The ignition of catalytic combustion of the stoichiometric propane/air mixture on an isothermally heated platinum wire in different experimental conditions of total pressure and wire temperature is studied and discussed on the basis of a simplified kinetic model. The platinum wire is heated electrically with a specially designed power supply, which ensures a quasi-rectangular profile of its temperature. The ignition process is monitored by measuring the input power required to maintain a constant temperature of the wire during an exothermic catalytic reaction. The difference between the input powers recorded in air and in a fuel/air mixture, for the same wire temperature and gas total pressure, allows the elimination of the heat transferred to surroundings and conversion of the results into the catalytic reaction rate rR versus time curves of S-shaped form, illustrating the transition from kinetic to diffusion regime. The curve can be used to evaluate the ignition delay, as reported previously and also to fit different models to the data. The quasi-exponential increase of the isothermal reaction rate during the early stages of the process can be rationalized on the basis of a simplified kinetic model implying the multiplication of the adsorbed active intermediates. The adopted hypotheses allow the derivation of an analytical solution for the catalytic reaction rate before and during the ignition process, without diffusion limitations.
1. Pfefferle, LD, Pfefferle, WC. Catalysis in combustion. Catal Rev Sci Eng 1987 29:219–267 .
2. Powell, F. Ignition of gases and vapors. Ind Eng Chem. 1969;61:29–37 .
3. Laurendeau, NM. Thermal ignition of methane-air mixtures by hot surfaces: a critical examination. Combust Flame. 1982;46:29–49 .
4. Arpentinier, Ph, Cavani, F, Trifiro, F. The contribution of homogeneous reactions in catalytic oxidation processes: safety and selectivity aspects. Catal Today 2005 99:15–22 .
5. Saint-Just, J, der Kinderen, J. Catalytic combustion: from reaction mechanism to commercial applications. Catal Today 1996 29:387–395 .
6. Forzatti, P, Groppi, G. Catalytic combustion for the production of energy. Catal Today 1999 54:165–180 .
7. Carroni, R, Schmidt, V, Griffin, T. Catalytic combustion for power generation. Catal Today 2002 75:287–295 .
8. Tahir, SF, Koh, CA. Catalytic destruction of volatile organic compound emissions by platinum based catalyst. Chemosphere 1999 38:2109–2116 .
9. O’Malley, A, Hodnett, BK. The influence of volatile organic compound structure on conditions required for total oxidation. Catal Today 1999 54:31–38 .
10. Garetto, TF, Apesteguía, CR. Oxidative catalytic removal of hydrocarbons over Pt/Al2O3 catalysts. Catal Today 2000 62:189–199 .
11. Shijie, L, Weiyong, Y, Dingye, F, Hideo, K. Kinetics of catalytic combustion in air over Pt/Al2O3/Al catalyst. React Kinet Catal Lett 2005 85:205–213 .
12. Twigg, MV. Roles of catalytic oxidation control of vehicle exhaust emissions. Catal Today. 2006;117:407–418 .
13. Griffin, TA, Pfefferle, LD. Gas phase and catalytic ignition of methane and ethane in air over platinum. AIChE J 1990 36:861–870 .
14. Veser, G, Schmidt, LD. Ignition and extinction in the catalytic oxidation of hydrocarbons over platinum. AIChE J 1996 42:1077–1087 .
15. Veser, G, Ziauddin, M, Schmidt, LD. Ignition in alkane oxidation on noble-metal catalysts. Catal Today 1999 47:219–228 .
16. Alkidas, A, Durbetaki, P. Ignition of a gaseous mixture by a heated surface. Combust Sci Technol 1973 7:135–140 .
17. Song, X, Williams, WR, Schmidt, LD, Aris, R. Ignition and extinction of homogeneous–heterogeneous combustion: CH4 and C3H8 oxidation on Pt. Proc Combust Inst 1990 23:1129–1137.
