TY - JOUR
T1 - Impact of fe content in laboratory-produced soot aerosol on its composition, structure, and thermo-chemical properties
AU - Bladt, Henrike
AU - Schmid, Johannes
AU - Kireeva, Elena D.
AU - Popovicheva, Olga B.
AU - Perseantseva, Natalia M.
AU - Timofeev, Mikhail A.
AU - Heister, Katja
AU - Uihlein, Johannes
AU - Ivleva, Natalia P.
AU - Niessner, Reinhard
PY - 2012/12/1
Y1 - 2012/12/1
N2 - Soot aerosol, which is a major pollutant in the atmosphere of urban areas, often contains not only carbonaceous matter but also inorganic material. These species, for example, iron compounds, originated from impurities in fuel or lubricating oil, additives or engine wear may change the physico-chemical characteristics of soot and hence its environmental impact. We studied the change of composition, structure, and oxidation reactivity of laboratory-produced soot aerosol with varying iron content. Soot types of various iron contents were generated in a propane/air diffusion flame by adjusting the doping amount of iron pentacarbonyl Fe(CO)5 to the flame. Scanning electron microscopy (SEM)/energy-dispersive X-ray spectroscopy (EDX) was combined with cluster analysis (CA) to separate individual particles into definable groups of similar chemical composition representing the particle types in dependence of the iron content in soot. Raman microspectroscopy (RM) and infrared spectroscopy were applied for the characterization of the graphitic soot structure, hydrocarbons, and iron species. For the analysis of soot reactivity, temperature-programmed oxidation (TPO) was used. It is demonstrated that iron is most dominantly present in the form of amorphous Fe (III) oxide crystallizing to hematite-Fe2O3 upon thermal treatment. Iron contaminations do not change the soot microstructure crucially, but Fe(CO)5 doping of the flame impacts hydrocarbon composition. Soot oxidation reactivity strongly depends on the iron content, as the temperature of maximum carbon (di)oxide emission Tmax follows an exponential decay with increasing iron content in soot. Based on the results of the thermo-chemical characterization of laboratory-produced internally mixed iron-containing soot, we can conclude that iron-containing combustion aerosol samples cannot be characterized unambiguously by current thermo-optical analysis protocols.
AB - Soot aerosol, which is a major pollutant in the atmosphere of urban areas, often contains not only carbonaceous matter but also inorganic material. These species, for example, iron compounds, originated from impurities in fuel or lubricating oil, additives or engine wear may change the physico-chemical characteristics of soot and hence its environmental impact. We studied the change of composition, structure, and oxidation reactivity of laboratory-produced soot aerosol with varying iron content. Soot types of various iron contents were generated in a propane/air diffusion flame by adjusting the doping amount of iron pentacarbonyl Fe(CO)5 to the flame. Scanning electron microscopy (SEM)/energy-dispersive X-ray spectroscopy (EDX) was combined with cluster analysis (CA) to separate individual particles into definable groups of similar chemical composition representing the particle types in dependence of the iron content in soot. Raman microspectroscopy (RM) and infrared spectroscopy were applied for the characterization of the graphitic soot structure, hydrocarbons, and iron species. For the analysis of soot reactivity, temperature-programmed oxidation (TPO) was used. It is demonstrated that iron is most dominantly present in the form of amorphous Fe (III) oxide crystallizing to hematite-Fe2O3 upon thermal treatment. Iron contaminations do not change the soot microstructure crucially, but Fe(CO)5 doping of the flame impacts hydrocarbon composition. Soot oxidation reactivity strongly depends on the iron content, as the temperature of maximum carbon (di)oxide emission Tmax follows an exponential decay with increasing iron content in soot. Based on the results of the thermo-chemical characterization of laboratory-produced internally mixed iron-containing soot, we can conclude that iron-containing combustion aerosol samples cannot be characterized unambiguously by current thermo-optical analysis protocols.
UR - http://www.scopus.com/inward/record.url?scp=84866384533&partnerID=8YFLogxK
U2 - 10.1080/02786826.2012.711917
DO - 10.1080/02786826.2012.711917
M3 - Article
AN - SCOPUS:84866384533
SN - 0278-6826
VL - 46
SP - 1337
EP - 1348
JO - Aerosol Science and Technology
JF - Aerosol Science and Technology
IS - 12
ER -
