Energy-pooling transitions to doubly excited K atoms at a promoted iron-oxidecatalyst surface: more than 30 eV available for reaction

Literature Information

Publication Date 2009-03-26
DOI 10.1039/B817380J
Impact Factor 3.676
Authors

Andrzej Kotarba, Leif Holmlid


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Abstract

The promoter action of alkali atoms, such as K atoms, at heterogeneous catalyst surfaces has been used in industrial catalysis for many decades, giving improved activity and selectivity in the catalyzed chemical reactions. Several mechanisms for this promotion effect have been proposed, among which the Rydberg excitation mechanism is well-supported by experiments from our groups. Further experiments now show that even doubly excited K Rydberg species are formed at an industrial catalyst (styrene catalyst) surface. This indicates that a large excitation energy of >30 eV can easily accumulate in an atomic or molecular species. The methods used for the identification of the excited species are pulsed laser-induced TOF-MS and intracavity stimulated emission. The doubly excited states are formed at the surface of the catalyst by thermal excitation through selective excitation and energy-pooling processes and are here observed outside the surface in the extended boundary layer. Experiments with ionization energy transfer indicate that no energy matching is required in reactions driven by the excitation energy.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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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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