18. Vlachos, DG. Homogeneous–heterogeneous oxidation reactions over platinum and inert surfaces. Chem Eng Sci. 1996;51:2429–2438 .
19. Rinnemo, M, Deutschmann, O, Behrendt, F, Kasemo, B. Experimental and numerical investigation of the catalytic ignition of mixtures of hydrogen and oxygen on platinum. Combust Flame 1997 111:312–326 .
20. Oancea, D, Staicu, O, Munteanu, V, Razus, D. Catalytic combustion of the stoichiometric n-butane/air mixture on isothermally heated platinum wire. Catal Lett 2008 121:247–254 .
21. Staicu, O, Munteanu, V, Oancea, D. The effect of operational parameters on the catalytic combustion of n-butane/air mixture on platinum wire. Catal Lett 2009 129:124–129 .
22. Staicu, O, Munteanu, V, Oancea, D. Overall kinetics for the catalytic ignition of ethane-air mixtures on platinum. Studia Universitatis Babes Bolyai Chem 2009 54:193–202.
23. Staicu, O, Razus, D, Munteanu, V, Oancea, D. Heterogeneous catalytic ignition of n-butane/air mixture on platinum. Cent Eur J Chem 2009 7:478–485 .
24. Oancea D , Munteanu V, Razus D. Isothermal catalytic combustion of n-pentane/air mixtures on platinum wire. J Therm Anal Calorim. 2010;102: 993–1000.
25. Oancea, D, Staicu, O, Munteanu, V. Kinetics of isothermal ignition of propane/air mixtures on platinum. Rev Roumaine Chim 2010 55:211–216.
26. Garetto, TF, Rincón, E, Apesteguía, CR. Deep oxidation of propane on Pt-supported catalysts: drastic turnover rate enhancement using zeolite supports. Appl Catal B Environ 2004 48:167–174 .
27. Frank-Kamenetskii, DA Diffusion and heat transfer in chemical kinetics, chap 1 1969 Plenum Press New York.
28. Oancea, D, Razus, D, Mitu, M, Constantinescu, S. Hot wire ignition of premixed flammable fuel-air mixtures using isothermally heated platinum wires. Rev Roumaine Chim 2002 47:91–97.
29. Peng, YK, Dawson, PT. The adsorption, desorption, and exchange reactions of oxygen, hydrogen, and water on platinum surfaces. I. Oxygen interaction. Can J Chem 1974 52:3507–3517 .
30. Deutschmann, O, Behrendt, F, Warnatz, J. Formal treatment of catalytic combustion and catalytic conversion of methane. Catal Today 1998 46:155–163 .
31. Reinke, M, Mantzaras, J, Schaeren, R, Bombach, R, Inauen, A, Schenker, S. High-pressure catalytic combustion of methane over platinum: in situ experiments and detailed numerical predictions. Combust Flame 2004 136:217–240 .
32. Warnatz, J, Maas, U, Dibble, RW Combustion, chap 6 Springer Berlin, Heidelberg 1999.
33. Vannice, MA Kinetics of catalytic reactions, chap 5 2005 Springer New York.
34. Oxley JC , Smith JL, Marimaganti K. Developing small-scale tests to predict explosivity. J Therm Anal Calorim. 2010. doi: .
35. Shen S-J , Wu S-H, Chi J-H, Wang Y-W, Shu C-M. Thermal explosion simulation and incompatible reaction of dicumyl peroxide by calorimetric technique. J Therm Anal Calorim. 2010. doi: .
36. Heynderickx, MP, Thybaut, JW, Poelman, H, Poelman, D, Marin, GB. Kinetic modeling of the total oxidation of propane over CuO–CeO2/g-Al2O3. Appl Catal B 2010 95:26–38 .
37. Kaisare, NS, Deshmukh, SR, Vlachos, DG. Stability and performance of catalytic microreactors: simulations of propane catalytic combustion on Pt. Chem Eng Sci 2008 63:1098–1116 .