Partitioning of metal species during an enriched fuel combustion experiment

Speciation in the gaseous and particulate phases

M P Pavageau, A Morin, F Seby, C Guimon, Eva Maria Krupp, C Pecheyran, J Poulleau, O F X Donard

Research output: Contribution to journalArticle

25 Citations (Scopus)

Abstract

Combustion processes are the most important source of metal in the atmosphere and need to be better understood to improve flue gas treatment and health impact studies. This combustion experiment was designed to study metal partitioning and metal speciation in the gaseous and particulate phases. A light fuel oil was enriched with 15 organometallic compounds of the following elements: Pb, Hg, As, Cu, Zn, Cd, Se, Sn, Mn, V, TI, Ni, Co, Cr, and Sb. The resulting mixture was burnt in a pilot-scale fuel combustion boiler under controlled conditions. After filtration of the particles, the gaseous species were sampled in the stack through a heated sampling tube simultaneously by standardized washing bottles-based sampling techniques and cryogenically. The cryogenic samples were collected at -80 degreesC for further speciation analysis by LT/GC-ICPMS. Three species of selenium and two of mercury were evidenced as volatile species in the flue gas. Thermodynamic predictions and experiments suggest the following volatile metal species to be present in the flue gas: H2Se, CSSe, CSe2, SeCl2, Hg-0, and HgCl2. Quantification of volatile metal species in comparison between cryogenic techniques and the washing bottles-based sampling method is also discussed. Concerning metal partitioning, the results indicated that under these conditions, at least 60% (by weight) of the elements Pb, Sn, Cu, Co, TI, Mn, V, Cr, Ni, Zn, Cd, and Sb mixed to the fuel were found in the particulate matter. For As and Se, 37 and 17%, respectively, were detected in the particles, and no particulate mercury was found. Direct metal speciation in particles was performed by XPS allowing the determination of the oxidation state of the following elements: Sb(V), TI(III), Mn(IV), Cd(II), Zn(II), Cr(III), Ni(II), CO(II), V(V), and Cu(II). Water soluble species of inorganic Cr, As, and Se in particulate matter were determined by HPLC/ICP-MS and identified in the oxidation state Cr(III), As(V), and Se(IV).

Original languageEnglish
Pages (from-to)2252-2263
Number of pages12
JournalEnvironmental Science & Technology
Volume38
Issue number7
DOIs
Publication statusPublished - 1 Apr 2004

Keywords

  • plasma-mass spectrometry
  • municipal solid-waste
  • fired power-plant
  • coal combustion
  • trace elements
  • volatile metal
  • flue-gas
  • pulverized coal
  • chemical speciation
  • mercury speciation

Cite this

Partitioning of metal species during an enriched fuel combustion experiment : Speciation in the gaseous and particulate phases. / Pavageau, M P ; Morin, A ; Seby, F ; Guimon, C ; Krupp, Eva Maria; Pecheyran, C ; Poulleau, J ; Donard, O F X .

In: Environmental Science & Technology, Vol. 38, No. 7, 01.04.2004, p. 2252-2263.

Research output: Contribution to journalArticle

Pavageau, M P ; Morin, A ; Seby, F ; Guimon, C ; Krupp, Eva Maria ; Pecheyran, C ; Poulleau, J ; Donard, O F X . / Partitioning of metal species during an enriched fuel combustion experiment : Speciation in the gaseous and particulate phases. In: Environmental Science & Technology. 2004 ; Vol. 38, No. 7. pp. 2252-2263.
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T1 - Partitioning of metal species during an enriched fuel combustion experiment

