Temperature-programmed plasma surface reaction: An approach to determine plasma-catalytic performance

Research output: Contribution to journalArticleAcademicpeer-review

9 Citations (Scopus)
70 Downloads (Pure)

Abstract

Plasma-enhanced heterogeneous catalysis offers a promising alternative to thermal catalysis due to the synergy between the plasma and the solid catalyst. However, there is only a limited mechanistic insight about the interactions of highly energetic electrons and excited molecules with heterogeneous catalysts in plasmas. Accurate performance comparison in a plasma-catalytic setting is complicated because of the intricate nature of the plasma-catalyst system: simultaneous reactions occurring in the gas-phase and at the catalytic surface; the dependence of the discharge on dielectric properties of the packed catalyst bed; and the dependence of permittivity and polarization of the catalyst on plasma parameters. Here, we present a method of temperature-programmed plasma surface reaction (TPPSR) that allows decoupling gas-phase processes from the surface plasma-induced reactions. Using this method we reveal the main reasons of apparent synergy between plasma and heterogeneous catalyst for the case of carbon dioxide hydrogenation. Experiments with isotopically labelled CO2 and temperature-programmed plasma reaction experiments in flow of CO2/H2 prove a substantial role of gas-phase dissociation/hydrogenation for the observed catalyst activity and selectivity. The product distribution and reaction pathways do not significantly depend on the discharge parameters. Taking into account overheating of the catalytic bed for comparison of catalytic activity with and without plasma, it was concluded that energy dissipation also plays an important role. The observed plasma enhancement is in part due to the acceleration of electron-induced surface reactions.

Original languageEnglish
Pages (from-to)168-177
Number of pages10
JournalApplied Catalysis. B, Environmental
Volume239
DOIs
Publication statusPublished - 30 Dec 2018

Fingerprint

Surface reactions
Plasmas
plasma
catalyst
temperature
Temperature
Catalysts
Gases
catalysis
Catalysis
Hydrogenation
Catalyst activity
gas
electron
dielectric property
Electrons
Catalyst selectivity
permittivity
energy dissipation
Carbon Dioxide

Keywords

  • Ceria-zirconia
  • COmethanation
  • Heterogeneous catalysis
  • Non-thermal plasma
  • TPR

Cite this

@article{7f18f41df5714cc1a57068f2e228419b,
title = "Temperature-programmed plasma surface reaction: An approach to determine plasma-catalytic performance",
abstract = "Plasma-enhanced heterogeneous catalysis offers a promising alternative to thermal catalysis due to the synergy between the plasma and the solid catalyst. However, there is only a limited mechanistic insight about the interactions of highly energetic electrons and excited molecules with heterogeneous catalysts in plasmas. Accurate performance comparison in a plasma-catalytic setting is complicated because of the intricate nature of the plasma-catalyst system: simultaneous reactions occurring in the gas-phase and at the catalytic surface; the dependence of the discharge on dielectric properties of the packed catalyst bed; and the dependence of permittivity and polarization of the catalyst on plasma parameters. Here, we present a method of temperature-programmed plasma surface reaction (TPPSR) that allows decoupling gas-phase processes from the surface plasma-induced reactions. Using this method we reveal the main reasons of apparent synergy between plasma and heterogeneous catalyst for the case of carbon dioxide hydrogenation. Experiments with isotopically labelled CO2 and temperature-programmed plasma reaction experiments in flow of CO2/H2 prove a substantial role of gas-phase dissociation/hydrogenation for the observed catalyst activity and selectivity. The product distribution and reaction pathways do not significantly depend on the discharge parameters. Taking into account overheating of the catalytic bed for comparison of catalytic activity with and without plasma, it was concluded that energy dissipation also plays an important role. The observed plasma enhancement is in part due to the acceleration of electron-induced surface reactions.",
keywords = "Ceria-zirconia, COmethanation, Heterogeneous catalysis, Non-thermal plasma, TPR",
author = "A. Parastaev and Wilfred Hoeben and {van Heesch}, {E.J.M. (Bert)} and N. Kosinov and E.J.M. Hensen",
year = "2018",
month = "12",
day = "30",
doi = "10.1016/j.apcatb.2018.08.011",
language = "English",
volume = "239",
pages = "168--177",
journal = "Applied Catalysis. B, Environmental",
issn = "0926-3373",
publisher = "Elsevier",

}

TY - JOUR

T1 - Temperature-programmed plasma surface reaction

T2 - An approach to determine plasma-catalytic performance

AU - Parastaev, A.

