Towards Dye Extraction Using A Three-Dimensional Graphene-Carbon Nanotubes Magnetic Aerogel
-
Abstract: A novel hybrid aerogel which can be magnetically extracted from water so filtration is unnecessary was developed. The hybrid (3DmGT-PVA) consists of 3D magnetic graphene-carbon nanotubes, which attracts dye, chained to polyvinyl alcohol, can be extracted from the water. Results indicated that a mass ratio of 12∶1 iron (III) chloride hexahydrate (FeCl3·6H2O) to graphene oxide (GO) and oxidized carbon nanotubes (O-CNT) mixture maximized adsorption capacity (qe=71.03 mg g−1 on methylene blue (MB)) and had a magnetic strength of MS=3.519 emu g−1. 3DmGT-PVA was shown to adsorb the most common dyes, crystal violet (CV, η=8.9%), methyl orange (MO, η=4.2%) and the mixture of MB, MO and CV (cocktail, η=11.1%). It was found that 3DmGT-PVA can be reused for three regeneration cycles, with a regeneration efficiency of over 82%. Finally, this aerogel was proved to be not toxic to the living organism, strongly proposing that this 3DmGT-PVA shows great promise as a means of treating industrial wastewater.
-
Key words:
- Magnetic aerogel /
- Dye removal /
- Graphene /
- Carbon nanotubes /
- Caenorhabditis elegans (C. elegans)
-
Figure 2. (a) Optical photographs of 3DmGT-PVA aerogels. FESEM images of aerogels: (b) F1 aerogel with pores, (c) F3 aerogel with 1500× and (d) 60000× magnification and (e) F6 aerogel
Figure 3. XRD patterns of (a) PVA, (b) GT, (c) Ni0.5Zn0.5Fe2O4 nanoparticles and (d) F3 aerogel
Figure 6. (a) MB solution treated by 3D mGT-PVA aerogel and GT after 48 h, (b) UV-Vis spectrums and (c) bar chart of qe and η.
Figure 7. Graph of η and amount of dye removed per mass of F3 aerogel against mass of F3 aerogel added.
Figure 9. Graphs of (a) qt against t, (b) pseudo-first-order and (c) pseudo-second-order kinetic models.
Figure 12. The effect of F3 on the overall lifespan of C. elegans. F3 did not significantly shorten the basal lifespan of the worm population (p>0.05), (n=90). Data are presented as mean ± standard deviation of one representative replicate.
Table 1. Saturation magnetization (MS), coercivity (HC) and retentivity (MR) at room temperature for the aerogels
Sample MS (emu g−1) HC (G) MR (emu g−1) F1 2.535 2.181 0.000937 F2 2.808 4.776 0.00203 F3 3.519 8.651 0.00338 F4 4.584 1.498 0.00211 F5 6.029 1.169 0.00237 F6 10.293 1.077 0.00278 Ni0.5Zn0.5Fe2O4 10.696 0.625 0.00252 
下载: 导出CSV
Table 2. Kinetic parameters for F3 aerogel.
Kinetic Model Parameters Value Pseudo first- order qe (mg g−1) 66.87 qe error (%) 5.85 k1 (1 min−1) 0.0109 R2 0.9453 Pseudo second-order qe (mg g−1) 84.75 qe error (%) 19.3 k2 (g mg−1 min−1) 0.00016 R2 0.9528 V0 (mg g−1 min−1) 1.15
下载: 导出CSV
-
[1] Chen D, Zeng Z, Zeng Y, et al. Removal of methylene blue and mechanism on magnetic γ-Fe2O3/SiO2 nanocomposite from aqueous solution[J]. Water Resources and Industry,2016,15:1-13. doi: 10.1016/j.wri.2016.05.003 [2] Liu C, Liu H, Xu A, et al. In situ reduced and assembled three-dimensional graphene aerogel for efficient dye removal[J]. Journal of Alloys and Compounds,2017,714:522-529. doi: 10.1016/j.jallcom.2017.04.245 [3] Nagelkerke NJD. A note on a general definition of the coefficient of determination[J]. Biometrika,1991,78(3):691-692. doi: 10.1093/biomet/78.3.691 [4] Xu Z, Li X, Teng K, et al. High flux and rejection of hierarchical composite membranes based on carbon nanotube network and ultrathin electrospun nanofibrous layer for dye removal[J]. Journal of Membrane Science,2017,535:94-102. doi: 10.1016/j.memsci.2017.04.029 [5] Ding Y, Tian Z, Li H, et al. Efficient removal