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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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    ViewPageProof_CNF_9942.pdf
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    Description:
    Accepted Manuscript
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    Type
    Article
    Authors
    Tao, Tao
    Sun, Wenyu
    Hansen, Nils
    Jasper, Ahren W.
    Moshammer, Kai
    Chen, Bingjie cc
    Wang, Zhandong cc
    Huang, Can
    Dagaut, Philippe cc
    Yang, Bin cc
    KAUST Department
    Chemical Engineering Program
    Clean Combustion Research Center
    Physical Science and Engineering (PSE) Division
    Date
    2018-03-20
    Online Publication Date
    2018-03-20
    Print Publication Date
    2018-06
    Permanent link to this record
    http://hdl.handle.net/10754/627380
    
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    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 O-addition to and the decomposition of the CHCO radical.
    Citation
    Tao T, Sun W, Hansen N, Jasper AW, Moshammer K, et al. (2018) Exploring the negative temperature coefficient behavior of acetaldehyde based on detailed intermediate measurements in a jet-stirred reactor. Combustion and Flame 192: 120–129. Available: http://dx.doi.org/10.1016/j.combustflame.2018.01.048.
    Sponsors
    We really appreciate the productive discussion with Dr. Ultan Burke and Dr. Henry J. Curran. This work is supported by the National Natural Science Foundation of China (Nos. 91741109 and 91541113). TT wants to thank for the support China Scholarship Council. The experiments profited from the expert technical assistance of Paul Fugazzi. This research used resources of the Advanced Light Source, supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DEAC02-05CH11231. NH, AWJ and KM were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under Contract DE-NA0003525. The work at Argonne is supported under Contract no. DE-AC02-06CH11357DOE-BES through the GPCP program.
    Publisher
    Elsevier BV
    Journal
    Combustion and Flame
    DOI
    10.1016/j.combustflame.2018.01.048
    Additional Links
    https://www.sciencedirect.com/science/article/pii/S0010218018300622
    ae974a485f413a2113503eed53cd6c53
    10.1016/j.combustflame.2018.01.048
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Engineering Program; Clean Combustion Research Center

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