Flyash carbon constitutes the char particles that are left in flyash after the incomplete combustion of coal in the furnace, rendering flyash above spec for ASTM C618 applications for cement. A beneficiation process allows the selective separation of unburned carbon from flyash to be used for upgrading into a higher value product. Flyash carton is composed of several microscopically distinguishable types; inertinite is relatively unreactive in the thermal processing of coal and occurs essentially unaltered in the flyash while {open_quotes}coke{close_quotes} is produced from the melting, devolatilization, swelling and resolidification of the reactive macerals vitrinite and liptinite. The porosity, surface area, and surface chemistry of flyash carbons are characterized using mercury porosimetry, BET analysis, and vapor- and liquid-phase adsorption of various organic compounds. Results suggest that different carbon forms in flyash affect the degree of adsorption of phenols as will as other hydrocarbon pollutants onto the flyash carbon. A comparison of adsorptability of the flyash carbon compared to commercially available active carbons are discussed.
Engineered nanoscale ceria is used as a diesel fuel catalyst. Little is known about its mammalian central nervous system effects. The objective of this paper is to characterize the biodistribution of a 5-nm citrate-stabilized ceria dispersion from blood into brain and its pro- or antioxidant effects. An ∼4% aqueous ceria dispersion was iv infused into rats (0, 100, and up to 250 mg/kg), which were terminated after 1 or 20 h. Ceria concentration, localization, and chemical speciation in the brain were assessed by inductively coupled plasma mass spectrometry, light and electron microscopy (EM), and electron energy loss spectroscopy (EELS). Pro- or antioxidative stress effects were assessed as protein carbonyls, 3-nitrotyrosine, and protein-bound 4-hydroxy-2-trans-nonenal in hippocampus, cortex, and cerebellum. Glutathione reductase, glutathione peroxidase, manganese superoxide dismutase, and catalase levels and activities were measured in hippocampus. Catalase levels and activities were also measured in cortex and cerebellum. Na fluorescein and horseradish peroxidase (HRP) were given iv as blood-brain barrier (BBB) integrity markers. Mortality was seen after administration of 175–250 mg ceria/kg. Twenty hours after infusion of 100 mg ceria/kg, brain HRP was marginally elevated. EM and EELS revealed mixed Ce(III) and Ce(IV) valence in the freshly synthesized ceria in vitro and in ceria agglomerates in the brain vascular compartment. Ceria was not seen in microvascular endothelial or brain cells. Ceria elevated catalase levels at 1 h and increased catalase activity at 20 h in hippocampus and decreased catalase activity at 1 h in cerebellum. Compared with a previously studied ∼30-nm ceria, this ceria was more toxic, was not seen in the brain, and produced little oxidative stress effect to the hippocampus and cerebellum. The results are contrary to the hypothesis that a smaller engineered nanomaterial would more readily permeate the BBB.
Oxidation of nitric oxide (NO) for subsequent efficient reduction in selective catalytic reduction or lean NO(x) trap devices continues to be a challenge in diesel engines because of the low efficiency and high cost of the currently used platinum (Pt)-based catalysts. We show that mixed-phase oxide materials based on Mn-mullite (Sm, Gd)Mn(2)O(5) are an efficient substitute for the current commercial Pt-based catalysts. Under laboratory-simulated diesel exhaust conditions, this mixed-phase oxide material was superior to Pt in terms of cost, thermal durability, and catalytic activity for NO oxidation. This oxide material is active at temperatures as low as 120°C with conversion maxima of ~45% higher than that achieved with Pt. Density functional theory and diffuse reflectance infrared Fourier transform spectroscopy provide insights into the NO-to-NO(2) reaction mechanism on catalytically active Mn-Mn sites via the intermediate nitrate species.
A combination of high-resolution transmission electron microscopy, scanning transmission electron microscopy, and electron energy-loss spectroscopy (HRTEM-STEM-EELS) was used to study fly ashes produced from the combustion of an eastern Kentucky coal at a southeastern-Kentucky wall-fired pulverized coal utility boiler. Fly ash was collected from individual hoppers in each row of the electrostatic precipitators (ESP) pollution-control system, with multiple hoppers sampled within each of the three rows. Temperatures within the ESP array range from about 200 degrees C at the entry to the first row to < 150 degrees C at the exit of the third row. HRTEM-STEM-EELS study demonstrated the presence of nanoscale (10 s nm) C agglomerates with typical soot-like appearance and others with graphitic fullerene-like nanocarbon structures. The minute carbon agglomerates are typically juxtaposed and intergrown with slightly larger aluminosilicate spheres and often form an ultrathin halo or deposit on the fly ash particles. The STEM-EELS analyses revealed that the nanocarbon agglomerates host even finer (< 3 nm) metal and metal oxide particles. Elemental analysis indicated an association of Hg with the nanocarbon. Arsenic, Se, Pb, Co, and traces of Ti and Ba are often associated with Fe-rich particles within the nanocarbon deposits.
Framboids are spherical, raspberry-like aggregates of pyrite which are typically associated with organic matter in black shales. Because framboids are often intimately intergrown with macerals of the kerogen in black shales the objectives of this study were to: (1) Select tramboidal pyrite with close spatial relationship to distinct maceral types; (2) Determine the trace-element variations within different maceral types and that of framboidal pyrite occurring adjacent to those macerals and; (3) Examine whether the S/Fe ratios of the tramboids vary based on different maceral-type association. This study investigates a Devonian-Mississippian black shale from East-Central Kentucky. The organic-rich matrix consists predominantly of bituminite, alginite and to lesser extent of vitrinite. Most framboids range between < 1[mu]m and 27 [mu]m in size and typically occur as clusters which are engulfed by lamellar flowing vitrinite, indicating that the framboids were already present before compaction. 161 PIXE-analyses were performed in both macerals and framboids. To understand the likelihood of framboid precursors in macerals the authors checked the constancy of the S, Fe and trace-element content in the immediate vicinity of the framboid particle. Moreover, the authors analyzed traverses through framboids associated with the three different maceral types. The S/Fe ratio of the framboids ismore » always that of stoichiometric pyrite. The combined results suggest that the framboids may have formed independent of the sulfur and trace-element concentration among the macerals. Globular, partly translucent grains were observed to have great resemblances in size and trace-element contents compared to those of framboids. The S/Fe ratio of these grains was typically well in excess of 2.0 suggesting that the transparent matrix may have been a sulfur-rich phase that possibly serves as precursor for the framboids.« less
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