Balcaen, Veerle

Marin, Guy

Poelman, Dirk

Poelman, Hilde

Roelant, Raf

Ghent University Academic Bibliography

On the role of CO2 in the total oxidation of propane over a CuO-CeO2/Al2O3 catalyst

6WCOC, Lille, France, July 5-10, 2009TAP-study on the total oxidation of propane over a CuO-CeO2/γ-Al2O3 catalyst1http://www.lct.ugent.beLaboratory for Chemical TechnologyV. Balcaen, R. Roelant, H. Poelman, D. Poelman, G.B. Marin+ 5 O2  3 CO2 + 4 H2O• VOCs = Volatile Organic Compounds  important air pollutantsV. Balcaen, 6WCOC, Lille, France, July 5-10, 2009IntroductionTotal catalytic oxidationC3H8C H1 23CO2O OO2CuO-CeO2/γ-Al2O33 81. Which species are responsible for converting propane to CO2?2. What is the role of the different metal oxide phases?CO2V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Outline1. Introduction2. Experimental set-up, conditions and catalysts3. Results3• Role and nature of active oxygen species • Oxygen mobility • Role of metal oxides 4. ConclusionsV. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Three types of TAP pulse experimentsInlet Outlet ResponseSingle-pulse=State-defining00.20.40.60.810 5 10 15Tijd (s)00.20.40.60.810 5 10 15Tijd (s)00.20.40.60.810 0.5 1 1.5Tijd (s)4Multi-pulse= State-alteringAlternatingpulse00.20.40.60.810 5 10 15Tijd (s)00.20.40.60.810 5 10 15Tijd (s)00.20.40.60.810 5 10 15Tijd (s)00.20.40.60.810 5 10 15Tijd (s)00.20.40.60.810 5 10 15Tijd (s)00.20.40.60.810 0.5 1 1.5 2 2.5Tijd (s)0 Li Li+Lc Li+Lc+Loquartz quartzcatV. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Experimental conditionsC3H8 / Kr O2 / ArCO2 / ArC18O2 / Ar523 K < T < 923 K50 mgO atoms related to CuO and/or CeO Al O5Upper limit for the total number of exchangeable O atomspre-treatment of catalyst sample heating to reaction temperature (5K/min) multi-pulses of O2 until constant level of oxygen reponse2(1019)2 3(1019)CuO-CeO2/γ-Al2O3 7 70CeO2/γ-Al2O3 2 80CuO/θ-Al2O3 5 70V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Participation of lattice oxygen at surfacequartzdiffusion only623 K6higher interactionmo conversion304050conversion  [%]V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Participation of adsorbed oxygen species623 K010200.00 0.05 0.10 0.15 0.20C3H8conversion  [%]mol O consumed  / mol O in CuO and CeO2 [-]pure C3H8C3H8 + O27673 K, delay = 0.5 s0.01.02.03.04.05.0Flow rate [10-8 mol/s]O2propaneCO2V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Life time of adsorbed oxygen species0 0.5 1 1.5 2 2.5 3Time [s]8V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Fast diffusion of oxygen species873 K3456mol of isotopes at reactor outlet mol]Ar90120.00 0.10 0.20 0.30 0.40 0.50 0.60 0.70mol of isotopes at reactor outlet [10-8mol 18O consumed / mol 16O in Al2O3 [-]C1802C160180C1602C160C180V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Participation of lattice oxygen from bulkwithout introducing any gas923 K10V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009CO2 as oxidant623 K304050conversion  [%]11010200.00 0.05 0.10 0.15 0.20C3H8conversion  [%]mol O consumed  / mol O in CuO and CeO2 [-]pure C3H8C3H8 + O2C3H8 + CO2V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009O produced from CO2873 K12V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Location of active speciesCuO-CeO2/γ-Al2O3 CeO2/γ-Al2O3 CuO/θ-Al2O3γ-Al2O3 θ-Al2O37%623 K1334%29%V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009CO2 adsorption on aluminaCuO-CeO2/γ-Al2O3 CeO2/γ-Al2O3 CuO/θ-Al2O3γ-Al2O3 θ-Al2O3Mo, CO2 Mo, Ar< Irreversible adsorption623 K14V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009Conclusions• Four origins of active oxygen species, participating in total oxidation reaction1. Lattice oxygen at surface2. Lattice oxygen in bulk3. Surface oxygen produced from gas-phase O2154. Lattice oxygen produced from gas-phase CO2• Location of these active oxygen species1. CuO and CeO2  active phases  contain active O species2. γ-Al2O3  carrier  can produce active O species based on CO2V. Balcaen, 6WCOC, Lille, France, July 5-10, 2009This work was performed in the framework of aConcerted Research Action (Ghent University) 16Thank you for your attention!veerle.balcaen@ugent.be http://www.lct.ugent.be

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TAP study on the total oxidation of propane over a CuO-CeO2/gamma-Al2O3 catalyst

https://biblio.ugent.be/publication/787780/file/813706

On the role of CO2 in the total oxidation of propane over a CuO-CeO2/Al2O3 catalyst

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Ghent University Academic Bibliography

Ghent University Academic Bibliography