Startseite Naturwissenschaften Numerical study on the temperature dependence of soot formation in acetylene pyrolysis blended with methane, formaldehyde, methanol, and dimethyl ether
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Numerical study on the temperature dependence of soot formation in acetylene pyrolysis blended with methane, formaldehyde, methanol, and dimethyl ether

  • Heidi Böhm EMAIL logo , Marina Braun-Unkhoff und Helga Jander
Veröffentlicht/Copyright: 3. April 2024
Zeitschrift für Physikalische Chemie
Aus der Zeitschrift Zeitschrift für Physikalische Chemie Band 238 Heft 12

Abstract

This paper addresses the combined effects of varying C/H and C/O ratios as well as of the molecular structure of the fuels selected on the normalized soot volume fraction f V. For the simulations, an already existing and validated reaction mechanism for the pyrolysis of C2H2 in argon, Aghsaee et al. (Combust. Flame 2014, 161, 2263–2269), was used in the current work. It was extended with PAH reactions from coronene (C24H12) up to ovalene (C32H14), whereas general principles for the rapid build-up of large PAHs were presented. Soot formation was modeled according to Appel et al. (Combust. Flame 2000, 121, 122–136) by applying the method of moments. A validation of the extended reaction model was carried out for shock-wave-induced O2/C2H2 mixtures from literature. In the following, the influence of blends of methane (CH4), formaldehyde (CH2O), methanol (CH3OH), and dimethyl ether (CH3)2O on soot formation during C2H2 pyrolysis diluted in Ar was studied. Special emphasis was laid on the inception chemistry of soot formation. The role of intermediates, such as the propargyl radical (C3H3), leading towards benzene and polyaromatic hydrocarbon (PAH) formation and their interplay with hydrogen molecules (H2) to H atoms (H) ratio was examined. All blends increased the ratio of the concentrations of H2 and H leading thus to reduced soot inception and soot formation. However, soot suppressing effects were overrun by supporting ones when the additives provided suitable molecular groups, such as methyl radicals (CH3), in sufficient high concentrations for early aromatic ring formation. Thus, a prominent synergistic effect on soot formation was found for the CH4/C2H2 mixture only. Besides, species able to mirror characteristics of the soot formation process, such as the peak value of the normalized soot volume fraction, are presented. The findings of this work indicate the synergistic effect of H2/H and C/O ratios as well as of methyl radicals on the PAHs’ production of appropriate size able to initiate soot inception process in an aliphatic fuel.

Keywords: chemical kinetcs; PAH formation; soot modeling; synergistic effects on soot formation; soot promoting effect of methyl radical
Corresponding author: Heidi Böhm, Institute for Combustion and Gas Dynamics – Reactive Fluids, University of Duisburg-Essen, Lotharstraße 1, Duisburg 47057, Germany, E-mail:

Funding source: Deutsche Forschungsgemeinschaft (DFG) project title "Der Einfluss von Wasserstoff und Sauerstoff auf die ersten Schritte der Rußbildung"

Award Identifier / Grant number: 275255277

Acknowledgments

The authors thank Prof. Dr. C. Schulz for providing the facilities at the Institute for Combustion and Gas Dynamics – Reactive Fluids, University of Duisburg-Essen, Germany, to support this work, Dr. M. Fikri for fruitful discussions, and Dr. Elke Goos (DLR Stuttgart, Germany) for preparing Figure 2 on the structures of essential PAHs presented here.

  1. Research ethics: Not applicable.

  2. Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  3. Competing interests: The authors state no conflict of interest.

  4. Research funding: Financial assistance from Deutsche Forschungsgemeinschaft (DFG) award number 275255277 is gratefully acknowledged.

  5. Data availability: Not applicable.

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Received: 2023-06-20
Accepted: 2024-03-07
Published Online: 2024-04-03
Published in Print: 2024-12-17

© 2024 Walter de Gruyter GmbH, Berlin/Boston

Artikel in diesem Heft

  1. Frontmatter
  2. Original Papers
  3. Gamma radiation-induced degradation of Acid Violet 49 in the presence of hydrogen peroxide (H2O2) in an aqueous medium
  4. Oxygen doped g-C3N4/LDH composite as highly efficient photocatalyst for wastewater treatment
  5. Facile synthesis of lanthanum carbonate octahydrate and lanthanum oxide nanoparticles by sonochemical method: systematic characterizations
  6. Numerical study on the temperature dependence of soot formation in acetylene pyrolysis blended with methane, formaldehyde, methanol, and dimethyl ether
  7. The role of greenhouse gases in radiative equilibrium – Thermodynamic evaluation
  8. Ab initio study of surfaces of lead and tin based metal halide perovskite structures
  9. Experimental study of heat pipes for battery cooling technology in EVs
  10. Cellulose acetate sheet supported gold nanoparticles for the catalytic reduction of toxic organic pollutants
https://doi.org/10.1515/zpch-2023-0283
Schlagwörter für diesen Artikel
chemical kinetcs; PAH formation; soot modeling; synergistic effects on soot formation; soot promoting effect of methyl radical

Artikel in diesem Heft

  1. Frontmatter
  2. Original Papers
  3. Gamma radiation-induced degradation of Acid Violet 49 in the presence of hydrogen peroxide (H2O2) in an aqueous medium
  4. Oxygen doped g-C3N4/LDH composite as highly efficient photocatalyst for wastewater treatment
  5. Facile synthesis of lanthanum carbonate octahydrate and lanthanum oxide nanoparticles by sonochemical method: systematic characterizations
  6. Numerical study on the temperature dependence of soot formation in acetylene pyrolysis blended with methane, formaldehyde, methanol, and dimethyl ether
  7. The role of greenhouse gases in radiative equilibrium – Thermodynamic evaluation
  8. Ab initio study of surfaces of lead and tin based metal halide perovskite structures
  9. Experimental study of heat pipes for battery cooling technology in EVs
  10. Cellulose acetate sheet supported gold nanoparticles for the catalytic reduction of toxic organic pollutants
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