Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor

Tao, Tao; Sun, Wenyu; Hansen, Nils; Jasper, Ahren W.; Moshammer, Kai; Chen, Bingjie; Wang, Zhandong; Huang, Can; Dagaut, Philippe; Yang, Bin

doi:10.1016/j.combustflame.2018.01.048

Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor

Journal Article · Tue Mar 20 04:00:00 EDT 2018 · Combustion and Flame

DOI:https://doi.org/10.1016/j.combustflame.2018.01.048· OSTI ID:1474084

Tao, Tao ^[1]; Sun, Wenyu ^[1]; Hansen, Nils ^[2]; Jasper, Ahren W. ^[3]; Moshammer, Kai ^[4]; Chen, Bingjie ^[5]; ^[5]; Huang, Can ^[1]; Dagaut, Philippe ^[6]; ^[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)

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. In this paper, 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. Finally, 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.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Lab. (SNL-CA), Livermore, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Tsinghua Univ., Beijing (China)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA); National Natural Science Foundation of China (NSFC); China Scholarship Council

Grant/Contract Number:: NA0003525; AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1474084

Alternate ID(s):: OSTI ID: 1515794
OSTI ID: 1483651

Report Number(s):: SAND--2018-10256J; 667990

Journal Information:: Combustion and Flame, Journal Name: Combustion and Flame Vol. 192; ISSN 0010-2180

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor

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