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Formation of Spinel from a Hydrotalcite-Like Compound at Low Temperature: Reaction between Edges of Crystallites

Published online by Cambridge University Press:  28 February 2024

Toshiyuki Hibino
Affiliation:
Materials Processing Department, National Institute for Resources and Environment, 16-3 Onogawa, Tsukuba, 305 Japan
Atsumu Tsunashima
Affiliation:
Materials Processing Department, National Institute for Resources and Environment, 16-3 Onogawa, Tsukuba, 305 Japan
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Abstract

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The thermal decomposition behavior of hydrotalcite-like compounds (HTlcs) prepared by reconstruction of calcined HTlcs is described. From the results of X-ray diffraction (XRD), it seems that dicarboxylate intercalates of HTlc calcined at 500 °C are completely reconstructed to Mg-Al-CO3 HTlc by exposure to aqueous Na2CO3. However, the Mg-Al-CO3 HTlc reconstructed under particular conditions yields spinel (MgAl2O4) at 400 °C. This temperature is very low, because Mg-Al-CO3 HTlc that has been reported yields spinel at 900 °C after forming a Mg-Al double oxide. The reconstructed Mg-Al-CO3 HTlc that yields spinel at 400 °C is obtained when the following conditions are fulfilled: the crystallites of the starting dicarboxylate intercalates are coagulated tightly and the calcined HTlcs and reconstructed materials are not ground. The Mg-Al-CO3 HTlc reconstructed under these conditions contains only 55–70% of carbonate anions required by stoichiometry. Therefore, we conclude that the transformation of reconstructed Mg-Al-CO3 HTlc to spinel at 400 °C is the result of a reaction occurring between edges of crystallites.

