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Dynamics of the Oxygen Atom Transfer Reaction between Carbon Dioxide and the Tantalum Cation
[Image: see text] The understanding of fundamental atomic-level processes often requires well-defined model systems. The oxygen atom transfer from CO(2) to a transition metal cation in the gas phase presents such a model system. We investigate the reaction of Ta(+) + CO(2) for which the formation of...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10291641/ https://www.ncbi.nlm.nih.gov/pubmed/37290113 http://dx.doi.org/10.1021/acs.jpclett.3c01078 |
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author | Meta, Marcel Huber, Maximilian E. Michaelsen, Tim Ayasli, Atilay Ončák, Milan Wester, Roland Meyer, Jennifer |
author_facet | Meta, Marcel Huber, Maximilian E. Michaelsen, Tim Ayasli, Atilay Ončák, Milan Wester, Roland Meyer, Jennifer |
author_sort | Meta, Marcel |
collection | PubMed |
description | [Image: see text] The understanding of fundamental atomic-level processes often requires well-defined model systems. The oxygen atom transfer from CO(2) to a transition metal cation in the gas phase presents such a model system. We investigate the reaction of Ta(+) + CO(2) for which the formation of TaO(+) is highly efficient and attributed to multistate reactivity. Here, we study the atomistic dynamics of the oxygen atom transfer reaction by recording experimental energy and angle differential cross sections by crossed beam velocity map imaging supported by ab initio quantum chemical calculations. Product ion velocity distributions are dominated by signatures for indirect dynamics, despite the reaction being highly exothermic. Product kinetic energy distributions show little dependence on additional collision energy even with only four atoms involved, which hints at dynamical trapping behind a submerged barrier. |
format | Online Article Text |
id | pubmed-10291641 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-102916412023-06-27 Dynamics of the Oxygen Atom Transfer Reaction between Carbon Dioxide and the Tantalum Cation Meta, Marcel Huber, Maximilian E. Michaelsen, Tim Ayasli, Atilay Ončák, Milan Wester, Roland Meyer, Jennifer J Phys Chem Lett [Image: see text] The understanding of fundamental atomic-level processes often requires well-defined model systems. The oxygen atom transfer from CO(2) to a transition metal cation in the gas phase presents such a model system. We investigate the reaction of Ta(+) + CO(2) for which the formation of TaO(+) is highly efficient and attributed to multistate reactivity. Here, we study the atomistic dynamics of the oxygen atom transfer reaction by recording experimental energy and angle differential cross sections by crossed beam velocity map imaging supported by ab initio quantum chemical calculations. Product ion velocity distributions are dominated by signatures for indirect dynamics, despite the reaction being highly exothermic. Product kinetic energy distributions show little dependence on additional collision energy even with only four atoms involved, which hints at dynamical trapping behind a submerged barrier. American Chemical Society 2023-06-08 /pmc/articles/PMC10291641/ /pubmed/37290113 http://dx.doi.org/10.1021/acs.jpclett.3c01078 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Meta, Marcel Huber, Maximilian E. Michaelsen, Tim Ayasli, Atilay Ončák, Milan Wester, Roland Meyer, Jennifer Dynamics of the Oxygen Atom Transfer Reaction between Carbon Dioxide and the Tantalum Cation |
title | Dynamics of
the Oxygen Atom Transfer Reaction between
Carbon Dioxide and the Tantalum Cation |
title_full | Dynamics of
the Oxygen Atom Transfer Reaction between
Carbon Dioxide and the Tantalum Cation |
title_fullStr | Dynamics of
the Oxygen Atom Transfer Reaction between
Carbon Dioxide and the Tantalum Cation |
title_full_unstemmed | Dynamics of
the Oxygen Atom Transfer Reaction between
Carbon Dioxide and the Tantalum Cation |
title_short | Dynamics of
the Oxygen Atom Transfer Reaction between
Carbon Dioxide and the Tantalum Cation |
title_sort | dynamics of
the oxygen atom transfer reaction between
carbon dioxide and the tantalum cation |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10291641/ https://www.ncbi.nlm.nih.gov/pubmed/37290113 http://dx.doi.org/10.1021/acs.jpclett.3c01078 |
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