of organic dyes using a three-dimensional graphene aerogel with excellent recycling stability[J]. New Carbon Materials,2019,34(4):315-324. doi: 10.1016/S1872-5805(19)30020-4 [6] El-Moselhy MM, Kamal SM. Selective removal and preconcentration of methylene blue from polluted water using cation exchange polymeric material[J]. Groundwater for Sustainable Development,2018,6:6-13. doi: 10.1016/j.gsd.2017.10.001 [7] Tolba GMK, Bastaweesy AM, Ashour EA, et al. Effective and highly recyclable ceramic membrane based on amorphous nanosilica for dye removal from the aqueous solutions[J]. Arabian Journal of Chemistry,2016,9(2):287-296. doi: 10.1016/j.arabjc.2015.05.009 [8] García JR, Sedran U, Zaini MAA, et al. Preparation, characterization, and dye removal study of activated carbon prepared from palm kernel shell[J]. Environmental Science and Pollution Research,2018,25(6):5076-5085. doi: 10.1007/s11356-017-8975-8 [9] Zheng W, Qi T, Zhang Y, et al. Fabrication and characterization of a multi-walled carbon nanotube-based counter electrode for dye-sensitized solar cells[J]. New Carbon Materials,2015,30(5):391-396. doi: 10.1016/S1872-5805(15)60198-6 [10] Shen Y, Zhu X, Zhu L, et al. Synergistic effects of 2D graphene oxide nanosheets and 1D carbon nanotubes in the constructed 3D carbon aerogel for high performance pollutant removal[J]. Chemical Engineering Journal,2017,314:336-346. doi: 10.1016/j.cej.2016.11.132 [11] GAO Feng, QIN Shi-hui, ZANG Yun-hao, GU Jian-feng QJ. Highly efficient formation of Mn3O4-graphene oxide hybrid aerogels for use as the cathode material of high performance lithium ion batteries[J]. New Carbon Materials,2020,35(2):121-130. doi: 10.1016/S1872-5805(20)60479-6 [12] Tran H V, Bui LT, Dinh TT, et al. Graphene oxide/Fe3O4/chitosan nanocomposite: a recoverable and recyclable adsorbent for organic dyes removal. Application to methylene blue[J]. Materials Research Express,2017,4(3):35701. doi: 10.1088/2053-1591/aa6096 [13] Lee B, Lee S, Lee M, et al. Carbon nanotube-bonded graphene hybrid aerogels and their application to water purification[J]. Nanoscale,2015,7(15):6782-6789. doi: 10.1039/C5NR01018G [14] Areerob Y, Cho JY, Jang WK, et al. Enhanced sonocatalytic degradation of organic dyes from aqueous solutions by novel synthesis of mesoporous Fe3O4-graphene/ZnO@SiO2 nanocomposites[J]. Ultrasonics Sonochemistry,2018,41:267-278. doi: 10.1016/j.ultsonch.2017.09.034 [15] Meidanchi A, Akhavan O. Superparamagnetic zinc ferrite spinel–graphene nanostructures for fast wastewater purification[J]. Carbon,2014,69:230-238. doi: 10.1016/j.carbon.2013.12.019 [16] Dai J, Huang T, Tian S, et al. High structure stability and outstanding adsorption performance of graphene oxide aerogel supported by polyvinyl alcohol for waste water treatment[J]. Materials & Design,2016,107:187-197. [17] Zhang L, Wang Z, Xu C, et al. High strength graphene oxide/polyvinyl alcohol composite hydrogels[J]. J. Mater. Chem,2011,21(28):10399-10406. doi: 10.1039/c0jm04043f [18] Yao W, Geng C, Han D, et al. Strong and conductive double-network graphene/PVA gel[J]. RSC Adv,2014,4(74):39588-39595. doi: 10.1039/C4RA02674H [19] Bai H, Li C, Wang X, et al. A pH-sensitive graphene oxide composite hydrogel[J]. Chem. Commun,2000,46(14):2376-2378. [20] K N, Ramana G V, D S, et al. Synthesis of Graphene Oxide by Modified Hummers Method and Hydrothermal Synthesis of Graphene-NiO Nano Composite for Supercapacitor Application[J]. Journal of Material Science & Engineering,2016,05(06):284. [21] Pawelec KM, Husmann A, Best SM, et al. Altering crystal growth and annealing in ice-templated