Environmental fate and impacts of graphene oxide (GO) nanoparticles are strongly influenced by their subsurface behaviors. The present work examined the aggregation and transport behaviors of GO in saturated sand columns under different temperature (6 and 24 °C), surfactant concentration (0.04% and 0.4%), cation valence, and electrolyte concentration conditions. In monovalent electrolyte (NaCl), although the presence of cationic surfactant (CTAB) notably increased GO stability and mobility, GO ripening happened due to their concurrent aggregation and transport in the columns. GO particles were more mobile at a lower temperature probably because the CTAB coating of GO increased with decreasing temperature, leading to stronger electrostatic repulsion. Furthermore, GO retention in the media increased with the increase of NaCl concentration due to the enhanced compression of the electric double layer. In multivalent electrolyte (CaCl2 or AlCl3), the presence of CTAB greatly improved GO stability and mobility and no deposition occurred in saturated porous media under all the tested conditions. This is because the CTAB coating of GO diminished the cation bridging effects in both GO-GO and GO-sand systems. Results from extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) theory considering steric repulsion suggest that secondary minimum aggregation and depositions were the main mechanisms of GO retention transport in monovalent electrolyte in saturated porous media.
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Adak, A., Bandyopadhyay, M., & Pal, A. (2005). Removal of anionic surfactant from wastewater by alumina: a case study. Colloids and Surfaces a-Physicochemical and Engineering Aspects, 254, 165–171.
Akhavan, O., Ghaderi, E., Hashemi, E., & Akbari, E. (2015). Dose-dependent effects of nanoscale graphene oxide on reproduction capability of mammals. Carbon, 95, 309–317.
Al Mahrouqi, D., Vinogradov, J., & Jackson, M. D. (2016). Temperature dependence of the zeta potential in intact natural carbonates. Geophysical Research Letters, 43, 11578–11587.
Albers, W., & Overbeek, J. T. G. (1959). Stability of emulsions of water in oil: I. the correlation between electrokinetic potential and stability. Journal of Colloid Science, 14, 501–509.
Alkan, M., Karadas, M., Dogan, M., & Demirbas, O. (2005). Adsorption of CTAB onto perlite samples from aqueous solutions. Journal of Colloid and Interface Science, 291, 309–318.
Bodznick, D. (1978). Calcium ion: an odorant for natural water discriminations and the migratory behavior of sockeye salmon. Journal of Comparative Physiology, 127, 157–166.
Bouchard, D., Zhang, W., Powell, T., & Rattanaudompol, U. S. (2012). Aggregation kinetics and transport of single-walled carbon nanotubes at low surfactant concentrations. Environmental Science & Technology, 46, 4458–4465.
Chen, D., Feng, H. B., & Li, J. H. (2012). Graphene oxide: preparation, functionalization, and electrochemical applications. Chemical Reviews, 112, 6027–6053.
Chen, C., Shang, J. Y., Zheng, X. L., Zhao, K., Yan, C. R., Sharma, P., et al. (2018). Effect of physicochemical factors on transport and retention of graphene oxide in saturated media. Environmental Pollution, 236, 168–176.
Clemente, Z., Castro, V. L. S. S., Franqui, L. S., Silva, C. A., & Martinez, D. S. T. (2017). Nanotoxicity of graphene oxide: assessing the influence of oxidation debris in the presence of humic acid. Environmental Pollution, 225, 118–128.
de la Cruz, E. F., Zheng, Y. D., Torres, E., Li, W., Song, W. H., & Burugapalli, K. (2012). Zeta potential of modified multi-walled carbon nanotubes in presence of poly (vinyl alcohol) hydrogel. International Journal of Electrochemical Science, 7, 3577–3590.
Dong, S. N., Sun, Y. Y., Gao, B., Shi, X. Q., Xu, H. X., Wu, J. F., et al. (2017). Retention and transport of graphene oxide in water-saturated limestone media. Chemosphere, 180, 506–512.
Duster, T. A., Na, C. Z., Bolster, D., & Fein, J. B. (2017). Transport of single-layered graphene oxide nanosheets through quartz and iron oxide-coated sand columns. Journal of Environmental Engineering, 143, 04016079.
Elimelech, M., & O’Melia, C. R. (1990). Effect of particle size on collision efficiency in the deposition of Brownian particles with electrostatic energy barriers. Langmuir, 6, 1153–1163.
Fest, E. P. M. J., Temminghoff, E. J. M., Griffioen, J., Van Der Grift, B., & Van Riemsdijk, W. H. (2007). Groundwater chemistry of Al under Dutch sandy soils: effects of land use and depth. Applied Geochemistry, 22, 1427–1438.
Furusawa, K., Sato, A., Shirai, J., & Nashima, T. (2002). Depletion flocculation of latex dispersion in ionic micellar systems. Journal of Colloid and Interface Science, 253, 273–278.
