Hetero-/homogeneous combustion of hydrogen/air mixtures over platinum at pressures up to 10 bar

Abstract The hetero-/homogeneous combustion of fuel-lean hydrogen/air premixtures over platinum was investigated experimentally and numerically in the pressure range 1 bar ⩽  p  ⩽ 10 bar. Experiments were carried out in an optically accessible channel-flow catalytic reactor and included planar laser induced fluorescence (LIF) of the OH radical for the assessment of homogeneous (gas-phase) ignition, and 1-D Raman measurements of major gas-phase species concentrations for the evaluation of the heterogeneous (catalytic) processes. Simulations were performed with a full-elliptic 2-D model that included detailed heterogeneous and homogeneous chemical reaction schemes. The predictions reproduced the measured catalytic hydrogen consumption, the onset of homogeneous ignition at pressures of up to 3 bar and the diminishing gas-phase combustion at p  ⩾ 4 bar. The suppression of gaseous combustion at elevated pressures bears the combined effects of the intrinsic homogeneous hydrogen kinetics and of the hetero/homogeneous chemistry coupling via the catalytically produced water over the gaseous induction zone. Transport effects, associated with the large diffusivity of hydrogen, have a smaller impact on the limiting pressure above which gaseous combustion is suppressed. It is shown that for practical reactor geometrical confinements, homogeneous combustion is still largely suppressed at p  ⩾ 4 bar even for inlet and wall temperatures as high as 723 and 1250 K, respectively. The lack of appreciable gaseous combustion at elevated pressures is of concern for the reactor thermal management since homogeneous combustion moderates the superadiabatic surface temperatures attained during the heterogeneous combustion of hydrogen.

[1]  Olav Bolland,et al.  A quantitative comparison of gas turbine cycles with CO2 capture , 2007 .

[2]  D. Vlachos,et al.  Surface reaction mechanism development for platinum-catalyzed oxidation of methane , 2002 .

[3]  Dionisios G. Vlachos,et al.  Fabrication of Single-Channel Catalytic Microburners: Effect of Confinement on the Oxidation of Hydrogen/Air Mixtures , 2004 .

[4]  O. Deutschmann,et al.  Kinetic model of an oxygen‐free methane conversion on a platinum catalyst , 1999 .

[5]  Robert J. Kee,et al.  SURFACE CHEMKIN-III: A Fortran package for analyzing heterogeneous chemical kinetics at a solid-surface - gas-phase interface , 1996 .

[6]  J. Mantzaras,et al.  Turbulent catalytically stabilized combustion of hydrogen/air mixtures in entry channel flows , 2005 .

[7]  Frank Behrendt,et al.  NUMERICAL MODELING OF CATALYTIC IGNITION , 1996 .

[8]  Robert W. Dibble,et al.  HYDROGEN ASSISTED CATALYTIC COMBUSTION OF METHANE ON PLATINUM , 2000 .

[9]  L. Schmidt,et al.  The Effect of Ceramic Supports on Partial Oxidation of Hydrocarbons over Noble Metal Coated Monoliths , 1998 .

[10]  D. Vlachos,et al.  A C1 mechanism for methane oxidation on platinum , 2003 .

[11]  J. Mantzaras,et al.  High-pressure experiments and modeling of methane/air catalytic combustion for power-generation applications , 2003 .

[12]  J. Mantzaras,et al.  High-pressure catalytic combustion of methane over platinum: In situ experiments and detailed numerical predictions , 2004 .

[13]  L. Pfefferle,et al.  Catalytically stabilized combustion , 1986 .

[14]  Yohannes Ghermay,et al.  Experimental and numerical investigation of hetero-/homogeneous combustion of CO/H2/O2/N2 mixtures over platinum at pressures up to 5 bar , 2011 .

[15]  M. Allendorf,et al.  Understanding Homogeneous and Heterogeneous Contributions to the Platinum-Catalyzed Partial Oxidation of Ethane in a Short-Contact-Time Reactor , 2000 .

[16]  O. Deutschmann,et al.  Detailed surface reaction mechanism for Pt-catalyzed abatement of automotive exhaust gases , 2009 .

[17]  Konstantinos Boulouchos,et al.  Hetero-/homogeneous combustion and stability maps in methane-fueled catalytic microreactors☆ , 2007 .

[18]  G. G. Stokes "J." , 1890, The New Yale Book of Quotations.

[19]  R. J. Kee,et al.  Chemkin-II : A Fortran Chemical Kinetics Package for the Analysis of Gas Phase Chemical Kinetics , 1991 .

[20]  N. Malik,et al.  The chemistry of ethane dehydrogenation over a supported platinum catalyst , 2008 .

[21]  Timothy Griffin,et al.  Catalytic combustion for power generation , 2002 .

[22]  John Mantzaras,et al.  Catalytic Combustion of Syngas , 2008 .

[23]  D. Vlachos,et al.  A reduced mechanism for methane and one-step rate expressions for fuel-lean catalytic combustion of small alkanes on noble metals , 2007 .

[24]  Robert J. Kee,et al.  A FORTRAN COMPUTER CODE PACKAGE FOR THE EVALUATION OF GAS-PHASE, MULTICOMPONENT TRANSPORT PROPERTIES , 1986 .

[25]  Rolf Bombach,et al.  Homogeneous ignition in high-pressure combustion of methane/air over platinum: Comparison of measurements and detailed numerical predictions , 2002 .

[26]  Catalytic combustion of methane/air mixtures over platinum: Homogeneous ignition distances in channel flow configurations , 2000 .

[27]  Peter Benz,et al.  An asymptotic and numerical investigation of homogeneous ignition in catalytically stabilized channel flow combustion , 1999 .

[28]  Zhenwei Zhao,et al.  An updated comprehensive kinetic model of hydrogen combustion , 2004 .

[29]  E. M. Bulewicz Combustion , 1964, Nature.

[30]  Robert J. Kee,et al.  A model of elementary chemistry and fluid mechanics in the combustion of hydrogen on platinum surfaces , 1994 .

[31]  L. Schmidt,et al.  A Multistep Surface Mechanism for Ethane Oxidative Dehydrogenation on Pt- and Pt/Sn-Coated Monoliths , 2005 .

[32]  R. Grabowski Kinetics of Oxidative Dehydrogenation of C2‐C3 Alkanes on Oxide Catalysts , 2006 .

[33]  J. Mantzaras,et al.  An experimental and numerical investigation of homogeneous ignition in catalytically stabilized combustion of hydrogen/air mixtures over platinum , 2002 .

[34]  F. Zaera,et al.  Kinetic study of the catalytic oxidation of alkanes over nickel, palladium, and platinum foils , 1997 .

[35]  Peter Benz,et al.  Two-dimensional modelling for catalytically stabilized combustion of a lean methane-air mixture with elementary homogeneous and heterogeneous chemical reactions , 1999 .

[36]  J. Mantzaras,et al.  Gas phase chemistry in catalytic combustion of methane/air mixtures over platinum at pressures of 1 to 16 bar , 2005 .

[37]  Konstantinos Boulouchos,et al.  EFFECTS OF H2O AND CO2 DILUTION ON THE CATALYTIC AND GAS-PHASE COMBUSTION OF METHANE OVER PLATINUM AT ELEVATED PRESSURES , 2007 .

[38]  Konstantinos Boulouchos,et al.  Experimental and Numerical Investigation of the Hetero-/Homogeneous Combustion of Lean Propane/Air Mixtures Over Platinum , 2009 .

[39]  Jörg Frauhammer,et al.  Modelling steady state and ignition during catalytic methane oxidation in a monolith reactor , 2000 .