Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor
Abstract
Acetaldehyde is an observed emission species and a key intermediate produced during the combustion and low-temperature oxidation of fossil and bio-derived fuels. Investigations into the low-temperature oxidation chemistry of acetaldehyde are essential to develop a better core mechanism and to better understand auto-ignition and cool flame phenomena. Here, the oxidation of acetaldehyde was studied at low-temperatures (528–946 K) in a jet-stirred reactor (JSR) with the corrected residence time of 2.7 s at 700 Torr. This work describes a detailed set of experimental results that capture the negative temperature coefficient (NTC) behavior in the low-temperature oxidation of acetaldehyde. The mole fractions of 28 species were measured as functions of the temperature by employing a vacuum ultra-violet photoionization molecular-beam mass spectrometer. To explain the observed NTC behavior, an updated mechanism was proposed, which well reproduces the concentration profiles of many observed peroxide intermediates. The kinetic analysis based on the updated mechanism reveals that the NTC behavior of acetaldehyde oxidation is caused by the competition between the O2-addition to and the decomposition of the CH3CO radical.
- Authors:
-
[5];
[1]
- Tsinghua Univ., Beijing (China). Center for Combustion Energy. Dept. of Energy and Power Engineering. Key Lab. for Thermal Science and Power Engineering of MOE
- Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
- Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility; Physikalisch-Technische Bundesanstalt (PTB), Braunschweig (Germany). Dept. of Thermophysical Quantities
- King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Saudi Arabia). Clean Combustion Research Center (CCRC)
- Inst. of Engineering Sciences and Systems (CNRS-INSIS), Orléans (France). Inst. of Combustion, Aerothermal, Reactivity and Environment (ICARE)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-CA), Livermore, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Tsinghua Univ., Beijing (China)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); National Natural Science Foundation of China (NSFC); China Scholarship Council; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1474084
- Alternate Identifier(s):
- OSTI ID: 1483651; OSTI ID: 1515794
- Report Number(s):
- SAND-2018-10256J
Journal ID: ISSN 0010-2180; 667990
- Grant/Contract Number:
- NA0003525; AC02-05CH11231; AC02-06CH11357; 91741109; 91541113; DEAC02-05CH11231; AC02-06CH11357DOE-BES
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Combustion and Flame
- Additional Journal Information:
- Journal Volume: 192; Journal ID: ISSN 0010-2180
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; acetaldehyde; negative temperature coefficient; jet-stirred reactor; molecular-beam mass spectrometry
Citation Formats
Tao, Tao, Sun, Wenyu, Hansen, Nils, Jasper, Ahren W., Moshammer, Kai, Chen, Bingjie, Wang, Zhandong, Huang, Can, Dagaut, Philippe, and Yang, Bin. Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor. United States: N. p., 2018.
Web. doi:10.1016/j.combustflame.2018.01.048.
Tao, Tao, Sun, Wenyu, Hansen, Nils, Jasper, Ahren W., Moshammer, Kai, Chen, Bingjie, Wang, Zhandong, Huang, Can, Dagaut, Philippe, & Yang, Bin. Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor. United States. https://doi.org/10.1016/j.combustflame.2018.01.048
Tao, Tao, Sun, Wenyu, Hansen, Nils, Jasper, Ahren W., Moshammer, Kai, Chen, Bingjie, Wang, Zhandong, Huang, Can, Dagaut, Philippe, and Yang, Bin. Tue .
"Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor". United States. https://doi.org/10.1016/j.combustflame.2018.01.048. https://www.osti.gov/servlets/purl/1474084.
@article{osti_1474084,
title = {Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor},
author = {Tao, Tao and Sun, Wenyu and Hansen, Nils and Jasper, Ahren W. and Moshammer, Kai and Chen, Bingjie and Wang, Zhandong and Huang, Can and Dagaut, Philippe and Yang, Bin},
abstractNote = {Acetaldehyde is an observed emission species and a key intermediate produced during the combustion and low-temperature oxidation of fossil and bio-derived fuels. Investigations into the low-temperature oxidation chemistry of acetaldehyde are essential to develop a better core mechanism and to better understand auto-ignition and cool flame phenomena. Here, the oxidation of acetaldehyde was studied at low-temperatures (528–946 K) in a jet-stirred reactor (JSR) with the corrected residence time of 2.7 s at 700 Torr. This work describes a detailed set of experimental results that capture the negative temperature coefficient (NTC) behavior in the low-temperature oxidation of acetaldehyde. The mole fractions of 28 species were measured as functions of the temperature by employing a vacuum ultra-violet photoionization molecular-beam mass spectrometer. To explain the observed NTC behavior, an updated mechanism was proposed, which well reproduces the concentration profiles of many observed peroxide intermediates. The kinetic analysis based on the updated mechanism reveals that the NTC behavior of acetaldehyde oxidation is caused by the competition between the O2-addition to and the decomposition of the CH3CO radical.},
doi = {10.1016/j.combustflame.2018.01.048},
journal = {Combustion and Flame},
number = ,
volume = 192,
place = {United States},
year = {Tue Mar 20 00:00:00 EDT 2018},
month = {Tue Mar 20 00:00:00 EDT 2018}
}
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