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Title: Source Signatures of Fine Particulate Matter from Petroleum Refining and Fuel Use

Abstract

Combustion experiments were carried out on four different residual fuel oils in a 732 kW boiler. Particulate matter (PM) emission samples were separated aerodynamically by a cyclone into fractions that were nominally less than and greater than 2.5 microns in diameter. However, examination of several of the samples by computer-controlled scanning electron microscopy (CCSEM) revealed that part of the <2.5 micron fraction (PM{sub 2.5}) in fact consists of carbonaceous cenospheres and vesicular particles that range up to 10 microns in diameter. X-ray absorption fine structure (XAFS) spectroscopy data were obtained at the S, V, Ni, Fe, Cu, Zn, and As Kedges, and at the Pb L-edge. Deconvolution of the x-ray absorption near edge structure (XANES) region of the S spectra established that the dominant molecular forms of S present were sulfate (26-84% of total S) and thiophene (13-39% of total S). Sulfate was greater in the PM{sub 2.5} samples than in the >2.5 micron samples (PM{sub 2.5+}). Inorganic sulfides and elemental sulfur were present in lower percentages. The Ni XANES spectra from all of the samples agree fairly well with that of NiSO4, while most of the V spectra closely resemble that of vanadyl sulfate (VO{center_dot}SO{sub 4}{center_dot}xH{sub 2}O). The othermore » metals investigated (Fe, Cu, Zn, and Pb) were also present predominantly as sulfates. Arsenic is present as an arsenate (As{sup +5}). X-ray diffraction patterns of the PM{sub 2.5} fraction exhibit sharp lines due to sulfate compounds (Zn, V, Ni, Ca, etc.) superimposed on broad peaks due to amorphous carbons. All of the samples contain a significant organic component, with the LOI ranging from 64 to 87 % for the PM{sub 2.5} fraction and from 88 to 97% for the PM{sub 2.5+} fraction. {sup 13}C nuclear magnetic resonance (NMR) analysis indicates that the carbon is predominantly condensed in graphitic structures. Aliphatic structure was detected in only one of seven samples examined.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Consortium For Fossil Fuel Liq
Sponsoring Org.:
USDOE
OSTI Identifier:
896538
DOE Contract Number:  
AC26-99BC15220
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
02 PETROLEUM; FINE STRUCTURE; NUCLEAR MAGNETIC RESONANCE; PARTICULATES; PETROLEUM; REFINING; RESIDUAL FUELS; SCANNING ELECTRON MICROSCOPY; SPECTRA; X-RAY DIFFRACTION

Citation Formats

Huffman, Gerald P, Huggins, Frank E, Shah, Naresh, and Huggins, Robert. Source Signatures of Fine Particulate Matter from Petroleum Refining and Fuel Use. United States: N. p., 1999. Web. doi:10.2172/896538.
Huffman, Gerald P, Huggins, Frank E, Shah, Naresh, & Huggins, Robert. Source Signatures of Fine Particulate Matter from Petroleum Refining and Fuel Use. United States. doi:10.2172/896538.
Huffman, Gerald P, Huggins, Frank E, Shah, Naresh, and Huggins, Robert. Fri . "Source Signatures of Fine Particulate Matter from Petroleum Refining and Fuel Use". United States. doi:10.2172/896538. https://www.osti.gov/servlets/purl/896538.
@article{osti_896538,
title = {Source Signatures of Fine Particulate Matter from Petroleum Refining and Fuel Use},
author = {Huffman, Gerald P and Huggins, Frank E and Shah, Naresh and Huggins, Robert},
abstractNote = {Combustion experiments were carried out on four different residual fuel oils in a 732 kW boiler. Particulate matter (PM) emission samples were separated aerodynamically by a cyclone into fractions that were nominally less than and greater than 2.5 microns in diameter. However, examination of several of the samples by computer-controlled scanning electron microscopy (CCSEM) revealed that part of the <2.5 micron fraction (PM{sub 2.5}) in fact consists of carbonaceous cenospheres and vesicular particles that range up to 10 microns in diameter. X-ray absorption fine structure (XAFS) spectroscopy data were obtained at the S, V, Ni, Fe, Cu, Zn, and As Kedges, and at the Pb L-edge. Deconvolution of the x-ray absorption near edge structure (XANES) region of the S spectra established that the dominant molecular forms of S present were sulfate (26-84% of total S) and thiophene (13-39% of total S). Sulfate was greater in the PM{sub 2.5} samples than in the >2.5 micron samples (PM{sub 2.5+}). Inorganic sulfides and elemental sulfur were present in lower percentages. The Ni XANES spectra from all of the samples agree fairly well with that of NiSO4, while most of the V spectra closely resemble that of vanadyl sulfate (VO{center_dot}SO{sub 4}{center_dot}xH{sub 2}O). The other metals investigated (Fe, Cu, Zn, and Pb) were also present predominantly as sulfates. Arsenic is present as an arsenate (As{sup +5}). X-ray diffraction patterns of the PM{sub 2.5} fraction exhibit sharp lines due to sulfate compounds (Zn, V, Ni, Ca, etc.) superimposed on broad peaks due to amorphous carbons. All of the samples contain a significant organic component, with the LOI ranging from 64 to 87 % for the PM{sub 2.5} fraction and from 88 to 97% for the PM{sub 2.5+} fraction. {sup 13}C nuclear magnetic resonance (NMR) analysis indicates that the carbon is predominantly condensed in graphitic structures. Aliphatic structure was detected in only one of seven samples examined.},
doi = {10.2172/896538},
journal = {},
number = ,
volume = ,
place = {United States},
year = {1999},
month = {12}
}