With the widespread application of fullerenes, it is critical to assess their environmental behaviors and their impacts on the transport and bioavailability of organic contaminants. The effects of fullerene particle size, chemistry of the solution, and natural organic matter on the adsorption of atrazine by aqueous dispersions of fullerenes (C60) were investigated in this work. The results showed that the Polanyi-Manes model could fit the adsorption isotherms well. Smaller sizes of fullerene particles led to increased available sites and, consequently, enhanced the adsorption of atrazine on C60. However, intensely dispersed C60 systems might not possess suitably high adsorptive capacities due to surface chemistry change. Adsorption of atrazine by aqueous dispersions of C60 increased with a decrease in the pH of the solution. Introduction of humic acid significantly reduced the size of the C60 particles, and resulted in the increase of the adsorption amount. Fullerene materials, once released into the aquatic environment, are inclined to form aqueous suspensions with different degrees of dispersion, which would greatly affect the transport and fate of organic contaminants.
Petroleum, natural gas, and natural gas condensate can contain low levels of mercury (Hg). The speciation of Hg can affect its behavior during processing, transport, and storage so efficient and safe management of Hg requires an understanding of its chemical form in oil, gas and byproducts. Here, X-ray absorption spectroscopy was used to determine the Hg speciation in samples of solid residues collected throughout the petroleum value chain including stabilized crude oil residues, sediments from separation tanks and condensate glycol dehydrators, distillation column pipe scale, and biosludge from wastewater treatment. In all samples except glycol dehydrators, metacinnabar (β-HgS) was the primary form of Hg. Electron microscopy on particles from a crude sediment showed nanosized (<100 nm) particles forming larger aggregates, and confirmed the colocalization of Hg and sulfur. In sediments from glycol dehydrators, organic Hg(SR) accounted for ∼60% of the Hg, with ∼20% present as β-HgS and/or Hg(SR) species. β-HgS was the predominant Hg species in refinery biosludge and pipe scale samples. However, the balance of Hg species present in these samples depended on the nature of the crude oil being processed, i.e. sweet (low sulfur crudes) vs sour (higher sulfur crudes). This information on Hg speciation in the petroleum value chain will inform development of better engineering controls and management practices for Hg.
Mercury (Hg) occurs as a myriad of species in environmental media, each with different physicochemical properties. The influence of Hg speciation on its transport in unsaturated soils is not well studied. Transport of four Hg species (dissolved inorganic Hg (II) species, a prepared Hg(II) and dissolved organic matter (DOM) complex, Hg(0), and HgS nanoparticles) was measured in sand and soil packed columns with partial water saturation under simulated rainfall (low ionic strength solution without DOM) and landfill leachate (high DOM content and high ionic strength) influent conditions. The Hg(II)-DOM species had the highest mobility among the four Hg species evaluated, and HgS particles (∼230 nm hydrodynamic diameter) had the poorest mobility, for all soil and influent conditions tested. The addition of 2 wt % clay particles to sand greatly retarded the transport of all Hg species, especially under simulated rainfall. DOM in the column influent facilitated the transport of all four Hg species in model and natural soils. For simulated rainfall, the transport trends observed in model sands were consistent with those measured in a sandy soil, except that the mobility of dissolved inorganic Hg(II) species was significantly lower in natural soils. For simulated rainfall, Hg transport was negligible in a high organic content (∼3.72 wt %) soil for all species except Hg-DOM. This work suggests that the Hg-DOM species presents the greatest potential for vertical migration to groundwater, especially with DOM in the influent solution.
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