Microkinetic modelling and detailed reaction mechanisms

To design the new catalytic materials and improve their performance at industrial applications, the mechanisms enabled by the catalysts, mainly on transition- metal surface as an active component, have to be understood. Our efforts focus on the development and validation of the detailed heterogeneous reaction mechanisms for different catalytic processes and the coupling between the catalytic kinetics and transport phenomena into the combined transport-kinetic models needed for optimization of the process.
The development of detailed reaction mechanisms (microkinetic analysis) is evolved into a promising tool for modeling surface reactions. The main advantage of the detailed reaction modeling compared to traditional power-law approximation is that a mechanism developed at certain conditions is expected, in many cases, to capture system features under significantly different conditions. The procedure involves setting up a network of reactions including independent information about the rates of the elementary steps and the stability of the intermediates such as sticking coefficients, preexponential factors, entropies and enthalpies adsorption, surface bond energies, activation energies, and active site densities, which capture the essential features of surface-catalyzed chemistry. The mechanisms are evaluated against the experimental measurements at different catalyst types, operating conditions and reactor configurations. The development of such detailed mechanism-based models offers the possibility of predictive kinetics models providing the information about the governing chemistry and reactor behavior.
The detailed surface reaction mechanisms developed in our group and successfully used for the modeling and numerical simulation of the different catalytic processes such as catalytic combustion of methane over Pt coated honeycomb monolith and Pt foil [1], partial oxidation of methane for short-contact-time reactors using Rh monoliths [2], reforming and oxidation of methane on Ni/Al2O3 catalysts [3, 4] and within a Ni–YSZ SOFC anode support [5], catalytic partial oxidation of i-octane over Rh coated monolith catalysts [6, 7], and steam reforming of hexadecane over a Rh/CeO2 in microreactors [8], you can find on our web page: http://www.detchem.com/mechanisms.

Staff members involved: Lubow Maier, reaction mechanisms group
Contact person: Lubow Maier

Selected publications:
[1] O. Deutschmann, L. Maier, U. Riedel, A. H. Stroemann, R. W. Dibble, Catalysis Today 59 (2000) 141-150.
[2] O. Deutschmann, R. Schwiedernoch, L.I. Maier, D. Chatterjee, Natural Gas Conversion VI, Studies in Surface Science and Catalysis 136, E. Iglesia, J.J. Spivey, T.H. Fleisch (eds.), p. 215-258, Elsevier, 2001.
[3] L. Maier, B. Schädel, K. Herrera Delgado, S. Tischer, O. Deutschmann, Topics in Catalysis 54 (2011) 845-858.
[4] K. Herrera Delgado, H. Stotz, L. Maier, S. Tischer, A. Zellner, O. Deutschmann, Catalysts 5 (2015) 871-904.
[5] E. Hecht, G.K. Gupta, H. Zhu. A.M. Dean, R.J. Kee, L. Maier, O. Deutschmann, Applied Catalysis A: 295 (2005) 40–51
[6] L. Maier, M. Hartmann, S. Tischer, O. Deutschmann, Combustion and Flame, 158 (2011) 796-808.
[7] M. Hartmann, L. Maier, H.D. Minh, O. Deutschmann, Combustion and Flame, 157 (2010) 1771-1782
[8] J. Thormann, L. Maier, P. Pfeifer, U. Kunz, O. Deutschmann and K. Schubert, International Journal of Hydrogen Energy, Volume 34, Issue 12, (2009), p. 5108-5120