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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...

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Autores principales: Meta, Marcel, Huber, Maximilian E., Michaelsen, Tim, Ayasli, Atilay, Ončák, Milan, Wester, Roland, Meyer, Jennifer
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
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.
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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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