TY - JOUR
T1 - Plasma-Assisted Chemical-Looping Combustion
T2 - Low-Temperature Methane and Ethylene Oxidation with Nickel Oxide
AU - Burger, Christopher M.
AU - Zhang, Angie J.
AU - Xu, Yijie
AU - Hansen, Nils
AU - Ju, Yiguang
N1 - Funding Information:
This material is based upon work supported by the DOE grant DE-SC0020233 of Plasma Science Center, the DOE-NETL grant DE-FE0026825, and the U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences under contract number DE-NA0003525. This research used resources of the Low Temperature Plasma Research Facility at Sandia National Laboratories, which is a collaborative research facility supported by the U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences. This manuscript has been authored by National Technology and Engineering Solutions of Sandia, LLC. under Contact No. DE-NA0003525 with the U.S. Department of Energy/National Nuclear Security Administration. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for Untied States Government purposes. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. DOE or the U.S. Government.
Funding Information:
This material is based upon work supported by the DOE grant DE-SC0020233 of Plasma Science Center, the DOE–NETL grant DE-FE0026825, and the U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences under contract number DE-NA0003525. This research used resources of the Low Temperature Plasma Research Facility at Sandia National Laboratories, which is a collaborative research facility supported by the U.S. Department of Energy, Office of Science, Office of Fusion Energy Sciences. This manuscript has been authored by National Technology and Engineering Solutions of Sandia, LLC. under Contact No. DE-NA0003525 with the U.S. Department of Energy/National Nuclear Security Administration. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for Untied States Government purposes. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. DOE or the U.S. Government.
Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/1/26
Y1 - 2023/1/26
N2 - The chemical reaction network of low-temperature plasma-assisted oxidation of methane (CH4) and ethylene (C2H4) with nickel oxide (NiO) was investigated in a heated plasma reactor through time-dependent species measurements by electron-ionization molecular beam mass spectrometry (EI-MBMS). Methane (ethylene) oxidation by NiO was explored in temperature ranges from 300-700 °C (300-500 °C) and 300-800 °C (300-600 °C) for the plasma and nonplasma conditions. Significant enhancement of methane oxidation was observed with plasma between 400 and 500 °C, where no oxidation was observed under nonplasma conditions. For the oxidation of methane at higher temperatures, three different oxidation stages were observed: (I) a period of complete oxidation, (II) a period of incomplete CO oxidation, and (III) a period of carbon buildup. For the C2H4 experiments, and unlike the CH4 experiments, the plasma resulted in a significant amount of new intermediate oxygenated species, such as CH2O, CH3OH, C2H4O, and C2H6O. Carbon deposits were observed under both methane and ethylene conditions and verified by X-ray photoelectron spectroscopy (XPS). ReaxFF (reactive force field) simulations were performed for the oxidation of CH4 and C2H4 in a nonplasma environment. The simulated intermediates and products largely agree with the species measured in the experiments, though the predicted intermediate oxygenated species such as CH2O and C2H6O were not observed in experiments under nonplasma conditions. A reaction pathway analysis for CH4 and C2H4 reacting with NiO was created based on the observed species from the MBMS spectra along with ReaxFF simulations.
AB - The chemical reaction network of low-temperature plasma-assisted oxidation of methane (CH4) and ethylene (C2H4) with nickel oxide (NiO) was investigated in a heated plasma reactor through time-dependent species measurements by electron-ionization molecular beam mass spectrometry (EI-MBMS). Methane (ethylene) oxidation by NiO was explored in temperature ranges from 300-700 °C (300-500 °C) and 300-800 °C (300-600 °C) for the plasma and nonplasma conditions. Significant enhancement of methane oxidation was observed with plasma between 400 and 500 °C, where no oxidation was observed under nonplasma conditions. For the oxidation of methane at higher temperatures, three different oxidation stages were observed: (I) a period of complete oxidation, (II) a period of incomplete CO oxidation, and (III) a period of carbon buildup. For the C2H4 experiments, and unlike the CH4 experiments, the plasma resulted in a significant amount of new intermediate oxygenated species, such as CH2O, CH3OH, C2H4O, and C2H6O. Carbon deposits were observed under both methane and ethylene conditions and verified by X-ray photoelectron spectroscopy (XPS). ReaxFF (reactive force field) simulations were performed for the oxidation of CH4 and C2H4 in a nonplasma environment. The simulated intermediates and products largely agree with the species measured in the experiments, though the predicted intermediate oxygenated species such as CH2O and C2H6O were not observed in experiments under nonplasma conditions. A reaction pathway analysis for CH4 and C2H4 reacting with NiO was created based on the observed species from the MBMS spectra along with ReaxFF simulations.
UR - http://www.scopus.com/inward/record.url?scp=85146617343&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85146617343&partnerID=8YFLogxK
U2 - 10.1021/acs.jpca.2c07184
DO - 10.1021/acs.jpca.2c07184
M3 - Article
C2 - 36648424
AN - SCOPUS:85146617343
SN - 1089-5639
VL - 127
SP - 789
EP - 798
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
IS - 3
ER -