Abstract
Graphene oxide (GO) with different sizes is inevitably released into the water environment during its production, use, and disposal. Aggregation and sedimentation would occur when GO entered into the water with high ionic strength. However, the environmental behavior and fate of GO in the coastal water are not well known. Therefore, in the present study, the aggregation and sedimentation of GO nanosheets with different sizes in seawater with different salinities were investigated. GO nanosheets with different sizes were prepared by the ultrasonic pulverization. Compared to original GO, the ultrasonically pulverized GO was more stably dispersed in deionized water. In artificial seawater, the aggregation–sedimentation process became more intense with increasing GO concentration and salinity. With the decrease of the GO nanosheet size, the aggregation–sedimentation rate increased, while the critical aggregation and sedimentation salinity decreased. As GO could deposit in wide coastal waters, which might cause potential ecological risks to marine benthic organisms, its environmental behavior, fate, and ecological risks in the coastal water should be further investigated.
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11051-018-4421-1/MediaObjects/11051_2018_4421_Fig1_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11051-018-4421-1/MediaObjects/11051_2018_4421_Fig2_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11051-018-4421-1/MediaObjects/11051_2018_4421_Fig3_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11051-018-4421-1/MediaObjects/11051_2018_4421_Fig4_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11051-018-4421-1/MediaObjects/11051_2018_4421_Fig5_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11051-018-4421-1/MediaObjects/11051_2018_4421_Fig6_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs11051-018-4421-1/MediaObjects/11051_2018_4421_Fig7_HTML.png)
Similar content being viewed by others
References
Acik M, Lee G, Mattevi C, Chhowalla M, Cho K, Chabal YJ (2010) Unusual infrared-absorption mechanism in thermally reduced graphene oxide. Nat Mater 9:840–845
Bijarbooneh FH, Zhao Y, Kim JH, Sun ZQ, Malgars V, Aboutalebi SH, Heo YU, Ikegami M, Dou SX (2013) Aqueous colloidal stability evaluated by zeta potential measurement and resultant TiO2 for superior photovoltaic performance. J Am Ceram Soc 96:2636–2643
Cai W, Piner RD, Stadermann FJ, Park S, Shaibat MA, Ishii Y, Yang D, Velamakanni A, An SJ, Stoller M, An J, Chen D, Ruoff RS (2008) Synthesis and solid-state NMR structural characterization of 13C-labeled graphite oxide. Science 321:1815–1817
Chen J, Chi FY, Huang L, Zhang M, Yao BW, Li YR, Li C, Shi GQ (2016) Synthesis of graphene oxide sheets with controlled sizes from sieved graphite flakes. Carbon 110:34–40
Chowdhury I, Duch MC, Mansukhani ND, Hersam MC, Bouchard D (2013) Collidal properties and stability of graphene oxide nanomaterials in the aquatic environment. Environ Sci Techol 47:6288–6296
Deguchi S, Alargova RG, Tsujii K (2001) Stable dispersion of fullerenes, C60 and C70, in water. Preparation and characterization. Langmuir 17:6013–6017
Fortner JD, Lyon DY, Sayes CM, Boyd AM, Falkner JC, Hotze EM, Alemany LB, Tao YJ, Guo W, Ausman KD, Colvin VL, Hughes JB (2005) C60 in water: nanocrystal formation and microbial response. Environ Sci Technol 39:4307–4316
Gudarzi MM (2016) Colloidal stability of graphene oxide: aggregation in two dimensions. Langmuir 32:5058–5068
Hou WC, Chowdhury I, Goodwin DG Jr, Henderson WM, Fairbrother DH, Bouchard D, Zepp RG (2015) Photochemical transformation of graphene oxide in sunlight. Environ Sci Technol 49:3435–3443
Hua ZL, Tang ZQ, Bai X, Zhang JN, Yu L, Cheng HM (2015) Aggregation and resuspension of graphene oxide in simulated natural surface aquatic environments. Environ Pollut 205:161–169
Jiang Y, Raliya R, Fortner JD, Biswas P (2016) Graphene oxides in water: correlating morphology and surface chemistry with aggregation behavior. Environ Sci Technol 50:6964–6973
Kumar R, Savu R, Joanni E, Vaz AR, Canesqui MA, Singh RK, Timm RA, Kubota LT, Moshkalev SA (2016) Fabrication of interdigitated micro-supercapacitor devices by direct laser writing onto ultra-thin, flexible and free-standing graphite oxide films. RSC Adv 6(88):84769–84776
Limbach LK, Li Y, Grass RN, Brunner TJ, Hintermann MA, Muller M, Gunther D, Stark WJ (2005) Oxide nanoparticle uptake in human lung fibroblasts: effects of particle size, agglomeration, and diffusion at low concentrations. Environ Sci Technol 39:9370–9376
Liu Z, Robinson JT, Sun X, Dai H (2008) PEGylated nanographene oxide for delivery of water insoluble cancer drugs. J Am Chem Soc 130:10876–10877
