magnetic behavior; nano-clusters; nanoparticles; sol-gel (xerogels); iron; Mossbauer effect and spectroscopy
Abstract :
[en] Fe/SiO2 catalysts have been prepared by two different sol-gel methods, cogelation and dissolution. The cogelation and dissolution preparative methods lead to xerogels with fundamentally different pore width distributions. The nature of the iron species obtained has been examined in detail by UN-visible and Mossbauer spectroscopy, and magnetic, transmission electron microscopy, and X-ray diffraction studies. There is no evidence for the presence of any ordered iron(III) oxides in the samples but all three contain two types of iron species, specifically paramagnetic high-spin iron(III) ions isolated in silica and iron(III) containing nanoparticles with a broad width distribution centered on 1.5 nm, nanoparticles that contain antiferromagnetically coupled clusters of a few ligated bridged iron(III) ions. (C) 2007 Elsevier B.V. All rights reserved.
Disciplines :
Materials science & engineering Chemistry Physics
Author, co-author :
Heinrichs, Benoît ; Université de Liège - ULiège > Département de chimie appliquée > Génie chimique - Chimie physique appliquée
Rebbouh, Leila; Université de Liège - ULiège > Département de physique
Geus, John W; Universiteit Utrecht
Lambert, Stéphanie ; Université de Liège - ULiège > Département de chimie appliquée > Ingéniérie électrochimique
Abbenhuis, Hendrikus C L; Eindhoven University
Grandjean, Fernande ; Université de Liège - ULiège > Département de physique > Département de physique
Long, Gary J; University of Missouri-Rolla
Pirard, Jean-Paul ; Université de Liège - ULiège > Département de chimie appliquée > Génie chimique - Chimie physique appliquée
van Santen, Rutger A; Eindhoven University
Language :
English
Title :
Iron(III) species dispersed in porous silica through sol-gel chemistry
Brinker C.J., and Scherer G.W. Sol-Gel Science: The Physics and Chemistry of Sol-Gel Processing (1990), Academic Press, San Diego
Weckhuysen B.M., and Schoonheydt R.A. Catal. Today 49 (1999) 441
Lecloux A.J. In: Anderson J.R., and Boudart M. (Eds). Catalysis: Science and Technology vol. 2 (1981), Springer, Berlin 171
Pirard R., Alié C., and Pirard J.-P. In: Sakka S. (Ed). Characterization of Sol-Gel Materials and Products. Handbook of Sol-Gel Technology vol. 2 (2004), Kluwer, Dordrecht 211
Mikhail R.S., Brunauer S., and Bodor E.E. J. Colloid Interface Sci. 26 (1968) 45, 54
Broekhoff J.C.P., and de Boer J.H. J. Catal. 9 (1967) 8
Broekhoff J.C.P., and de Boer J.H. J. Catal. 9 (1967) 15
Broekhoff J.C.P., and de Boer J.H. J. Catal. 10 (1968) 153
Washburn E.W. Proc. Natl. Acad. Sci. 7 (1921) 115
Pirard R., Blacher S., Brouers F., and Pirard J.-P. J. Mater. Res. 10 (1995) 2114
Bordiga S., Buzzoni R., Geobaldo F., Lamberti C., Giamello E., Zecchina A., Leofanti G., Petrini G., Tozzola G., and Vlaic G. J. Catal. 158 (1996) 486
