Catalytic ignition and pressure dependence of methane/air combustion over palladium oxide

Ran Sui, Wenkai Liang, John Mantzaras, Chung K. Law

Research output: Contribution to conferencePaper

Abstract

The catalytic ignition and kinetics of CH4/air oxidation over PdO were studied using wire microcalorimetry. Ignition temperatures and heat release rates were measured and global kinetic parameters were extracted. Key reactions rates were amended and a detailed surface reaction scheme for atmospheric pressure was proposed. In a subsequent step, the pressure dependence of CH4/air catalytic oxidation over PdO was investigated in the range 1-12 bar in a channel-flow catalytic reactor. In situ Raman measurements of major gas phase species concentrations assessed the heterogeneous reactivity, while planar laser induced fluorescence (LIF) of the OH radical monitored homogeneous combustion. Simulations were performed using a 2-D code with detailed hetero-/homogeneous reaction mechanisms. Comparisons between Raman measured and numerically predicted profiles of major species allowed for the construction of a global catalytic step valid for 1-12 bar. The CH4 catalytic reaction rate had an overall pressure dependence ∼p1-n where the exponent n was itself a monotonically increasing function of pressure. This resulted in non-monotonic pressure dependence, a behavior in stark contrast to other noble metals such at Pt and Rh.

Original languageEnglish (US)
StatePublished - Jan 1 2018
Event2018 Spring Technical Meeting of the Eastern States Section of the Combustion Institute, ESSCI 2018 - State College, United States
Duration: Mar 4 2018Mar 7 2018

Other

Other2018 Spring Technical Meeting of the Eastern States Section of the Combustion Institute, ESSCI 2018
CountryUnited States
CityState College
Period3/4/183/7/18

All Science Journal Classification (ASJC) codes

  • Mechanical Engineering
  • Physical and Theoretical Chemistry
  • Chemical Engineering(all)

Keywords

  • Catalytic ignition
  • Methane total oxidation over PdO
  • Pressure dependence of catalytic reactivity

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  • Cite this

    Sui, R., Liang, W., Mantzaras, J., & Law, C. K. (2018). Catalytic ignition and pressure dependence of methane/air combustion over palladium oxide. Paper presented at 2018 Spring Technical Meeting of the Eastern States Section of the Combustion Institute, ESSCI 2018, State College, United States.