T2 - Speciation in the gaseous and particulate phases

AU - Pavageau, M P

AU - Morin, A

AU - Seby, F

AU - Guimon, C

AU - Krupp, Eva Maria

AU - Pecheyran, C

AU - Poulleau, J

AU - Donard, O F X

PY - 2004/4/1

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N2 - Combustion processes are the most important source of metal in the atmosphere and need to be better understood to improve flue gas treatment and health impact studies. This combustion experiment was designed to study metal partitioning and metal speciation in the gaseous and particulate phases. A light fuel oil was enriched with 15 organometallic compounds of the following elements: Pb, Hg, As, Cu, Zn, Cd, Se, Sn, Mn, V, TI, Ni, Co, Cr, and Sb. The resulting mixture was burnt in a pilot-scale fuel combustion boiler under controlled conditions. After filtration of the particles, the gaseous species were sampled in the stack through a heated sampling tube simultaneously by standardized washing bottles-based sampling techniques and cryogenically. The cryogenic samples were collected at -80 degreesC for further speciation analysis by LT/GC-ICPMS. Three species of selenium and two of mercury were evidenced as volatile species in the flue gas. Thermodynamic predictions and experiments suggest the following volatile metal species to be present in the flue gas: H2Se, CSSe, CSe2, SeCl2, Hg-0, and HgCl2. Quantification of volatile metal species in comparison between cryogenic techniques and the washing bottles-based sampling method is also discussed. Concerning metal partitioning, the results indicated that under these conditions, at least 60% (by weight) of the elements Pb, Sn, Cu, Co, TI, Mn, V, Cr, Ni, Zn, Cd, and Sb mixed to the fuel were found in the particulate matter. For As and Se, 37 and 17%, respectively, were detected in the particles, and no particulate mercury was found. Direct metal speciation in particles was performed by XPS allowing the determination of the oxidation state of the following elements: Sb(V), TI(III), Mn(IV), Cd(II), Zn(II), Cr(III), Ni(II), CO(II), V(V), and Cu(II). Water soluble species of inorganic Cr, As, and Se in particulate matter were determined by HPLC/ICP-MS and identified in the oxidation state Cr(III), As(V), and Se(IV).

AB - Combustion processes are the most important source of metal in the atmosphere and need to be better understood to improve flue gas treatment and health impact studies. This combustion experiment was designed to study metal partitioning and metal speciation in the gaseous and particulate phases. A light fuel oil was enriched with 15 organometallic compounds of the following elements: Pb, Hg, As, Cu, Zn, Cd, Se, Sn, Mn, V, TI, Ni, Co, Cr, and Sb. The resulting mixture was burnt in a pilot-scale fuel combustion boiler under controlled conditions. After filtration of the particles, the gaseous species were sampled in the stack through a heated sampling tube simultaneously by standardized washing bottles-based sampling techniques and cryogenically. The cryogenic samples were collected at -80 degreesC for further speciation analysis by LT/GC-ICPMS. Three species of selenium and two of mercury were evidenced as volatile species in the flue gas. Thermodynamic predictions and experiments suggest the following volatile metal species to be present in the flue gas: H2Se, CSSe, CSe2, SeCl2, Hg-0, and HgCl2. Quantification of volatile metal species in comparison between cryogenic techniques and the washing bottles-based sampling method is also discussed. Concerning metal partitioning, the results indicated that under these conditions, at least 60% (by weight) of the elements Pb, Sn, Cu, Co, TI, Mn, V, Cr, Ni, Zn, Cd, and Sb mixed to the fuel were found in the particulate matter. For As and Se, 37 and 17%, respectively, were detected in the particles, and no particulate mercury was found. Direct metal speciation in particles was performed by XPS allowing the determination of the oxidation state of the following elements: Sb(V), TI(III), Mn(IV), Cd(II), Zn(II), Cr(III), Ni(II), CO(II), V(V), and Cu(II). Water soluble species of inorganic Cr, As, and Se in particulate matter were determined by HPLC/ICP-MS and identified in the oxidation state Cr(III), As(V), and Se(IV).

KW - plasma-mass spectrometry

KW - municipal solid-waste

KW - fired power-plant

KW - coal combustion

KW - trace elements

KW - volatile metal

KW - flue-gas

KW - pulverized coal

KW - chemical speciation

KW - mercury speciation

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DO - 10.1021/es034408i

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VL - 38

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JO - Environmental Science & Technology

JF - Environmental Science & Technology

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