期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 106, 期 28, 页码 11454-11459出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0901836106
关键词
high-pressure chemistry; photocatalysis
资金
- European Union [RII3-CT2003-506350]
- Italian Ministero dell'Universita e della Ricerca Scientifica e Tecnologica
- Firenze Hydrolab through a grant by Ente Cassa di Risparmio di Firenze
High-pressure methods have been demonstrated to be efficient in providing new routes for the synthesis of materials of technological interest. In several molecular compounds, the drastic pressure conditions required for spontaneous transformations have been lowered to the kilobar range by photoactivation of the reactions. At these pressures, the syntheses are accessible to large-volume applications and are of interest to bioscience, space, and environmental chemistry. Here, we show that the short-lived hydroxyl radicals, produced in the photodissociation of water molecules by near-UV radiation at room temperature and pressures of a few tenths of a gigapascal (GPa), can be successfully used to trigger chemical reactions in mixtures of water with carbon monoxide or nitrogen. The detection of molecular hydrogen among the reaction products is of particular relevance. Besides the implications in fundamental chemistry, the mild pressure and irradiation conditions, the efficiency of the process, and the nature of the reactant and product molecules suggest applications in synthesis.
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