Morelos-Gomez, R. Cruz-Silva, H. Muramatsu, J. Ortiz-Medina, T. Araki, T. Fukuyo, S. Tejima, K. Takeuchi, T. Hayashi, M. Terrones, M. Endo, Nat. Nanotechnol., 12(2017), pp. 1083-1088
[7]	A. Akbari, P. Sheath, S.T. Martin, D.B. Shinde, M. Shaibani, P.C. Banerjee, R. Tkacz, D. Bhattacharyya, M. Majumder, Nat. Commun., 7(2016), p. 10891
[8]	L. Chen, G. Shi, J. Shen, B. Peng, B. Zhang, Y. Wang, F. Bian, J. Wang, D. Li, Z. Qian, G. Xu, G. Liu, J. Zeng, L. Zhang, Y. Yang, G. Zhou, M. Wu, W. Jin, J. Li, H. Fang, Nature, 550(2017), p. 380
[9]	R.K. Joshi, P. Carbone, F.C. Wang, V.G. Kravets, Y. Su, I.V. Grigorieva, H.A. Wu, A.K. Geim, R.R. Nair, Science, 343(2014), pp. 752-754
[10]	Q. Yang, Y. Su, C. Chi, C.T. Cherian, K. Huang, V.G. Kravets, F.C. Wang, J.C. Zhang, A. Pratt, A.N. Grigorenko, F. Guinea, A.K. Geim, R.R. Nair, Nat. Mater., 16(2017), pp. 1198-1202
[11]	J. Abraham, K.S. Vasu, C.D. Williams, K. Gopinadhan, Y. Su, C.T. Cherian, J. Dix, E. Prestat, S.J. Haigh, I.V. Grigorieva, P. Carbone, A.K. Geim, R.R. Nair, Nat. Nanotechnol., 12(2017), pp. 546-550
[12]	K.H. Thebo, X. Qian, Q. Zhang, L. Chen, H.M. Cheng, W. Ren, Nat. Commun., 9(2018), p. 486
[13]	S. Pei, Q. Wei, K. Huang, H.M. Cheng, W. Ren, Nat. Commun., 9(2018), p. 145
[14]	R.R. Nair, H.A. Wu, P.N. Jayaram, I.V. Grigorieva, A.K. Geim, Science, 335(2012), pp. 442-444
[15]	Y. You, X.H. Jin, X.Y. Wen, V. Sahajwalla, V. Chen, H. Bustamante, R.K. Joshi, Carbon, 129(2018), pp. 415-419
[16]	L. Qiu, X. Zhang, W. Yang, Y. Wang, G.P. Simon, D. Li, Chem. Commun., 47(2011), pp. 5810-5812
[17]	Y. Han, Z. Xu, C. Gao, Adv. Funct. Mater., 23(2013), pp. 3693-3700
[18]	M. Hu, B. Mi, J. Membr. Sci., 469(2014), pp. 80-87
[19]	M. Hu, B. Mi, Environ. Sci. Technol., 47(2013), pp. 3715-3723
[20]	X. Zhao, Y. Su, Y. Liu, Y. Li, Z. Jiang, ACS Appl. Mater. Interfaces, 8(2016), pp. 8247-8256
[21]	Y. Jiang, W. Wang, D. Liu, Y. Nie, W. Li, J. Wu, F. Zhang, P. Biswas, J.D. Fortner, Environ. Sci. Technol., 49(2015), pp. 6846-6854
[22]	Y. Zhang, S. Zhang, T.S. Chung, Environ. Sci. Technol., 49(2015), pp. 10235-10242
[23]	D. Qin, Z. Liu, D.D. Sun, X. Song, H. Bai, Sci. Rep., 5(2015), p. 14530
[24]	R. Wang, Z. Li, W. Liu, W. Jiao, L. Hao, F. Yang, Compos. Sci. Technol., 87(2013), pp. 29-35
[25]	Q. Cheng, M. Wu, M. Li, L. Jiang, Z. Tang, Angew. Chem. Int. Ed., 52(2013), pp. 3750-3755
[26]	S.M. Kang, S. Park, D. Kim, S.Y. Park, R.S. Ruoff, H. Lee, Adv. Funct. Mater., 21(2011), pp. 108-112
[27]	K.W. Putz, O.C. Compton, M.J. Palmeri, S.T. Nguyen, L.C. Brinson, Adv. Funct. Mater., 20(2010), pp. 3322-3329
[28]	V. Georgakilas, M. Otyepka, A.B. Bourlinos, V. Chandra, N. Kim, K.C. Kemp, P. Hobza, R. Zboril, K.S. Kim, Chem. Rev., 112(2012), pp. 6156-6214
[29]	G. Bottari, M.A. Herranz, L. Wibmer, M. Volland, L. Rodr?guez-Pe?ez, D.M. Guldi, A. Hirsch, N. Martin, F. D’Souza, T. Torres, Chem. Soc. Rev., 46(2017), pp. 4464-4500
[30]	E. Yang, A.B. Alayande, C. Kim, J. Song, I.S. Kim, Desalination, 426(2018), pp. 21-31
[31]	M. Zhang, K. Guan, J. Shen, G. Liu, Y. Fan, W. Jin, J. AIChE, 63(2017), pp. 5054-5063
[32]	K. Goh, W. Jiang, H. Karahan, S. Zhai, L. Wei, D. Yu, A.G. Fane, R. Wang, Y. Chen, Adv. Funct. Mater., 25(2015), pp. 7348-7359
[33]	L. Huang, J. Chen, T. Gao, M. Zhang, Y. Li, L. Dai, L. Qu, G. Shi, Adv. Mater., 28(2016), pp. 8669-8674
[34]	W.S. Hummers, R.E. Offeman, J. Am. Chem. Soc., 80(1958)1339-1339
[35]	Y. Sun, X. Hu, W. Luo, Y. Huang, ACS Nano, 5(2011), pp. 7100-7107
[36]	L. Gan, L. Xu, S. Shang, X. Zhou, L. Meng, Ceram. Int., 42(2016), pp. 15235-15241
[37]	Z. Wu, W. Ren, L. Wen, L. Gao, J. Zhao, Z. Chen, G. Zhou, F. Li, H.M. Cheng, ACS Nano, 4(2010), pp. 3187-3194
[38]	Z. Wu, D. Wang, W. Ren, J. Zhao, G. Zhou, F. Li, H.M. Cheng, Adv. Funct. Mater., 20(2010), pp. 3595-3602
[39]	G. Zhou, D. Wang, L. Yin, N. Li, F. Li, H.M. Cheng, ACS Nano, 6(2012), pp. 3214-3223
[40]	J. Deng, Y. You, H. Bustamante, V. Sahajwalla, R.K. Joshi, Chem. Sci., 8(2017), pp. 1701-1704
[41]	K. Cao, Z. Jiang, J. Zhao, C. Zhao, C. Gao, F. Pan, B. Wang, X. Cao, J. Yang, J. Membr. Sci., 469(2014), pp. 272-283