Heteroaggregation of Graphene Oxide with Nanometer- and Micrometer-Sized Hematite Colloids: Influence on Nanohybrid Aggregation and Microparticle Sedimentation

Heteroaggregation of graphene oxide (GO) with nanometer- and micrometer-sized hematite colloids, which are naturally present in aquatic systems, is investigated in this study. The heteroaggregation rates between GO and hematite nanoparticles (HemNPs) were quantified by dynamic light scattering, while the heteroaggregation between GO and micrometer-sized hematite particles (HemMPs) was examined through batch adsorption and sedimentation experiments. The heteroaggregation rates of GO with HemNPs first increased and then decreased with increasing GO/HemNP mass concentration ratios. The conformation of GO–HemNP heteroaggregates at different GO/HemNP mass concentration ratios was observed through transmission electron microscopy imaging. Initially, GO underwent heteroaggregation with HemNPs through electrostatic attraction to form primary heteroaggregates, which were further bridged by GO to form bigger clusters. At high GO/HemNP mass concentration ratios where GO outnumbered HemNPs, heteroaggregation resulted in the formation of stable GO–HemNP nanohybrids that have a critical coagulation concentration of 308 mM NaCl at pH 5.2. In the case of HemMPs, GO adsorbed readily on the microparticles and, at an optimal GO/HemMP ratio of ∼0.002, the sedimentation of HemMPs was the fastest, most likely because of the formation of “electrostatic patches” leading to favorable aggregation of the microparticles.