From oxidative degradation to direct oxidation: size regimes in the consecutive reaction of cationic tantalum clusters with dioxygen

Literature Information

Publication Date 2017-04-04
DOI 10.1039/C7CP01293D
Impact Factor 3.676
Authors

J. F. Eckhard, D. Neuwirth, M. Tschurl, U. Heiz


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Abstract

Cationic tantalum clusters (Ta9–12+) are reacted with molecular oxygen under multi-collision conditions in the gas phase in order to analyze the reaction kinetics. Clusters in this transitional size regime demonstrate reaction pathways associated with smaller clusters that mainly degrade upon oxidation (loss of a TaO unit) and those of larger clusters that are oxidized in absence of fragmentation. This behavior is exemplified by Ta9+, which generates Ta9O14+ and Ta4O11+, and the underlying, intricate reaction network is subsequently investigated. Ultimately, rate constants, reaction pathways and final products of cluster sizes up to n = 40 are compared to reveal the size-dependent oxidation behavior.

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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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