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Title: XAFS Studies of Nickel and Sulfur Speciation in Residual Oil Fly-Ash Particulate Matters (ROFA PM)

Authors:
; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org.:
Doe - Office Of Science
OSTI Identifier:
930314
Report Number(s):
BNL-81024-2008-JA
DOE Contract Number:
DE-AC02-98CH10886
Resource Type:
Journal Article
Resource Relation:
Journal Name: Environmental Science and Technology; Journal Volume: 41
Country of Publication:
United States
Language:
English
Subject:
national synchrotron light source

Citation Formats

Pattanaik,S., Huggins, F., Huffman, G., Linak, W., and Miller, C.. XAFS Studies of Nickel and Sulfur Speciation in Residual Oil Fly-Ash Particulate Matters (ROFA PM). United States: N. p., 2007. Web. doi:10.1021/es061635m.
Pattanaik,S., Huggins, F., Huffman, G., Linak, W., & Miller, C.. XAFS Studies of Nickel and Sulfur Speciation in Residual Oil Fly-Ash Particulate Matters (ROFA PM). United States. doi:10.1021/es061635m.
Pattanaik,S., Huggins, F., Huffman, G., Linak, W., and Miller, C.. Mon . "XAFS Studies of Nickel and Sulfur Speciation in Residual Oil Fly-Ash Particulate Matters (ROFA PM)". United States. doi:10.1021/es061635m.
@article{osti_930314,
title = {XAFS Studies of Nickel and Sulfur Speciation in Residual Oil Fly-Ash Particulate Matters (ROFA PM)},
author = {Pattanaik,S. and Huggins, F. and Huffman, G. and Linak, W. and Miller, C.},
abstractNote = {},
doi = {10.1021/es061635m},
journal = {Environmental Science and Technology},
number = ,
volume = 41,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}
  • XAFS spectroscopy has been employed to evaluate the effect of fuel compositions and combustion conditions on the amount, form, and distribution of sulfur and nickel in size-fractionated ROFA PM. Analysis of S K-edge XANES establish that sulfate is abundant in all PM. However, depending upon the combustion conditions, lesser amounts of thiophenic sulfur, metal sulfide, and elemental sulfur may also be observed. Least-squares fitting of Ni K-edge XANES reveals that most of the nickel in PM is present as bioavailable NiSO{sub 4}.nH{sub 2}O. The insoluble Ni mainly exists as a minor species, as nickel ferrite in PM{sub 2.5} (PM <more » 2.5 {micro}m) and nickel sulfide, NixSy in PM{sub 2.5+} (PM > 2.5 {micro}m). The Ni K-edge XANES results are in agreement with the EXAFS data. Such detailed speciation of Ni and S in PM is needed for determining their mobility, bioavailability, and reactivity, and hence, their role in PM toxicity. This information is also important for understanding the mechanism of PM formation, developing effective remediation measures, and providing criteria for identification of potential emission sources. Transition metals complexing with sulfur is ubiquitous in nature. Therefore, this information on metal sulfur complex can be critical to a large body of environmental literature.« less
  • Representative duplicate fly ash samples were obtained from the stacks of 400- and 385-MW utility boilers (Unit A and Unit B, respectively) using a modified U.S. Environmental Protection Agency (EPA) Method 17 sampling train assembly as they burned 0.9 and 0.3 wt % S residual (No. 6 fuel) oils, respectively, during routine power plant operations. Residual oil fly ash (ROFA) samples were analyzed for Ni concentrations and speciation using inductively coupled plasma-atomic emission spectroscopy, X-ray absorption fine structure (XAFS) spectroscopy, and X-ray diffraction.
  • Identification of constituents responsible for the pulmonary toxicity of fugitive combustion emission source particles may provide insight into the adverse health effects associated with exposure to these particles as well as ambient air particulate pollution. Herein, we describe results of studies conducted to identify constituents responsible for the acute lung injury induced by residual oil fly ash (ROFA) and to assess physical-chemical factors that influence the pulmonary toxicity of these constituents. Biochemical and cellular analyses performed on bronchoalveolar lavage fluid obtained from rats following intratracheal instillation of ROFA suspension demonstrated the presence of severe inflammation, an indicator of pulmonary injury,more » which included recruitment of neutrophils, eosinophils, and monocytes into the airway. A leachate prepared from ROFA, containing predominantly Fe, Ni, V, Ca, Mg, and sulfate, produced similar lung injury to that induced by ROFA suspension. Depletion of Fe, Ni, and V from the ROFA leachate abrogated its pulmonary toxicity. Correspondingly, minimal lung injury was observed in animals exposed to saline-washed rifa particles. A surrogate transition metal sulfate solution containing Fe, V, and Ni largely reproduced the lung injury induced by ROFA. Metal interactions and pH were found to influence the severity and kinetics of lung injury induced by ROFA and soluble transition metals. These findings provide direct evidence for the role of soluble transition metals in the pulmonary injury induced by the combustion emission source particulate, ROFA. 44 refs., 5 figs., 3 tabs.« less