Abstract
FT-IR spectroscopy and mass spectrometry have been used to study the adsorption and decomposition of nitrous oxide on zirconia. It was determined that zirconia cations in the 4+ oxidation state are the site for molecular adsorption of N2O, whereas Zr3+ sites are active toward dissociative adsorption of N2O at temperatures as low as 25°C. Catalytic decomposition of N2O on ZrO2 occurs at temperatures above 350°C and follows first-order reaction kinetics. Experiments utilizing isotopic labeling in conjunction with mass spectrometry were done to elucidate the details of the reaction mechanism. Based on the results presented here, a mechanism for N2O decomposition on ZrO2 is proposed.
Similar content being viewed by others
References
M.H. Theimens and W.C. Trogler, Science 251 (1991) 932.
R. Reimer, C.S. Slaten, M. Seapan, M.W. Lower and P.E. Tomlinson, Environm. Progr. 13 (1994) 134.
T.M. Miller and V.H. Grassian, J. Am. Chem. Soc. 117 (1995) 10969.
K. Anseth and T.A. Koch, US Patent 5314673.
H.C. Zeng, J. Lin, W.K. Teo, J.C. Wu and K.L. Tan, J. Mater. Res. 10 (1995) 545.
V.E. Henrich and P.A. Cox, The Surface Science of Metal Oxides (Cambridge University Press, Cambridge, 1994).
M.A. Barteau, J. Vac. Soc. Technol. A11 (1993) 2162.
A.A. Davydov, Infrared Spectroscopy of Adsorbed Species on the Surface of Transition Metal Oxides, ed. C.H. Rochester (Wiley, NewYork, 1990).
C. Morterra, E. Giamello, L. Orio and M. Volante, J. Phys. Chem. 94 (1990) 3111.
Z.X. Liu, Q.X. Bao and N.J. Wu, J. Catal. 113 (1988) 45.
J. Haber and E.M. Serwicka, React. Kinet. Catal. Lett. 35 (1987) 369.
J.B. Black, J.D. Scott, E.M. Serwicka and J.B. Goodenough, J. Catal. 106 (1987) 16.
Z.X. Liu, K. Xie, Y.Q. Li and Q.X. Bao, J. Catal. 119 (1989) 249.
M.E. Lashier and G.L. Schrader, J. Catal. 128 (1991) 113.
T. Jin, T. Okuhara, G.J. Mainsand and J.M. White, J. Phys. Chem. 91 (1987) 3310.
P. Basu, T.H. Ballinger and J.T. Yates Jr., Rev. Sci. Instrum. 59 (1988) 1321.
T. Yamaguchi, Catal. Today 20 (1994) 199.
K.-H. Jacob, E. Knozinger and S. Benfer, J. Chem. Soc. Faraday Trans. 90 (1994) 2969.
C. Morterra, L. Orio and C. Emanuel, J. Chem. Soc. Faraday Trans. 86 (1990) 3003.
(a) E.R.S. Winter, J. Catal. 15 (1969) 144; (b) E.R.S. Winter, J. Catal. 34 (1974) 431.
S.L. Raj, B. Viswanathan, and V. Srinivasan, Ind. J. Chem. 21A (1982) 689.
J.F. Read, J. Catal. 28 (1973) 428.
A. Cimino, V. Indova, F. Pepe and F.S. Stone, Gaz. Chim. Ital. 103 (1973) 935.
Y. Yanagisawa, K. Takaoka and S. Yamabe, J. Chem. Soc. Faraday Trans. 90 (1994) 2561.
R. Stevens, Zirconia and Zirconia Ceramics (Magnesium Elektron, 1986).
K. Aika and E. Iwamatsu, in: Studies in Surface Science and Catalysis, Vol. 90, eds. H. Hattori, M. Misono and Y. Ono (Elsevier, Amsterdam, 1994).
Y.-X. Li and K. Klabunde, Chem. Mater. 4 (1992) 611.
G.K. Boreskov, Adv. Catal. 15 (1964) 285.
G.K. Boreskov, Discuss. Faraday Soc. 41 (1966) 263.
L.G. Harrison and J.A. Morrison, J. Phys. Chem. 62 (1958) 372.
Z. Sojka and M. Che, J. Phys.Chem. 100 (1996) 4776.
Rights and permissions
About this article
Cite this article
Miller, T., Grassian, V. A mechanistic study of nitrous oxide adsorption and decomposition on zirconia. Catalysis Letters 46, 213–221 (1997). https://doi.org/10.1023/A:1019058232683
Issue Date:
DOI: https://doi.org/10.1023/A:1019058232683