In this study, we correlated the deposition behavior of graphene oxide (GO) materials with their morphology and surface chemistry. GO materials with various crumpling extents (flat, wrinkled, and crumpled) and different surface chemistries (surface reduction extents) were produced using an aerosol-based method. In a furnace aerosol reactor (FuAR), flat 2D GO nanosheets were transformed into 3D wrinkled and crumpled structures via the capillary force caused by water evaporation. For all the synthesized materials, the aggregation and deposition kinetics were investigated over a wide range of monovalent and divalent cation concentrations by employing time-resolved dynamic light scattering (DLS) and a real-time quartz crystal microbalance with dissipation monitoring (QCM-D), respectively. Critical coagulation concentrations (CCC) and critical deposition concentrations (CDC) were determined for NaCl and CaCl2 electrolytes. Flat GO first turned into wrinkled and then into crumpled GO (CGO), and the corresponding CCC increased by 89% and CDC increased by 46%, indicating a weakened interaction between nanoparticles or with the microbalance sensor surfaces, caused by the crumpled morphology. In addition, for the same crumpled morphology, CCC decreased by 31% and CDC decreased by 23% with a higher degree of reduction. Based on simulations, CGO nanoparticles fit better with the DLVO model for classic 3D colloids, while the flat GO nanosheet deviated from predictions due to its ultrathin 2D structure. The release of GO was highly dependent on material properties and salt types, with the flat GO in the initial CaCl2 suspension forming the most stable layer on the silica sensor surface, due to its effective contact with the smooth shape and the bridging effect of Ca2+. Based on these aggregation, deposition, and release kinetics studies, both material morphology and surface chemistry can have significant influences on GO’s fate and transport in the environment.

Correlating material morphology and surface chemistry with the surface deposition process of graphene oxide

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.