AU - Hoeben, Wilfred

AU - van Heesch, E.J.M. (Bert)

AU - Kosinov, N.

AU - Hensen, E.J.M.

PY - 2018/12/30

Y1 - 2018/12/30

N2 - Plasma-enhanced heterogeneous catalysis offers a promising alternative to thermal catalysis due to the synergy between the plasma and the solid catalyst. However, there is only a limited mechanistic insight about the interactions of highly energetic electrons and excited molecules with heterogeneous catalysts in plasmas. Accurate performance comparison in a plasma-catalytic setting is complicated because of the intricate nature of the plasma-catalyst system: simultaneous reactions occurring in the gas-phase and at the catalytic surface; the dependence of the discharge on dielectric properties of the packed catalyst bed; and the dependence of permittivity and polarization of the catalyst on plasma parameters. Here, we present a method of temperature-programmed plasma surface reaction (TPPSR) that allows decoupling gas-phase processes from the surface plasma-induced reactions. Using this method we reveal the main reasons of apparent synergy between plasma and heterogeneous catalyst for the case of carbon dioxide hydrogenation. Experiments with isotopically labelled CO2 and temperature-programmed plasma reaction experiments in flow of CO2/H2 prove a substantial role of gas-phase dissociation/hydrogenation for the observed catalyst activity and selectivity. The product distribution and reaction pathways do not significantly depend on the discharge parameters. Taking into account overheating of the catalytic bed for comparison of catalytic activity with and without plasma, it was concluded that energy dissipation also plays an important role. The observed plasma enhancement is in part due to the acceleration of electron-induced surface reactions.

AB - Plasma-enhanced heterogeneous catalysis offers a promising alternative to thermal catalysis due to the synergy between the plasma and the solid catalyst. However, there is only a limited mechanistic insight about the interactions of highly energetic electrons and excited molecules with heterogeneous catalysts in plasmas. Accurate performance comparison in a plasma-catalytic setting is complicated because of the intricate nature of the plasma-catalyst system: simultaneous reactions occurring in the gas-phase and at the catalytic surface; the dependence of the discharge on dielectric properties of the packed catalyst bed; and the dependence of permittivity and polarization of the catalyst on plasma parameters. Here, we present a method of temperature-programmed plasma surface reaction (TPPSR) that allows decoupling gas-phase processes from the surface plasma-induced reactions. Using this method we reveal the main reasons of apparent synergy between plasma and heterogeneous catalyst for the case of carbon dioxide hydrogenation. Experiments with isotopically labelled CO2 and temperature-programmed plasma reaction experiments in flow of CO2/H2 prove a substantial role of gas-phase dissociation/hydrogenation for the observed catalyst activity and selectivity. The product distribution and reaction pathways do not significantly depend on the discharge parameters. Taking into account overheating of the catalytic bed for comparison of catalytic activity with and without plasma, it was concluded that energy dissipation also plays an important role. The observed plasma enhancement is in part due to the acceleration of electron-induced surface reactions.

KW - Ceria-zirconia

KW - COmethanation

KW - Heterogeneous catalysis

KW - Non-thermal plasma

KW - TPR

UR - http://www.scopus.com/inward/record.url?scp=85051269447&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2018.08.011

DO - 10.1016/j.apcatb.2018.08.011

M3 - Article

AN - SCOPUS:85051269447

VL - 239

SP - 168

EP - 177

JO - Applied Catalysis. B, Environmental

JF - Applied Catalysis. B, Environmental

SN - 0926-3373

ER -