Luo J, Zhao X, Wu J, Jang HD, Kung HH, Huang J (2012) Crumpled graphene-encapsulated Si nanoparticles for Lithium ion battery anodes. J Phys Chem Lett 3:1824–1829
Luo ZJ, Geng HZ, Zhang X, Du B, Ding EX, Wang J, Lu Z, Sun B, Wang J, Liu J (2016) A timesaving low-cost, high-yield method for the synthesis of ultrasmall uniform graphene oxide nanosheets and their application in surfactants. Nanotechnology 27:055601
Markus AA, Parsons JR, Roex EW, de Voogt P, Laane RW (2015) Modeling aggregation and sedimentation of nanoparticles in the aquatic environment. Sci Total Environ 506−507:323–329
Qi XD, Zhou TN, Deng S, Zong GY, Yao XL, Fu Q (2014) Size-specified graphene oxide sheets: Ultrasonication assisted preparation and characterization. J Mater Sci 49:1785–1793
Quik JTK, Stuart MC, Wouterse M, Peijnenburg W, Hendriks AJ, van de Meent D (2012) Natural colloids are the dominant factor in the sedimentation of nanoparticles. Environ Toxicol Chem 31:1019–1022
Sager TM, Porter DW, Robinson VA, Linsley WG, Schwegler-berry DE, Castranova V (2007) Improved method to disperse nanoparticles for in vitro and in vivo investigation of toxicity. Nanotoxicology 1:118–129
Satapathy MK, Chiang WH, Chuang EY, Chen CH, Liao JL, Huang HN (2017) Microplasma-assisted hydrogel fabrication: a novel method for gelatin-graphene oxide nano composite hydrogel synthesis for biomedical application. PeerJ 5:e3498
Singh DP, Herrera CE, Singh B, Singh S, Singh RK, Kumar R (2018) Graphene oxide: an efficient material and recent approach for biotechnological and biomedical applications. Mater Sci Eng C 86:173–197
Su Y, Yang GQ, Lu K, Petersen EJ, Mao L (2017) Colloidal properties and stability of aqueous suspensions of few-layer graphene: importance of graphene concentration. Environ Pollut 220:469–477
Sun X, Luo D, Liu J, Evans DG (2010) Monodisperse chemically modified graphene obtained by density gradient ultracentrifugal rate separation. ACS Nano 4:3381–3389
Wang X, Bai H, Shi G (2011) Size fractionation of graphene oxide sheets by pH-assisted selective sedimentation. J Am Chem Soc 133:6338–6342
Wang J, Chen ZM, Chen BL (2014) Adsorption of polycyclic aromatic hydrocarbons by graphene and graphene oxide nanosheets. Environ Sci Technol 48:4817–4825
Wu L, Liu L, Gao B, Muñoz-Carpena R, Zhang M, Chen H, Zhou Z, Wang H (2013) Aggregation kinetics of graphene oxides in aqueous solutions: experiments, mechanisms, and modeling. Langmuir 29:15174–15181
Xu PC, Xu T, Yu HT, Li XX (2016) Graphene-oxide (GO) nano-sheets: lateral and vertical size-effects on chemical-gas sensitivity enhancement. IEEE 29th International Conference on Micro Electro Mechanical Systems (MEMS): Shanghai, China, 535–538
Yadav SK, Kumar R, Sundramoorthy AK, Singh RK, Koo CM (2016) Simultaneous reduction and covalent grafting of polythiophene on graphene oxide sheets for excellent capacitance retention. RSC Adv 6:52945–52949
Yang YK, Nakada N, Nakajima R, Yasojima M, Wang C, Tanaka H (2013) pH, ionic strength and dissolved organic matter alter aggregation of fullerene C60 nanoparticles suspensions in wastewater. J Hazard Mater 244–245:582–587
Yang KJ, Chen BL, Zhu XY, Xing BS (2016) Aggregation, adsorption, and morphological transformation of graphene oxide in aqueous solutions containing different metal cations. Environ Sci Technol 50:11066–11075
Yousefi N, Gudarzi MM, Zheng Q, Aboutalebi SH, Sharif F, Kim JK (2012) Self-alignment and high electrical conductivity of ultralarge graphene oxide-polyurethane nanocomposites. J Mater Chem 22:12709–12717
Zhao GX, Li JX, Ren XM, Chen CL, Wang XK (2011) Few-layered graphene oxide nanosheets as superior sorbents for heavy metal ion pollution management. Environ Sci Technol 45:10454–10462
Zhang H, Peng C, Yang JZ, Lv M, Liu R, He DN, Fan CH, Huang Q (2013) Uniform ultrasmall graphene oxide nanosheets with low cytotoxicity and high cellular uptake. ACS Appl Mater Interfaces 5:1761–1767
Zhang LM, Xia JG, Zhao QH, Liu LW, Zhang ZJ (2010) Functional graphene oxide as a nanocarrier for controlled loading and targeted delivery of mixed anticancer drugs. Small 6:537–544
Funding
This work is financially supported by the National Natural Science Foundation of China (51479016), the Startup Foundation for Doctoral Scientific Research of Liaoning Province (20170520368), and the Natural Science Foundation of Liaoning Province (20180510004).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Rights and permissions
About this article
Cite this article
Ding, G., Zhang, N., Wang, C. et al. Effect of the size on the aggregation and sedimentation of graphene oxide in seawaters with different salinities. J Nanopart Res 20, 313 (2018). https://doi.org/10.1007/s11051-018-4421-1
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11051-018-4421-1