skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Formation mechanism of polycyclic aromatic hydrocarbons and fullerenes in premixed benzene flames

Abstract

A better understanding of the formation of polycyclic aromatic hydrocarbons (PAH) and fullerenes is of practical interest due to the apparent environmental health effects of many PAH and potential industrial applications of fullerenes. In the present work, a kinetic model describing the growth of PAH up to coronene (C{sub 24}H{sub 12}) and of C{sub 60} and C{sub 70} fullerenes is developed. Comparison of the model predictions with concentration profiles in a nearly sooting low-pressure premixed, laminar, one-dimensional benzene/oxygen/argon flame (equivalence ratio {phi} = 1.8, pressure = 2.67 kPa) measured by Bittner using a molecular beam system coupled to mass spectrometry shows reasonably good predictive capability for stable and radical intermediates and growth species up to C{sub 16}H{sub 10} isomers. Cyclopentadienyl is found to be a key species for naphthalene formation. The further growth process is based on H abstraction and acetylene addition but also the contribution of small PAH is considered. Good to fair agreement between model predictions and experimental data for larger PAH including the different C{sub 16}H{sub 10} isomers obtained by gas chromatography coupled to mass spectrometry and high performance liquid chromatography could be achieved for PAH in a sooting low-pressure premixed, laminar, one-dimensional benzene/oxygen/argon flame ({phi} =more » 2.4, 5.33 kPa). C{sub 60} and C{sub 70} fullerenes are underpredicted, and possible reasons such as uncertainties in rate coefficients or the existence of other formation pathways are discussed. PAH depletion in the burnt gas is not reproduced by the model and is believed to involve supplementary sinks such as reactions involving PAH and growing soot particles.« less

Authors:
; ;
Publication Date:
Research Org.:
Massachusetts Inst. of Tech., Cambridge, MA (US)
Sponsoring Org.:
USDOE; National Institute of Environmental Health Sciences; National Aeronautics and Space Administration
OSTI Identifier:
20000572
DOE Contract Number:  
FG02-84ER13282
Resource Type:
Journal Article
Journal Name:
Combustion and Flame
Additional Journal Information:
Journal Volume: 119; Journal Issue: 1-2; Other Information: PBD: Oct 1999; Journal ID: ISSN 0010-2180
Country of Publication:
United States
Language:
English
Subject:
40 CHEMISTRY; POLYCYCLIC AROMATIC HYDROCARBONS; FULLERENES; CHEMICAL REACTION YIELD; BENZENE; COMBUSTION KINETICS; MATHEMATICAL MODELS; REACTION INTERMEDIATES; SOOT

Citation Formats

Richter, H, Grieco, W J, and Howard, J B. Formation mechanism of polycyclic aromatic hydrocarbons and fullerenes in premixed benzene flames. United States: N. p., 1999. Web. doi:10.1016/S0010-2180(99)00032-2.
Richter, H, Grieco, W J, & Howard, J B. Formation mechanism of polycyclic aromatic hydrocarbons and fullerenes in premixed benzene flames. United States. https://doi.org/10.1016/S0010-2180(99)00032-2
Richter, H, Grieco, W J, and Howard, J B. 1999. "Formation mechanism of polycyclic aromatic hydrocarbons and fullerenes in premixed benzene flames". United States. https://doi.org/10.1016/S0010-2180(99)00032-2.
@article{osti_20000572,
title = {Formation mechanism of polycyclic aromatic hydrocarbons and fullerenes in premixed benzene flames},
author = {Richter, H and Grieco, W J and Howard, J B},
abstractNote = {A better understanding of the formation of polycyclic aromatic hydrocarbons (PAH) and fullerenes is of practical interest due to the apparent environmental health effects of many PAH and potential industrial applications of fullerenes. In the present work, a kinetic model describing the growth of PAH up to coronene (C{sub 24}H{sub 12}) and of C{sub 60} and C{sub 70} fullerenes is developed. Comparison of the model predictions with concentration profiles in a nearly sooting low-pressure premixed, laminar, one-dimensional benzene/oxygen/argon flame (equivalence ratio {phi} = 1.8, pressure = 2.67 kPa) measured by Bittner using a molecular beam system coupled to mass spectrometry shows reasonably good predictive capability for stable and radical intermediates and growth species up to C{sub 16}H{sub 10} isomers. Cyclopentadienyl is found to be a key species for naphthalene formation. The further growth process is based on H abstraction and acetylene addition but also the contribution of small PAH is considered. Good to fair agreement between model predictions and experimental data for larger PAH including the different C{sub 16}H{sub 10} isomers obtained by gas chromatography coupled to mass spectrometry and high performance liquid chromatography could be achieved for PAH in a sooting low-pressure premixed, laminar, one-dimensional benzene/oxygen/argon flame ({phi} = 2.4, 5.33 kPa). C{sub 60} and C{sub 70} fullerenes are underpredicted, and possible reasons such as uncertainties in rate coefficients or the existence of other formation pathways are discussed. PAH depletion in the burnt gas is not reproduced by the model and is believed to involve supplementary sinks such as reactions involving PAH and growing soot particles.},
doi = {10.1016/S0010-2180(99)00032-2},
url = {https://www.osti.gov/biblio/20000572}, journal = {Combustion and Flame},
issn = {0010-2180},
number = 1-2,
volume = 119,
place = {United States},
year = {1999},
month = {10}
}