Mechanisms for sonochemical oxidation of nitrogen

文献信息

发布日期 2022-06-09

DOI 10.1039/D2CP01995G

影响因子 3.676

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摘要

N2O, and mixtures of N2 and O2, dissolved in water—both in the presence and absence of added noble gases—have been subjected to ultrasonication with quantification of nitrite and nitrate products. Significant increase in product formation upon adding noble gas for both reactant systems is observed, with the reactivity order Ne < Ar < Kr < Xe. These observations lend support to the idea that extraordinarily high electronic and vibrational temperatures arise under these conditions. This is based on recent observations of sonoluminescence in the presence of noble gases and is inconsistent with the classical picture of adiabatic bubble collapse upon acoustic cavitation. The reaction mechanisms of the first few reaction steps necessary for the critical formation of NO are discussed, illustrated by quantum chemical calculations. The role of intermediate N2O in this series of elementary steps is also discussed to better understand the difference between the two reactant sources (N2O and 2 : 1 N2 : O2; same stoichiometry).

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来源期刊

Physical Chemistry Chemical Physics

CiteScore: 5.5

自引率: 10.3%

年发文量: 3036

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.