A New Model of Thermal Desorption of Nitrogen from a Nonhomogeneous Catalyst Surface

Computational Mathematics and Modeling - Tập 12 - Trang 91-106 - 2001
N. L. Semendyaeva, E. S. Kurkina

Tóm tắt

A new mathematical model is proposed for temperature recombination of atomic nitrogen on the (111) face of the iridium single crystal and on iridium foil, allowing for geometrical nonhomogeneity of the catalyst surface. The model describes the main qualitative features of laboratory experiments: the effect of the catalyst surface structure and the adsorbed oxygen on nitrogen thermal desorption spectra. Conditions are determined when an additional low-temperature peak appears in the N2 thermal desorption spectrum. The results are compared with calculations using traditional models of associative thermal desorption from homogeneous surfaces, including models that allow for lateral interactions in the adsorption layer. The numerical analysis is carried out using deterministic and stochastic approaches.

Tài liệu tham khảo

G. K. Boreskov, Heterogeneous Catalysis[in Russian], Nauka, Moscow (1986). V. P. Zhdanov, Elementary Physico-Chemical Processes on the Surface[in Russian], Nauka, Novosibirsk (1988). P. A. Zhdan, G. K. Boreskov, A. I. Boronin, A. P. Scheppelin, W. F. Egelhoff, Jr., and W. H. Weinberg, “ Nitric oxide adsorption and decomposition on the (111) and (110) surfaces of iridium, ” J. Catal., 60, 93 (1979). A. I. Boronin and P. A. Zhdan, “ Adsorption and electron state of CO, NO, O2on Pt and Ir: investigation by methods of photoelectron spectroscopy and thermal desorption, ” Izv. Akad. Nauk SSSR, Ser. Fiz., 46, 1247 (1982). A. I. Boronin, Investigation of Mechanisms of Catalytic Oxidation of Carbon Monoxide by Oxygen and Nitric Oxide on Iridium and Platinum by Methods of Photoelectron Spectroscopy and Thermal Desorption[in Russian], Candidate-Degree Thesis (Chemistry), Novosibirsk (1983). D. E. Ibbotson, T. S. Wittrig, and W. H. Weinberg, “ The chemisorption and decomposition of NO on the (110) surface of iridium, ” Surf. Sci., 110, 294 (1981). A. V. Myshlyavtsev and G. S. Yablonskii, “ Kinetic models of surface reactions with phase transformations of the adsorbed layer, ” in: Adsorption and Catalysis Mechanisms[in Russian], Institut Kataliza SO RAN, Novosibirsk (1989). A. G. Makeev and N. L. Semendyaeva, “ Comparison of stochastic and deterministic approaches to simulation of monomolecular thermal desorption, ” Matem. Modelirovanie 7, No. 3, 29 (1995). A. G. Makeev and M. M. Slinko, “ Mathematical modeling of the peculiarities of NO decomposition on Rh(111), ” Surf. Sci., 359, 1467 (1996). A. A. Samarskii and M. G. Slin'ko, “ Mathematical models of heterogeneous catalytic reactions and processes, ” Izv. RAN, Ser. Khim., 10, 1895 (1998). M. Yu. Smirnov and V. V. Gorodetskii, “ Investigation of the NO + H2and NH3+ O3reactions on Pt(111) by high-resolution electron energy loss spectroscopy and thermal desorption, ” in: Adsorption and Catalysis Mechanisms[in Russian], Institut Kataliza SO RAN, Novosibirsk (1989). J. C. L. Cornish and N. R. Avery, “ Adsorption of N2, O2, N2O on Ir(111) by EELS and TPD, ” Surf. Sci., 235, 209 (1990). A. I. Boronin and V. I. Elokhin, “Dynamics of surface processes over iridium in carbon monoxide oxidation reaction,” Proc. First Soviet-Chinese Seminar on CatalysisNovosibirsk (June 1990). D. N. Belton, C. L. DiMaggio, and K. Y. Simon Ng, “Reaction of coadsorbed nitric oxide and nitric atoms on Rh(111),” J. Catal., 144, 273 (1993). V. I. Savchenko, “Thermal desorption from a discretely nonhomogeneous surface,” Kinetika Kataliz 35, No. 3, 349 (1994). K. Binder (ed.), Monte Carlo Methods in Statistical Physics[Russian translation], Mir, Moscow (1982). H. Eyring, S. H. Lin, and S. M. Lin, Basic Chemical Kinetics[Russian translation], Mir, Moscow (1983). Yu. K. Tovbin, Theory of Physico-Chemical Processes on the Gas-Solid Interface[in Russian], Nauka, Moscow (1990). G. G. Elenin, “Mathematical modeling of heterogeneous catalytic reactions on faces of noble metal single crystals. Part I: Superstructures and phase transitions,” Ross. Khim. Zh., 40, No. 2, 19 (1996). P. A. Redhead, “Thermal desorption of gases,” Vacuum 12, No. 4, 203 (1962). C. W. Gear, Numerical Initial Value Problems in Ordinary Differential EquationsChap. 9, Prentice-Hall, Englewood Cliffs, NJ (1971). M. Roberts and C. McKee, Chemistry of the Metal-Gas Interface[Russian translation], Mir, Moscow (1981).