Godinez, I. G., & Darnault, C. J. (2011). Aggregation and transport of nano-TiO2 in saturated porous media: effects of pH, surfactants and flow velocity. Water Research, 45, 839–851.
Gurses, A., Yalcin, M., Sozbilir, M., & Dogar, C. (2003). The investigation of adsorption thermodynamics and mechanism of a cationic surfactant, CTAB, onto powdered active carbon. Fuel Processing Technology, 81, 57–66.
Hahn, M. W., & O’Melia, C. R. (2004). Deposition and reentrainment of Brownian particles in porous media under unfavorable chemical conditions: some concepts and applications. Environmental Science & Technology, 38, 210–220.
Hua, Z., Tang, Z., Bai, X., Zhang, J., Yu, L., & Cheng, H. (2015). Aggregation and resuspension of graphene oxide in simulated natural surface aquatic environments. Environmental Pollution, 205, 161–169.
Huysmans, M., & Dassargues, A. (2005). Review of the use of Peclet numbers to determine the relative importance of advection and diffusion in low permeability environments. Hydrogeology Journal, 13, 895–904.
Iwatsuki, T., & Yoshida, H. (1999). Groundwater chemistry and fracture mineralogy in the basement granitic rock in the Tono uranium mine area, Gifu prefecture, Japan - groundwater composition, Eh evolution analysis by fracture filling minerals. Geochemical Journal, 33, 19–32.
Kuperkar, K., Abezgauz, L., Prasad, K., & Bahadur, P. (2010). Formation and growth of micelles in dilute aqueous CTAB solutions in the presence of NaNO3 and NaClO3. Journal of Surfactants and Detergents, 13, 293–303.
Lanphere, J. D., Luth, C. J., & Walker, S. L. (2013). Effects of solution chemistry on the transport of graphene oxide in saturated porous media. Environmental Science & Technology, 47, 4255–4261.
Lanphere, J. D., Rogers, B., Luth, C., Bolster, C. H., & Walker, S. L. (2014). Stability and transport of graphene oxide nanoparticles in groundwater and surface water. Environmental Engineering Science, 31, 350–359.
Li, T., Li, Z., Zhou, J., Pan, B., Xiao, X., Guo, Z., et al. (2017). The application of graphene in biosensors. In: T. Li & Z. Liu (Eds.), Outlook and challenges of nano devices, sensors, and MEMS (pp. 299–329). Cham: Springer.
Liu, L., Gao, B., Wu, L., Morales, V. L., Yang, L., Zhou, Z., et al. (2013a). Deposition and transport of graphene oxide in saturated and unsaturated porous media. Chemical Engineering Journal, 229, 444–449.
Liu, L., Gao, B., Wu, L., Yang, L. Y., Zhou, Z. H., & Wang, H. (2013b). Effects of pH and surface metal oxyhydroxides on deposition and transport of carboxyl-functionalized graphene in saturated porous media. Journal of Nanoparticle Research, 15, 2079.
Liu, L., Gao, B., Wu, L., Sun, Y. Y., & Zhou, Z. H. (2015). Effects of surfactant type and concentration on graphene retention and transport in saturated porous media. Chemical Engineering Journal, 262, 1187–1191.
Lu, Y., Yang, K., & Lin, D. (2014). Transport of surfactant-facilitated multiwalled carbon nanotube suspensions in columns packed with sized soil particles. Environmental Pollution, 192, 36–43.
Marsalek, R., Pospisil, J., & Taraba, B. (2011). The influence of temperature on the adsorption of CTAB on coals. Colloids and Surfaces a-Physicochemical and Engineering Aspects, 383, 80–85.
Mayora-Curzio, C. A., Cremades-Oliver, L. V., & Cusido-Fabregas, J. A. (2015). Graphene. Part II: processes and feasibility of its production. DYNA, 90, 344–347.
Morales, V. L., Zhang, W., Gao, B., Lion, L. W., Bisogni, J. J., McDonough, B. A., et al. (2011). Impact of dissolved organic matter on colloid transport in the vadose zone: deterministic approximation of transport deposition coefficients from polymeric coating characteristics. Water Research, 45, 1691–1701.
Naghizadeh, A., Nasseri, S., Rashidi, A. M., Kalantary, R. R., Nabizadeh, R., & Mahvi, A. H. (2013). Adsorption kinetics and thermodynamics of hydrophobic natural organic matter (NOM) removal from aqueous solution by multi-wall carbon nanotubes. Water Science and Technology Water Supply, 13, 273–285.
Nogueira, P. F. M., Nakabayashi, D., & Zucolotto, V. (2015). The effects of graphene oxide on green algae Raphidocelis subcapitata. Aquatic Toxicology, 166, 29–35.
Peng, S. N., Wu, D., Ge, Z., Tong, M. P., & Kim, H. J. (2017). Influence of graphene oxide on the transport and deposition behaviors of colloids in saturated porous media. Environmental Pollution, 225, 141–149.