Centi G., Fazzini F., Fierro J.L.G., Lopèz Granados M., Sanz R., and Serrano D. Stud. Surf. Sci. Catal. 118 (1998) 577
Maxim N., Overweg A., Kooyman P.J., van Wolput J.H.M.C., Hanssen R.W.J.M., van Santen R.A., and Abbenhuis H.C.L. J. Phys. Chem. B 106 (2002) 2203
Hensen E.J.M., Zhu Q., Hendrix M.M.R.M., Overweg A.R., Kooyman P.J., Sychev M.V., and van Santen R.A. J. Catal. 221 (2004) 560
Tippins H.H. Phys. Rev. B 1 (1970) 126
Ribera A., Arends I., de Vries S., Perez-Ramirez J., and Sheldon R.A. J. Catal. 195 (2000) 287
Le Caër G., and Dubois J.M. J. Phys. E 12 (1979) 1083
Cannas C., Gatteschi D., Musinu A., Piccaluga G., and Sangregorio C. J. Phys. Chem. B 102 (1998) 7721
Cannas C., Musinu A., Peddis D., and Piccaluga G. Chem. Mater. 18 (2006) 3835
Zboril R., Machala L., Mashlan M., and Sharma V. Cryst. Growth Des. 4 (2004) 1317
Heinrichs B., Noville F., and Pirard J.-P. J. Catal. 170 (1997) 366
Lambert S., Alié C., Pirard J.-P., and Heinrichs B. J. Non-Cryst. Solids 342 (2004) 70
Lambert S., Sacco L., Ferauche F., Heinrichs B., Noels A., and Pirard J.-P. J. Non-Cryst. Solids 343 (2004) 109
Alié C., Pirard R., Lecloux A.J., and Pirard J.-P. J. Non-Cryst. Solids 246 (1999) 216
Gommes C.J., de Jong K., Pirard J.-P., and Blacher S. Langmuir 21 (2005) 12378
Heinrichs B., Geus J.W., Lambert S., and Pirard J.-P. J. Catal. 241 (2006) 229
Ramesh S., Felner I., Koltypin Y., and Gedanken A. J. Mater. Res. 15 (2000) 944
Cannas C., Casula M.F., Concas G., Corrias A., Gatteschi D., Falqui A., Musinu A., Sangregorio C., and Spano G. J. Mater. Chem. 11 (2001) 3180
Casas Ll., Roig A., Molins E., Grenèche J.M., Asenjo J., and Tejada J. Appl. Phys. A 74 (2002) 591
Predoi D., Kuncser V., Zaharescu M., Keune W., Sahoo B., Valeanu M., Crisan M., Raileanu M., Jitianu A., and Filoti G. Phys. Status Solidi (c) 1 (2004) 3507
Cannas C., Concas G., Congiu F., Musinu A., Piccaluga G., and Spano G. Z. Naturforsch. 57a (2002) 154
Rebbouh L., Rosso V., Renotte Y., Lion Y., Grandjean F., Heinrichs B., Pirard J.-P., Delwiche J., Hubin-Franskin M.-J., and Long G.J. J. Mater. Sci. 41 (2006) 2839
S. Mørup, Paramagnetic and Superparamagnetic Relaxation Phenomena Studied by Mössbauer Spectroscopy, Polyteknisk Forlag, 1981.
Hoy G. In: Long G.J. (Ed). Mössbauer Spectroscopy Applied to Inorganic Chemistry vol. 1 (1984), Plenum Press, New York 195-226
Reiff W.M., Long G.J., and Baker Jr. W.A. J. Am. Chem. Soc. 90 (1968) 6347
Bertrand J.A., Breece J.L., Kalyanaraman A.R., Long G.J., and Baker Jr. W.A. J. Am. Chem. Soc. 92 (1970) 5233
Long G.J., Wrobleski J.T., Thundathil R.V., Sparlin D.M., and Schlemper E.O. J. Am. Chem. Soc. 102 (1980) 6040
Adams R.W., Barraclough C.G., Martin R.L., and Winter G. Inorg. Chem. 5 (1966) 346
Long G.J., Robinson W.T., Tappmeyer W.P., and Bridges D.L. J. Chem. Soc. Dalton Trans. (1973) 573
Zheng Y.-Z., Tong M.-L., Xue W., Zhang W.-X., Chen X.-M., Grandjean F., and Long G.J. Angew. Chem. 46 (2007) 6076
Kittel C. Introduction to Solid State Physics (1971), Wiley, New York
