TY - JOUR
T1 - Analysis of gas phase compounds in chemical vapor deposition of carbon from light hydrocarbons
AU - Norinaga, Koyo
AU - Deutschmann, Olaf
AU - Hüttinger, Klaus J.
N1 - Funding Information:
This research was conducted in the Sonderforschungsbereich (SFB) 551 “Carbon from gas-phase: elementary reactions, structures, materials,” which is funded by the Deutsche Forschungsgemeinschaft (DFG). The Alexander von Humboldt Foundation is acknowledged for providing a research fellowship to KN.
PY - 2006/8
Y1 - 2006/8
N2 - Product distributions in the pyrolysis of ethylene, acetylene, and propylene are studied to obtain an experimental database for a detailed kinetic modeling of gas phase reactions in chemical vapor deposition of carbon from these light hydrocarbons. Experiments were performed with a vertical flow reactor at 900 °C and pressures from 2 to 15 kPa. Gas phase components were analyzed by both on-line and off-line gas chromatography. More than 40 compounds from hydrogen to coronene were identified and quantitatively determined as a function of the residence time varied up to 1.6 s. Product recoveries were generally more than 90%. Analysis of the kinetics of the conversion of the hydrocarbons resulted in global reaction orders of 1.2 (ethylene), 2.7 (acetylene), and 1.5 (propylene). First order dehydrogenation reactions and third order trimerization reactions leading to benzene are decisive reactions for ethylene and acetylene, respectively. Conversion of propylene should also be based on two simultaneous reactions, a first order dissociation reaction, and second order reactions such as bimolecular reaction of propylene resulting an allyl and a propyl radical. These insights should be useful to develop a reaction mechanism based on elementary reactions in forthcoming studies.
AB - Product distributions in the pyrolysis of ethylene, acetylene, and propylene are studied to obtain an experimental database for a detailed kinetic modeling of gas phase reactions in chemical vapor deposition of carbon from these light hydrocarbons. Experiments were performed with a vertical flow reactor at 900 °C and pressures from 2 to 15 kPa. Gas phase components were analyzed by both on-line and off-line gas chromatography. More than 40 compounds from hydrogen to coronene were identified and quantitatively determined as a function of the residence time varied up to 1.6 s. Product recoveries were generally more than 90%. Analysis of the kinetics of the conversion of the hydrocarbons resulted in global reaction orders of 1.2 (ethylene), 2.7 (acetylene), and 1.5 (propylene). First order dehydrogenation reactions and third order trimerization reactions leading to benzene are decisive reactions for ethylene and acetylene, respectively. Conversion of propylene should also be based on two simultaneous reactions, a first order dissociation reaction, and second order reactions such as bimolecular reaction of propylene resulting an allyl and a propyl radical. These insights should be useful to develop a reaction mechanism based on elementary reactions in forthcoming studies.
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U2 - 10.1016/j.carbon.2005.12.050
DO - 10.1016/j.carbon.2005.12.050
M3 - Article
AN - SCOPUS:33646465852
SN - 0008-6223
VL - 44
SP - 1790
EP - 1800
JO - Carbon
JF - Carbon
IS - 9
ER -