Silicon carbonate phase formed from carbon dioxide and silica under pressure

Year: 2011

Authors: Santoro M., Gorelli F., Haines J., Cambon O., Levelut C., Garbarino G.

Autors Affiliation: European Laboratory for Nonlinear Spectroscopy, Via Nello Carrara 1, 50019 Sesto Fiorentino, Italy;
Istituto per i Processi Chimico-Fisici–Consiglio Nazionale delle Ricerche, Unità Organizzativa di Supporto di Roma, Piazzale Aldo Moro 2,00185 Rome, Italy;
Institut Charles Gerhardt Montpellier, Equipe Chimie et Cristallochimie des Matériaux, Unité Mixte de Recherche 5253, Centre National de la Recherche Scientifique, Université Montpellier 2, Place Eugène Bataillon, cc1504, 34095 Montpellier Cedex 5, France;
Laboratoire Charles Coulomb, Unité Mixte de Recherche 5221, Centre National de la Recherche Scientifique, Université Montpellier 2, Place Eugène Bataillon, cc026, 34095 Montpellier Cedex 5, France; and European Synchrotron Radiation Facility, 38343 Grenoble, France

Abstract: The discovery of nonmolecular carbon dioxide under high-pressure conditions shows that there are remarkable analogies between this important substance and other group IV oxides. A natural and long-standing question is whether compounds between CO2 and SiO2 are possible. Under ambient conditions, CO2 and SiO2 are thermodynamically stable and do not react with each other. We show that reactions occur at high pressures indicating that silica can behave in a manner similar to ionic metal oxides that form carbonates at room pressure. A silicon carbonate phase was synthesized by reacting silicalite, a microporous SiO2 zeolite, and molecular CO2 that fills the pores, in diamond anvil cells at 18–26 GPa and 600–980 K; the compound was then temperature quenched. The material was characterized by Raman and IR spectroscopy, and synchrotron X-ray diffraction. The experiments reveal unique oxide chemistry at high pressures and the potential for synthesis of a class of previously uncharacterized materials. There are also potential implications for CO2 segregation in planetary interiors and for CO2 storage.


Volume: 108 (19)      Pages from: 7689  to: 7692

More Information: We thank M. Mezouar for discussions and D. Maurin and D. Bourgogne for technical support for Raman and IR measurements at Universite Montpellier 2. We acknowledge support from the European Union (European Laboratory for Nonlinear Spectroscopy Contract FP7 G. A. No. 228334 LASERLABEUROPE), the Ente Cassa di Risparmio di Firenze, and the Agence Nationale de la Recherche (Contract ANR-09-BLAN-0018-01). We also thank the ESRF for provision of beam time at ID27. M. S. thanks the Region Languedoc-Roussillon for having supported his research at the Universite Montpellier 2, in 2009, and the Universite de Nimes, in 2010, as an Invited Professor.
KeyWords: high-pressure chemistry; material science; optical spectroscopy
DOI: 10.1073/pnas.1019691108

Citations: 62
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