Identification of copper species present in Cu-ZSM-5 catalysts for NOx reduction

Millar, Graeme J., Canning, A., Rose, G., Wood, B., Trewartha, L., & Mackinnon, Ian D. R. (1999) Identification of copper species present in Cu-ZSM-5 catalysts for NOx reduction. Journal of Catalysis, 183(2), pp. 169-181.

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The structure of Cu-ZSM-5 catalysts that show activity for direct NO decomposition and selective catalytic reduction of NOx by hydrocarbons has been investigated by a multitude of modern surface analysis and spectroscopy techniques including X-ray photoelectron spectroscopy, thermogravimetric analysis, and in situ Fourier transform infrared spectroscopy. A series of four catalysts were prepared by exchange of Na-ZSM-5 with dilute copper acetate, and the copper loading was controlled by variation of the solution pH. Underexchanged catalysts contained isolated Cu2+OH-(H2O) species and as the copper loading was increased Cu2+ ions incorporated into the zeolite lattice appeared. The sites at which the latter two copper species were located were fundamentally different. The Cu2+OH-(H2O) moieties were bound to two lattice oxygen ions and associated with one aluminum framework species. In contrast, the Cu2+ ions were probably bound to four lattice oxygen ions and associated with two framework aluminum ions. Once the Cu-ZSM-5 samples attained high levels of exchange, the development of [Cu(μ-OH)2Cu]n2+OH-(H2O) species along with a small concentration of Cu(OH)2 was observed. On activation in helium to 500°C the Cu2+OH-(H2O) species transformed into Cu2+O- and Cu+ moieties, whereas the Cu2+ ions were apparently unaffected by this treatment (apart from the loss of ligated water molecules). Calcination of the precursors resulted in the formation of Cu2+O2- and a one-dimensional CuO species. Temperature-programmed desorption studies revealed that oxygen was removed from the latter two species at 407 and 575°C, respectively. © 1999 Academic Press.

