TY - JOUR
T1 - Low- and intermediate-temperature oxidation of dimethyl ether up to 100 atm in a supercritical pressure jet-stirred reactor
AU - Yan, Chao
AU - Zhao, Hao
AU - Wang, Ziyu
AU - Song, Guohui
AU - Lin, Ying
AU - Mulvihill, Clayton R.
AU - Jasper, Ahren W.
AU - Klippenstein, Stephen J.
AU - Ju, Yiguang
N1 - Funding Information:
YJ would like to sincerely thank Prof. Katherina Kohse-Höinghaus for her long-time support and collaborations in combustion chemistry. We would like to present this work to honor her great contributions to combustion chemistry and to remember our collaboration on dimethyl ether chemistry. This work was partly supported by ARO grant W911NF-16–1–0076 and the DOE BES award DE-SC0021135. The material in this study is based in part on work at ANL supported by the U.S. Department of Energy (USDOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under DOE Contract Number DE-AC02–06CH11357 through the Argonne-Sandia Consortium on High-Pressure Combustion Chemistry, FWP 59044.
Publisher Copyright:
© 2022 The Combustion Institute
PY - 2022/9
Y1 - 2022/9
N2 - Understanding the low- and intermediate-temperature oxidation chemistry of oxygenated fuels like dimethyl ether (DME) at high pressure is paramount to the development of advanced engines with low carbon emissions. The supercritical pressure jet-stirred reactor (SP-JSR) recently developed at Princeton provides a new platform for conducting kinetic studies at low and intermediate temperatures at extremely high pressures with a uniform temperature distribution and a short flow residence time. This paper uses the SP-JSR to investigate DME oxidation at equivalence ratios of 0.175, 1.0, and 1.72, for pressures of 10 and 100 atm, and temperatures ranging from 400 to 900 K. The results demonstrate weakened NTC behavior at 100 atm relative to 10 atm due to increased flux through QOOH + O2 = O2QOOH relative to QOOH = 2 CH2O + OH at 100 atm. Furthermore, the intermediate-temperature oxidation window is shifted to lower temperatures at 100 atm. The experimental data are compared with several chemical kinetic models from the literature. The existing models are seen to agree quite well with the experimental data at 10 atm. However, the models fail to properly capture the NTC behavior at 100 atm. Reaction pathway analyses indicate that both the low- and intermediate-temperature chemistries are controlled by RO2 consumption pathways. The reaction rates for several of the important reactions, such as DME + OH = CH3OCH2 + H2O, H2O2 (+M) = 2 OH (+M), and 2 HO2 = 2 OH + O2 are updated in this work. The updated model improves the predictability for all key species compared to the original model.
AB - Understanding the low- and intermediate-temperature oxidation chemistry of oxygenated fuels like dimethyl ether (DME) at high pressure is paramount to the development of advanced engines with low carbon emissions. The supercritical pressure jet-stirred reactor (SP-JSR) recently developed at Princeton provides a new platform for conducting kinetic studies at low and intermediate temperatures at extremely high pressures with a uniform temperature distribution and a short flow residence time. This paper uses the SP-JSR to investigate DME oxidation at equivalence ratios of 0.175, 1.0, and 1.72, for pressures of 10 and 100 atm, and temperatures ranging from 400 to 900 K. The results demonstrate weakened NTC behavior at 100 atm relative to 10 atm due to increased flux through QOOH + O2 = O2QOOH relative to QOOH = 2 CH2O + OH at 100 atm. Furthermore, the intermediate-temperature oxidation window is shifted to lower temperatures at 100 atm. The experimental data are compared with several chemical kinetic models from the literature. The existing models are seen to agree quite well with the experimental data at 10 atm. However, the models fail to properly capture the NTC behavior at 100 atm. Reaction pathway analyses indicate that both the low- and intermediate-temperature chemistries are controlled by RO2 consumption pathways. The reaction rates for several of the important reactions, such as DME + OH = CH3OCH2 + H2O, H2O2 (+M) = 2 OH (+M), and 2 HO2 = 2 OH + O2 are updated in this work. The updated model improves the predictability for all key species compared to the original model.
KW - Dimethyl ether
KW - Jet-stirred reactor
KW - Low-temperature chemistry
KW - SP-JSR
KW - Ultra-high pressure
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U2 - 10.1016/j.combustflame.2022.112059
DO - 10.1016/j.combustflame.2022.112059
M3 - Article
AN - SCOPUS:85123457891
SN - 0010-2180
VL - 243
JO - Combustion and Flame
JF - Combustion and Flame
M1 - 112059
ER -