Qi, Z., Hou, L., Zhu, D., Ji, R., & Chen, W. (2014). Enhanced transport of phenanthrene and 1-naphthol by colloidal graphene oxide nanoparticles in saturated soil. Environmental Science & Technology, 48, 10136–10144.
Sophia, A. C., Lima, E. C., Allaudeen, N., & Rajan, S. (2016). Application of graphene based materials for adsorption of pharmaceutical traces from water and wastewater: a review. Desalination and Water Treatment, 57, 27573–27586.
Sun, L., & Fugetsu, B. (2013). Mass production of graphene oxide from expanded graphite. Materials Letters, 109, 207–210.
Sun, Y. Y., Gao, B., Bradford, S. A., Wu, L., Chen, H., Shi, X. Q., et al. (2015). Transport, retention, and size perturbation of graphene oxide in saturated porous media: effects of input concentration and grain size. Water Research, 68, 24–33.
Tardani, F., & La Mesa, C. (2014). Attempts to control depletion in the surfactant-assisted stabilization of single-walled carbon nanotubes. Colloids and Surfaces a-Physicochemical and Engineering Aspects, 443, 123–128.
Tian, Y. A., Gao, B., Silvera-Batista, C., & Ziegler, K. J. (2010). Transport of engineered nanoparticles in saturated porous media. Journal of Nanoparticle Research, 12, 2371–2380.
Tian, Y., Gao, B., & Ziegler, K. J. (2011). High mobility of SDBS-dispersed single-walled carbon nanotubes in saturated and unsaturated porous media. Journal of Hazardous Materials, 186, 1766–1772.
Tian, Y., Gao, B., Morales, V. L., Wang, Y., & Wu, L. (2012). Effect of surface modification on single-walled carbon nanotube retention and transport in saturated and unsaturated porous media. Journal of Hazardous Materials, 239, 333–339.
Vinogradov, J., & Jackson, M. D. (2015). Zeta potential in intact natural sandstones at elevated temperatures. Geophysical Research Letters, 42, 6287–6294.
Wang, Y., Gao, B., Morales, V. L., Tian, Y., Wu, L., Gao, J., et al. (2012). Transport of titanium dioxide nanoparticles in saturated porous media under various solution chemistry conditions. Journal of Nanoparticle Research, 14, 1095.
Wang, D., Su, C., Liu, C., & Zhou, D. (2014). Transport of fluorescently labeled hydroxyapatite nanoparticles in saturated granular media at environmentally relevant concentrations of surfactants. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 457, 58–66.
Wang, M., Gao, B., & Tang, D. S. (2016). Review of key factors controlling engineered nanoparticle transport in porous media. Journal of Hazardous Materials, 318, 233–246.
Wang, M., Gao, B., Tang, D. S., Sun, H. M., Yin, X. Q., & Yu, C. R. (2017). Effects of temperature on graphene oxide deposition and transport in saturated porous media. Journal of Hazardous Materials, 331, 28–35.
Wang, M., Gao, B., Tang, D., Sun, H., Yin, X., & Yu, C. (2018a). Effects of temperature on aggregation kinetics of graphene oxide in aqueous solutions. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 538, 63–72.
Wang, M., Gao, B., Tang, D., & Yu, C. (2018b). Concurrent aggregation and transport of graphene oxide in saturated porous media: roles of temperature, cation type, and electrolyte concentration. Environmental Pollution, 235, 350–357.
Wu, L., Liu, L., Gao, B., Munoz-Carpena, R., Zhang, M., Chen, H., et al. (2013). Aggregation kinetics of graphene oxides in aqueous solutions: experiments, mechanisms, and modeling. Langmuir, 29, 15174–15181.
Xia, T. J., Qi, Y., Liu, J., Qi, Z. C., Chen, W., & Wiesner, M. R. (2017). Cation-inhibited transport of graphene oxide nanomaterials in saturated porous media: the Hofmeister effects. Environmental Science & Technology, 51, 828–837.
Zheng, D. Y., Hu, H., Liu, X. J., & Hu, S. S. (2015). Application of graphene in electrochemical sensing. Current Opinion in Colloid & Interface Science, 20, 383–405.
Zhou, X. F., & Liang, F. (2014). Application of graphene/graphene oxide in biomedicine and biotechnology. Current Medicinal Chemistry, 21, 855–869.
This work was partially supported by the National Natural Science Foundation of China (Grant No. 51509069), the Special Fund of State Key Laboratory of Hydrology-Water Resources and Hydraulic Engineering (No. 2017490811), China Postdoctoral Science Foundation, and China Scholarship Council (CSC).
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Wang, M., Yu, C., Tang, D. et al. Effects of Surfactant and Electrolyte Concentrations, Cation Valence, and Temperature on Graphene Oxide Retention and Transport in Saturated Porous Media. Water Air Soil Pollut 230, 21 (2019). https://doi.org/10.1007/s11270-018-4076-7
- Graphene oxide
- Cation valence