High-pressure photodissociation of water as a tool for hydrogen synthesis and fundamental chemistry

化学 光解 一氧化碳 激进的 分子 化学反应 光化学 大气压力 有机化学 催化作用 海洋学 地质学
作者
Matteo Ceppatelli,Roberto Bini,Vincenzo Schettino
出处
期刊:Proceedings of the National Academy of Sciences of the United States of America [National Academy of Sciences]
卷期号:106 (28): 11454-11459 被引量:52
标识
DOI:10.1073/pnas.0901836106
摘要

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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