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ID Code: 57455
Item Type: Journal Article
Refereed: Yes
Additional Information: Cited By (since 1996): 27 Export Date: 19 February 2013 Source: Scopus Language of Original Document: English Correspondence Address: Millar, G.J.; Department of Chemistry, University of Queensland, Brisbane, QLD 4072, Australia; email: References: Taylor, K.C., (1993) Catal. Rev. Sci. Eng., 35, p. 457; Shelef, M., (1995) Chem Rev., 95, p. 209; Armor, J.N., (1995) Catal. Today, 26, p. 147; Walker, A.P., (1995) Catal. Today, 26, p. 107; Kharas, K.C., Liu, D.-J., Robota, H.J., (1995) Catal. Today, 26, p. 129; Iwamoto, M., Yahiro, H., Mine, Y., Kagawa, S., (1989) Chem. Lett., p. 213; Grinsted, R.A., Jen, H.-W., Montreuil, C.N., Rokosz, M.J., Shelef, M., (1993) Zeolites, 13, p. 602; Centi, G., Perathoner, S., (1995) Appl. Catal. A, 132, p. 179; Liu, D.-J., Robota, H.J., (1993) Catal. Lett., 21, p. 291; Liu, D.-J., Robota, H.J., (1994) Appl. Catal. B, 4, p. 155; Jang, H.-J., Hall, W.K., D'Itri, J., (1996) J. Phys. Chem., 100, p. 9416; Valyon, J., Hall, W.K., (1993) J. Phys. Chem., 97, p. 7054; Valyon, J., Hall, W.K., (1993) J. Catal., 143, p. 520; Sarkany, J., D'Itri, J.L., Sachtler, W.M.H., (1992) Catal. Lett., 16, p. 241; Lei, G.D., Adelman, B.J., Sarkany, J., Sachtler, W.M.H., (1995) Appl. Catal. B, 5, p. 245; Larsen, S.C., Aylor, A.W., Bell, A.T., Reimer, J.A., (1994) J. Phys. Chem., 98, p. 11533; Aylor, A.W., Larsen, S.C., Reimer, J.A., Bell, A.T., (1995) J. Catal., 157, p. 592; Chang, Y.-F., McCarty, J.G., (1997) J. Catal., 165, p. 1; Zhang, Y., Leo, K.M., Sarofim, A.F., Hu, Z., Flytzani-Stephanopoulos, M., (1995) Catal. Lett., 31, p. 75; Haack, L.P., Shelef, M., (1993) Proceedings of the Symposium on Catalytic Reduction of NOx, ACS Spring Meeting, , Denver, March; Grunert, W., Hayes, N.W., Joyner, R.W., Shapiro, E.S., Rafiq, M., Siddiqui, H., Baeva, G.N., (1994) J. Phys. Chem., 98, p. 10832; Basu, P., Ballinger, T.H., Yates, J.T., (1998) Rev. Sci. Instrum., 59, p. 1321; Wagner, C.D., Riggs, W.M., Davis, L.E., Moulder, J.F., (1979) The Handbook of X-ray Photoelectron Spectroscopy, p. 82. , G. E. Muilenberg, Ed., Perkin-Elmer Corp; Frost, J.C., (1988) Nature, 334, p. 577; Kuroda, Y., Kotani, A., Maeda, H., Moriwaki, H., Morimato, T., Nagao, M., (1992) J. Chem. Soc. Faraday Trans., 88, p. 1583; Schoonheydt, R.A., Vandamme, L.J., Jacobs, P.A., Uytterhoeven, J.B., (1976) J. Catal., 43, p. 292; Anpo, M., Matsuoka, M., Shioya, Y., Yamashita, H., Giamello, E., Morterra, C., Che, M., Fox, M.A., (1994) J. Phys. Chem., 98, p. 5744; Spoto, G., Zecchina, A., Bordiga, S., Ricchiardi, G., Martra, G., Loefanti, G., Petrini, G., (1994) Appl. Catal. B, 3, p. 151; Centi, G., Nigro, C., Perathoner, S., (1994) React. Kinet. Catal. Lett., 53, p. 79; Lokhov, Yu.A., Sadykov, V.A., Tikhov, S.F., Popouskii, V.V., (1985) Kinet. Katal., 26, p. 152; Giamello, E., Murphy, D., Magnacca, G., Morterra, C., Shioya, Y., Nomura, T., Anpo, M., (1992) J. Catal., 136, p. 510; Kucherov, A.V., Gerlock, J.L., Jen, H.-W., Shelef, M., (1994) J. Phys. Chem., 98, p. 4892; Parillo, D.J., Dolenec, D., Gorte, R.J., McCabe, R.W., (1993) J. Catal., 142, p. 708; Okamoto, Y., Fukino, K., Imanaka, T., Teranishi, S., (1983) J. Phys. Chem., 87, p. 3740; Trout, B.L., Chakraborty, A.K., Bell, A.T., (1996) J. Phys. Chem., 100, p. 4173; Nomura, M., Kazusaka, A., Kakuta, N., Ukisu, Y., Miyahara, K., (1987) J. Chem. Soc. Faraday Trans. 1, 83, p. 1227; Kakuta, N., Kazusaka, A., Miyahara, K., (1986) Bull. Chem. Soc. Japan, 59, p. 3267; Nomura, M., Kazusaka, A., Ukisu, Y., Kakuta, N., (1987) J. Chem. Soc. Faraday Trans. 1, 83, p. 2635; Kakuta, N., Kazusaka, A., Yamazaki, A., Miyahara, K., (1984) J. Chem. Soc. Faraday Trans. 1, 80, p. 3245; Anderson, M.W., Kevan, L., (1987) J. Phys. Chem., 91, p. 4174; Hadjiivanov, K., Klissurski, D., Ramis, G., Busca, G., (1996) Appl. Catal. B, 7, p. 251; Attfield, M.P., Weigel, S.J., Cheetham, A.K., (1997) J. Catal., 170, p. 227; Attfield, M.P., Weigel, S.J., Cheetham, A.K., (1997) J. Catal., 172, p. 274
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Keywords: ion exchanged ZSM-5, methanol synthesis catalysts, selective reduction, nitric oxide, spectroscopic characterisation, acetate monohydrate, nitrogen oxides
DOI: 10.1006/jcat.1999.2391
ISSN: 1090-2694 (online) 0021-9517 (print)
Subjects: Australian and New Zealand Standard Research Classification > CHEMICAL SCIENCE (030000) > PHYSICAL CHEMISTRY (INCL. STRUCTURAL) (030600) > Catalysis and Mechanisms of Reactions (030601)
Australian and New Zealand Standard Research Classification > CHEMICAL SCIENCE (030000) > PHYSICAL CHEMISTRY (INCL. STRUCTURAL) (030600) > Structural Chemistry and Spectroscopy (030606)
Divisions: Current > Schools > School of Chemistry, Physics & Mechanical Engineering
Current > Institutes > Institute for Future Environments
Current > QUT Faculties and Divisions > Science & Engineering Faculty
Copyright Owner: Copyright 1999 Academic Press All rights of reproduction in any form reserved.
Deposited On: 25 Feb 2013 21:52
Last Modified: 25 Feb 2013 21:52

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