High-pressure reactivity of clathrate hydrates by two-photon dissociation of water
文献信息
It is shown that photoinduced reactions are observed at room temperature and pressure of few tenths of gigapascal in clathrate hydrates of CO and of model hydrocarbons under mild irradiation at 350 nm with power in the 50ā610 mW range. The reactions are triggered by highly reactive OH radicals produced by two-photon excitation of the lowest electronic excited state of water having dissociative character. The formation of CO2 is observed in all the reactions involving carbonaceous clathrate hydrates, and direct or indirect evidence for the formation of molecular hydrogen is obtained. The CO2 produced in the reactions can be sequestered as a clathrate hydrate whose stability range seems to extend to room temperature at pressures of 0.5ā0.6 GPa. Although the N2 hydrate is stable up to 0.9 GPa under irradiation, a partial cleavage of the NāN triple bond is produced once the hydrate decomposes at 0.1 GPa.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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