Type
Research Article
Copyright
Copyright © 1997, The Clay Minerals Society

References

Allmann, R., 1968 The crystal structure of pyroaurite Acta Crystallogr B24 972977 10.1107/S0567740868003511.CrossRefGoogle Scholar
Bratton, R.J., 1969 Coprecipitates yielding MgAl2O4 spinel powders Am Ceram Soc Bull 48 759762.Google Scholar
Brindley, G.W. and Kikkawa, S., 1979 A crystal-chemical study of Mg,Al and Ni,Al hydroxy-perchlorates and hydroxy-car-bonates Am Mineral 64 836843.Google Scholar
Cavani, F. Trifirò, F. and Vaccari, A., 1991 Hydrotalcite-type anionic clays: Preparation, roperties and applications Catal Today 11 173301 10.1016/0920-5861(91)80068-K.CrossRefGoogle Scholar
Chibwe, K. and Jones, W., 1989 Synthesis of polyoxometalate-pillared layered double hydroxides via calcined precursors Chem Mater 1 489490 10.1021/cm00005a006.CrossRefGoogle Scholar
Chibwe, K. and Jones, W., 1989 Intercalation of organic and inorganic anions into layered double hydroxides J Chem Soc, Chem Commun 926927.CrossRefGoogle Scholar
Constantino, V.R.L. and Pinnavaia, T.J., 1995 Basic properties of Mg2+,1-x Al3+ x layered double hydroxides intercalated by carbonate, hydroxide, chloride and sulfate anions Inorg Chem 34 883892 10.1021/ic00108a020.CrossRefGoogle Scholar
Dimotakis, E.D. and Pinnavaia, T.J., 1990 New route to layered double hydroxides intercalated by organic anions: Precursors to polyoxometalate-pillared derivatives Inorg Chem 13 23932394 10.1021/ic00338a001.CrossRefGoogle Scholar
Drezdzon, M.A., 1988 Synthesis of isopolymetalate-pillared hydrotalcite via organic-anion-pillared precursors Inorg Chem 27 46284632 10.1021/ic00298a024.CrossRefGoogle Scholar
Giannelis, E.P. Nocera, D.G. and Pinnavaia, T.J., 1987 Anionic pho-tocatalysts supported in layered double hydroxides: Intercalation and photophysical properties of a ruthenium complex anion in synthetic hydrotalcite Inorg Chem 26 203205 10.1021/ic00248a039.CrossRefGoogle Scholar
Gusmano, G. Nunziante, P. Traversa, E. and Chiozzini, G., 1991 The mechanism of MgAl2O4 spinel formation from the thermal decomposition of coprecipitated hydroxides J Eur Ceram Soc 7 3139 10.1016/0955-2219(91)90051-Z.CrossRefGoogle Scholar
Hibino, T. Yamashita, Y. Kosuge, K. and Tsunashima, A., 1995 De-carbonation behavior of Mg-Al-CO3 hydrotalcite-like compounds during heat treatment Clays Clay Miner 43 427432 10.1346/CCMN.1995.0430405.CrossRefGoogle Scholar
Hibino, T. Kosuge, K. and Tsunashima, A., 1996 Synthesis of carbon-hydrotalcite complex and its thermal degradation behavior Clays Clay Miner 44 151154 10.1346/CCMN.1996.0440114.CrossRefGoogle Scholar
Hokazono, S. Nagai, H. and Kato, A., 1991 Synthesis of spinel powder by the homogeneous precipitation method Nippon Kagaku Kaishi 275280.CrossRefGoogle Scholar
Hudson, M.J. Carlino, S. and Apperley, D.C., 1995 Thermal conversion of a layered (Mg/Al) double hydroxide to the oxide J Mater Chem 5 323329 10.1039/jm9950500323.CrossRefGoogle Scholar
Ingram, L. and Taylor, H.F.W., 1967 The crystal structures of sjögrenite and pyroaurite Mineral Mag 36 465479.Google Scholar
Itaya, K. Chang, H.-C. and Uchida, I., 1987 Anion-exchanged hy-drotalcite-like-clay-modified electrodes Inorg Chem 26 624626 10.1021/ic00251a028.CrossRefGoogle Scholar
Kodama, H. Kotlyar, L.S. and Ripmeester, J.A., 1989 Quantification of crystalline and noncrystalline material in ground kaolin-ite by X-ray powder diffraction, infrared, solid-state nuclear magnetic resonance, and chemical-dissolution analyses Clays Clay Miner 37 364370 10.1346/CCMN.1989.0370410.CrossRefGoogle Scholar
Kristof, Juhász, A.Z. and Vassányi, I., 1993 The effect of mechanical treatment on the crystal structure and thermal behavior of kaolinite Clays Clay Miner 41 608612 10.1346/CCMN.1993.0410511.CrossRefGoogle Scholar
MacKenzie, K.J.D. Meinhold, R.H. Sherriff, B.L. and Xu, Z., 1993 27Al and 25Mg solid-state magic-angle spinning nuclear magnetic resonance study of hydrotalcite and its thermal decomposition sequence J Mater Chem 3 12631269 10.1039/jm9930301263.CrossRefGoogle Scholar
Miyata, S. and Kumura, T., 1973 Synthesis of new hydrotalcite-like compounds and their physico-chemical properties Chem Lett 843848.CrossRefGoogle Scholar
Miyata, S., 1975 The syntheses of hydrotalcite-like compounds and their structures and physico-chemical properties—I: The systems Mg2+-Al3+-NCV, Mg2+-Al3+-CL, Mg2+-Al3+-C1O4-, Ni2+-Al3+-CL and Zn2+-Al3+-CL Clays Clay Miner 23 369375 10.1346/CCMN.1975.0230508.CrossRefGoogle Scholar
Miyata, S., 1980 Physico-chemical properties of synthetic hy-drotalcites in relation to composition Clays Clay Miner 28 5056 10.1346/CCMN.1980.0280107.CrossRefGoogle Scholar
Narita, E. Kaviratna, P. and Pinnavaia, T.J., 1991 Synthesis of het-eropolyoxometalate pillared layered double hydroxides via calcined zinc-aluminium oxide precursors Chem Lett 805808.CrossRefGoogle Scholar
Pesic, L. Salipurovic, S. Markovic, V. Vucelic, D. Kagunya, W. and Jones, W., 1992 Thermal characteristics of a synthetic hydrotalcite-like material J Mater Chem 2 10691073 10.1039/jm9920201069.CrossRefGoogle Scholar
Rey, F. Fornés, V. and Rojo, J.M., 1992 Thermal decomposition of hydrotalcites: An infrared and nuclear magnetic resonance spectroscopic study J Chem Soc, Faraday Trans 88 22332238 10.1039/FT9928802233.CrossRefGoogle Scholar
Rouxhet, P.G. and Taylor, H.F.W., 1969 Thermal decomposition of sjögrenite and pyroaurite Chimia 23 480485.Google Scholar
Yun, S.K. Constantino, V.R.L. and Pinnavaia, T.J., 1995 New polyol route to keggin ion-pillared layered double hydroxides Microporous Mater 4 2129 10.1016/0927-6513(94)00079-B.CrossRefGoogle Scholar