Heteroaggregation of graphene oxide nanoparticles and kaolinite colloids.

Graphene oxide (GO) is a material with rapid production growth, and consequently GO nanoparticles are expected to eventually penetrate subsurface formations, where fine mineral particles are in abundance. This study examines the heteroaggregation of GO nanoparticles with kaolinite (KGa-1b) colloids under various conditions. Dynamic batch experiments were conducted in solutions with different pH values (pH=4, 7, and 10), different ionic strengths (IS=7, 12, and 27mM), and at three controlled temperatures (8, 14, and 25°C). The experimental results showed that a relatively small amount of GO nanoparticles (5-20% of the initial concentration) attached immediately onto KGa-1b colloids, and reached equilibrium in <20min. It was shown that neither temperature nor pH played a significant role in the attachment of GO nanoparticles onto KGa-1b colloids. In contrast, the attachment of GO nanoparticles onto KGa-1b colloids was shown to increase with increasing IS. Additionally, time-resolved dynamic light scattering (DLS) was used to identify the influence of IS on heteroaggregation between GO nanoparticles and KGa-1b colloids. The critical coagulation concentration (CCC) for the interaction between GO nanoparticles and KGa-1b colloids was 152mM (NaCl). The interaction energies were calculated, for all experimental conditions, by using measured zeta potentials and applying the classical DLVO theory. The equilibrium experimental data were fitted with a Freundlich isotherm, and the attachment kinetics were described very well with a pseudo-second-order model. Furthermore, thermodynamic analysis revealed that the attachment process was nonspontaneous and exothermic.

Interaction Between Graphene Oxide Nanoparticles and Quartz Sand.

In this study, the influence of pH, ionic strength (IS), and temperature on graphene oxide (GO) nanoparticles attachment onto quartz sand were investigated. Batch experiments were conducted at three controlled temperatures (4, 12, and 25 °C) in solutions with different pH values (pH 4, 7, and 10), and ionic strengths (IS = 1.4, 6.4, and 21.4 mM), under static and dynamic conditions. The surface properties of GO nanoparticles and quartz sand were evaluated by electrophoretic mobility measurements. Derjaguin-Landau-Verwey-Overbeek (DLVO) potential energy profiles were constructed for the experimental conditions, using measured zeta potentials. The experimental results showed that GO nanoparticles were very stable under the experimental conditions. Both temperature and pH did not play a significant role in the attachment of GO nanoparticles onto quartz sand. In contrast, IS was shown to influence attachment. The attachment of GO particles onto quartz sand increased significantly with increasing IS. The experimental data were fitted nicely with a Freundlich isotherm, and the attachment kinetics were satisfactorily described with a pseudo-second-order model, which implies that the quartz sand exhibited substantial surface heterogeneity and that GO retention was governed by chemisorption. Furthermore, thermodynamic analysis revealed that the attachment process was nonspontaneous and endothermic, which may be associated with structural changes of the sand surfaces due to chemisorption. Therefore, secondary minimum interaction may not be the dominant mechanism for GO attachment onto the quartz sand under the experimental conditions.