CO and byproduct formation during CO2 reduction in dielectric barrier discharges

F.K. Brehmer, S. Welzel, M.C.M. Sanden, van de, R.A.H. Engeln

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Uittreksel

The dissociation of CO2 and the formation of CO, O3, and O2 were studied in a dielectric barrier discharge (DBD) at atmospheric pressure by means of ex-situ infrared absorption spectroscopy. CO mixing ratios of 0.1%–4.4% were determined for specific injected energies between 0.1 and 20¿eV per molecule (0.3–70¿kJ/l). A lower limit of the gas temperature of 320–480¿K was estimated from the wall temperature of the quartz reactor as measured with an infrared camera. The formation of CO in the DBD could be described as function of the total number of transferred charges during the residence time of the gas in the active plasma zone. An almost stoichiometric CO:O2 ratio of 2:1 was observed along with a strongly temperature dependent O3 production up to 0.075%. Although the ideal range for an efficient CO2 dissociation in plasmas of 1¿eV per molecule for the specific injected energy was covered, the energy efficiency remained below 5% for all conditions. The present results indicate a reaction mechanism which is initiated by electron impact processes followed by charge transfer reactions and non-negligible surface enhanced O and CO recombination. While electron-driven CO2 dissociation is relatively energy inefficient by itself, fast O recombination and the low gas temperatures inhibit the synergistic reuse of atomic oxygen in a secondary CO2¿+¿O dissociation step.
Originele taal-2Engels
Artikelnummer123303
Pagina's (van-tot)123303-1/14
TijdschriftJournal of Applied Physics
Volume116
DOI's
StatusGepubliceerd - 2014

Vingerafdruk

dissociation
gas temperature
energy
reuse
wall temperature
mixing ratios
infrared absorption
electron impact
molecules
atmospheric pressure
absorption spectroscopy
quartz
infrared spectroscopy
cameras
reactors
charge transfer
oxygen
gases
electrons
temperature

Citeer dit

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title = "CO and byproduct formation during CO2 reduction in dielectric barrier discharges",
abstract = "The dissociation of CO2 and the formation of CO, O3, and O2 were studied in a dielectric barrier discharge (DBD) at atmospheric pressure by means of ex-situ infrared absorption spectroscopy. CO mixing ratios of 0.1{\%}–4.4{\%} were determined for specific injected energies between 0.1 and 20¿eV per molecule (0.3–70¿kJ/l). A lower limit of the gas temperature of 320–480¿K was estimated from the wall temperature of the quartz reactor as measured with an infrared camera. The formation of CO in the DBD could be described as function of the total number of transferred charges during the residence time of the gas in the active plasma zone. An almost stoichiometric CO:O2 ratio of 2:1 was observed along with a strongly temperature dependent O3 production up to 0.075{\%}. Although the ideal range for an efficient CO2 dissociation in plasmas of 1¿eV per molecule for the specific injected energy was covered, the energy efficiency remained below 5{\%} for all conditions. The present results indicate a reaction mechanism which is initiated by electron impact processes followed by charge transfer reactions and non-negligible surface enhanced O and CO recombination. While electron-driven CO2 dissociation is relatively energy inefficient by itself, fast O recombination and the low gas temperatures inhibit the synergistic reuse of atomic oxygen in a secondary CO2¿+¿O dissociation step.",
author = "F.K. Brehmer and S. Welzel and {Sanden, van de}, M.C.M. and R.A.H. Engeln",
year = "2014",
doi = "10.1063/1.4896132",
language = "English",
volume = "116",
pages = "123303--1/14",
journal = "Journal of Applied Physics",
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publisher = "American Institute of Physics",

}

CO and byproduct formation during CO2 reduction in dielectric barrier discharges. / Brehmer, F.K.; Welzel, S.; Sanden, van de, M.C.M.; Engeln, R.A.H.

In: Journal of Applied Physics, Vol. 116, 123303, 2014, blz. 123303-1/14.

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

TY - JOUR

T1 - CO and byproduct formation during CO2 reduction in dielectric barrier discharges

AU - Brehmer, F.K.

AU - Welzel, S.

AU - Sanden, van de, M.C.M.

AU - Engeln, R.A.H.

PY - 2014

Y1 - 2014

N2 - The dissociation of CO2 and the formation of CO, O3, and O2 were studied in a dielectric barrier discharge (DBD) at atmospheric pressure by means of ex-situ infrared absorption spectroscopy. CO mixing ratios of 0.1%–4.4% were determined for specific injected energies between 0.1 and 20¿eV per molecule (0.3–70¿kJ/l). A lower limit of the gas temperature of 320–480¿K was estimated from the wall temperature of the quartz reactor as measured with an infrared camera. The formation of CO in the DBD could be described as function of the total number of transferred charges during the residence time of the gas in the active plasma zone. An almost stoichiometric CO:O2 ratio of 2:1 was observed along with a strongly temperature dependent O3 production up to 0.075%. Although the ideal range for an efficient CO2 dissociation in plasmas of 1¿eV per molecule for the specific injected energy was covered, the energy efficiency remained below 5% for all conditions. The present results indicate a reaction mechanism which is initiated by electron impact processes followed by charge transfer reactions and non-negligible surface enhanced O and CO recombination. While electron-driven CO2 dissociation is relatively energy inefficient by itself, fast O recombination and the low gas temperatures inhibit the synergistic reuse of atomic oxygen in a secondary CO2¿+¿O dissociation step.

AB - The dissociation of CO2 and the formation of CO, O3, and O2 were studied in a dielectric barrier discharge (DBD) at atmospheric pressure by means of ex-situ infrared absorption spectroscopy. CO mixing ratios of 0.1%–4.4% were determined for specific injected energies between 0.1 and 20¿eV per molecule (0.3–70¿kJ/l). A lower limit of the gas temperature of 320–480¿K was estimated from the wall temperature of the quartz reactor as measured with an infrared camera. The formation of CO in the DBD could be described as function of the total number of transferred charges during the residence time of the gas in the active plasma zone. An almost stoichiometric CO:O2 ratio of 2:1 was observed along with a strongly temperature dependent O3 production up to 0.075%. Although the ideal range for an efficient CO2 dissociation in plasmas of 1¿eV per molecule for the specific injected energy was covered, the energy efficiency remained below 5% for all conditions. The present results indicate a reaction mechanism which is initiated by electron impact processes followed by charge transfer reactions and non-negligible surface enhanced O and CO recombination. While electron-driven CO2 dissociation is relatively energy inefficient by itself, fast O recombination and the low gas temperatures inhibit the synergistic reuse of atomic oxygen in a secondary CO2¿+¿O dissociation step.

U2 - 10.1063/1.4896132

DO - 10.1063/1.4896132

M3 - Article

VL - 116

SP - 123303-1/14

JO - Journal of Applied Physics

JF - Journal of Applied Physics

SN - 0021-8979

M1 - 123303

ER -