Mechanisms for sonochemical oxidation of nitrogen,Physical Chemistry Chemical Physics

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Mechanisms for sonochemical oxidation of nitrogen
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-06-09 , DOI: 10.1039/d2cp01995g
Thomas Qureishy _{1,

2} , Sverre Løyland _{1,

3} , Susanne J Jørgensen _{1,

4} , Eline M Færgestad _{1,

4} , Truls Norby _{1,

2} , Einar Uggerud _{1,

3}

Affiliation

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).

中文翻译：

氮的声化学氧化机制

N ₂ O，以及 N ₂和 O _{2的混合物}，溶解在水中——在存在和不存在添加惰性气体的情况下——已经过超声波处理，对亚硝酸盐和硝酸盐产物进行了定量分析。观察到在两种反应系统中添加惰性气体后产物形成的显着增加，反应顺序为 Ne < Ar < Kr < Xe。这些观察结果支持了在这些条件下会出现非常高的电子和振动温度的想法。这是基于最近在惰性气体存在下对声致发光的观察，并且与声空化时绝热气泡坍塌的经典图像不一致。讨论了关键形成 NO 所必需的前几个反应步骤的反应机制，并通过量子化学计算进行了说明。还讨论了这一系列基本步骤中的 O，以更好地了解两种反应物来源（N ₂ O 和 2 : 1 N ₂ : O ₂；相同的化学计量）之间的区别。

更新日期：2022-06-09

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