Experimental and kinetic study on the low-temperature oxidation of pyridine as a representative of fuel-N compounds

Ling Nan Wu, Zhen Yu Tian*, Jun Jie Weng, Dan Yu, Yue Xi Liu, Dong Xu Tian, Chuang Chuang Cao, Jia Biao Zou, Yan Zhang, Jiu Zhong Yang

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

36 Scopus citations

Abstract

The low-temperature oxidation (LTO) of pyridine was studied in a jet-stirred reactor over the temperature range of 700–1000 K at atmospheric pressure and equivalence ratio of 2.0. Mole fraction profiles of the reaction products were obtained based on molecular beam mass spectrometry and tunable vacuum ultraviolet synchrotron photoionization techniques. Hydrogen peroxide, methanamine, acetylenamine, ethenamine, acetaldimine, ethylamine, allyamine, and methylformamide were newly identified compared with previous studies of pyridine flame and pyrolysis. HCN was found to be the dominant N-containing species of pyridine LTO. Pyrrole, acrylonitrile, acetonitrile, and ammonia were also found at the same level of N2O and NO. Based on the new measurements and updated rate constants of several reactions including the H-abstractions of pyridine as well as the oxidation of ortho-pyridyl using density functional theory calculations, a new pyridine LTO kinetic model consisting of 588 species and 3516 reactions was developed with a reasonable agreement with the experimental results. In general, the predictions of the predominant species have been improved compared with the existing model. Rate-of-production analysis indicates that pyridine mainly consumes via C5H5N→C5H4N→C5H4NO2→HCN+CO+CH2CHC˙O, and C5H5N→C5H5NO→C2H2+HCN+CH2CO. Sensitivity analysis shows that C5H4N+O2=>C5H4NO2, and C5H5N+OH[dbnd]C5H4N+H2O have significant promoting effect on pyridine consumption, while the reverse of C5H4N+HO2[dbnd]C5H4NO+OH has strong inhibiting effect. The results will enrich the understanding of pyridine low-temperature oxidation mechanism, which can be applied to the fields of coal pre-treatment, staged combustion and mild combustion.

Original languageEnglish (US)
Pages (from-to)394-404
Number of pages11
JournalCombustion and Flame
Volume202
DOIs
StatePublished - Apr 2019

Bibliographical note

Funding Information:
The authors are grateful for the financial support from National Natural Science Foundation of China (No. 91541102/51476168), the Ministry of Science and Technology of China (2017YFA0402800) and Recruitment Program of Global Youth Experts. The authors thank the mechanism checker tool provided by Lawrence Livermore National Laboratory. The authors are very grateful for the kind help from Profs. Maria U. Alzueta and Peter Glarborg for their help in the modeling part of this work.

Funding Information:
The authors are grateful for the financial support from National Natural Science Foundation of China (No. 91541102/51476168 ), the Ministry of Science and Technology of China ( 2017YFA0402800 ) and Recruitment Program of Global Youth Experts. The authors thank the mechanism checker tool provided by Lawrence Livermore National Laboratory. The authors are very grateful for the kind help from Profs. Maria U. Alzueta and Peter Glarborg for their help in the modeling part of this work.

Publisher Copyright:
© 2019 The Combustion Institute

Keywords

  • Intermediates
  • Kinetic modeling
  • Low-temperature oxidation
  • Nitrogen chemistry
  • Pyridine

ASJC Scopus subject areas

  • General Chemistry
  • General Chemical Engineering
  • Fuel Technology
  • Energy Engineering and Power Technology
  • General Physics and Astronomy

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