scaffolds[J]. Journal of Materials Science,2015,50(23):7537-7543. doi: 10.1007/s10853-015-9343-z [22] Kong C, Yehye WA, Abd Rahman N, et al. Discovery of potential anti-infectives against Staphylococcus aureus using a Caenorhabditis elegans infection model[J]. BMC Complementary and Alternative Medicine,2014,14(1):4. doi: 10.1186/1472-6882-14-4 [23] Chen L, Li Y, Du Q, et al. High performance agar/graphene oxide composite aerogel for methylene blue removal[J]. Carbohydrate Polymers,2017,155:345-353. doi: 10.1016/j.carbpol.2016.08.047 [24] Liu D, Li J, Sun F, et al. Liquid crystal microphase separation of cellulose nanocrystals in wet-spun PVA composite fibers[J]. RSC Adv,2014,4(58):30784-30789. doi: 10.1039/C4RA04063E [25] Shahriary L, Athawale AA. Graphene oxide synthesized by using modified hummers approach[J]. Int. J. Renew. Energy Environ. Eng,2014,2(1):58-63. [26] Chiang Y-C, Lin W-H, Chang Y-C. The influence of treatment duration on multi-walled carbon nanotubes functionalized by H2SO4/HNO3 oxidation[J]. Applied Surface Science,2011,257(6):2401-2410. doi: 10.1016/j.apsusc.2010.09.110 [27] El-Sheikh SM, Rashad MM, Harraz FA. Morphological investigation and magnetic properties of nickel zinc ferrite 1D nanostructures synthesized via thermal decomposition method[J]. Journal of Nanoparticle Research,2013,15(10):1967. doi: 10.1007/s11051-013-1967-9 [28] Wang X, Liu X, Yuan H, et al. Non-covalently functionalized graphene strengthened poly(vinyl alcohol)[J]. Materials & Design,2018,139:372-379. [29] Shahane GS, Kumar A, Arora M, et al. Synthesis and characterization of Ni–Zn ferrite nanoparticles[J]. Journal of Magnetism and Magnetic Materials,2010,322(8):1015-1019. doi: 10.1016/j.jmmm.2009.12.006 [30] Afkhami A, Sayari S, Moosavi R, et al. Magnetic nickel zinc ferrite nanocomposite as an efficient adsorbent for the removal of organic dyes from aqueous solutions[J]. Journal of Industrial and Engineering Chemistry,2015,21:920-924. doi: 10.1016/j.jiec.2014.04.033 [31] Ho Y-S. Review of second-order models for adsorption systems[J]. Journal of Hazardous Materials,2006,136(3):681-689. doi: 10.1016/j.jhazmat.2005.12.043 [32] Sun H, Cao L, Lu L. Magnetite/reduced graphene oxide nanocomposites: One step solvothermal synthesis and use as a novel platform for removal of dye pollutants[J]. Nano Research,2011,4(6):550-562. doi: 10.1007/s12274-011-0111-3 [33] Plazinski W, Dziuba J, Rudzinski W. Modeling of sorption kinetics: the pseudo-second order equation and the sorbate intraparticle diffusivity[J]. Adsorption,2013,19(5):1055-1064. doi: 10.1007/s10450-013-9529-0 [34] Ai L, Zhang C, Chen Z. Removal of methylene blue from aqueous solution by a solvothermal-synthesized graphene/magnetite composite[J]. Journal of Hazardous Materials,2011,192(3):1515-1524. doi: 10.1016/j.jhazmat.2011.06.068 [35] Robati D, Mirza B, Rajabi M, et al. Removal of hazardous dyes-BR 12 and methyl orange using graphene oxide as an adsorbent from aqueous phase[J]. Chemical Engineering Journal,2016,284:687-697. doi: 10.1016/j.cej.2015.08.131 [36] Pei Y, Wang M, Tian D, et al. Synthesis of core–shell SiO2@MgO with flower like morphology for removal of crystal violet in water[J]. Journal of Colloid and Interface Science,2015,453:194-201. doi: 10.1016/j.jcis.2015.05.003 [37] Geng Z, Lin Y, Yu X, et al. Highly efficient dye adsorption and removal: a functional hybrid of reduced graphene oxide–Fe3O4 nanoparticles as an easily regenerative adsorbent[J]. Journal of Materials Chemistry,2012,22(8):3527-3535. doi: 10.1039/c2jm15544c -
点击查看大图
图(12) / 表(2)
计量
- 文章访问数: 46
- HTML全文浏览量: 10
- PDF下载量: 13
- 被引次数: 0
