Mechanisms for sonochemical oxidation of nitrogen.

Autor: Qureishy T; Department of Chemistry, University of Oslo, Norway. einar.uggerud@kjemi.uio.no.; Centre for Materials Science and Nanotechnology, University of Oslo, Norway., Løyland S; Department of Chemistry, University of Oslo, Norway. einar.uggerud@kjemi.uio.no.; Hylleraas Centre for Quantum Molecular Sciences, University of Oslo, Norway., Jørgensen SJ; Department of Chemistry, University of Oslo, Norway. einar.uggerud@kjemi.uio.no.; Centre for Biogeochemistry in the Anthropocene, University of Oslo, Norway., Færgestad EM; Department of Chemistry, University of Oslo, Norway. einar.uggerud@kjemi.uio.no.; Centre for Biogeochemistry in the Anthropocene, University of Oslo, Norway., Norby T; Department of Chemistry, University of Oslo, Norway. einar.uggerud@kjemi.uio.no.; Centre for Materials Science and Nanotechnology, University of Oslo, Norway., Uggerud E; Department of Chemistry, University of Oslo, Norway. einar.uggerud@kjemi.uio.no.; Hylleraas Centre for Quantum Molecular Sciences, University of Oslo, Norway.
Jazyk: angličtina
Zdroj: Physical chemistry chemical physics : PCCP [Phys Chem Chem Phys] 2022 Jun 29; Vol. 24 (25), pp. 15357-15364. Date of Electronic Publication: 2022 Jun 29.
DOI: 10.1039/d2cp01995g
Abstrakt: N 2 O, and mixtures of N 2 and O 2 , 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 N 2 O in this series of elementary steps is also discussed to better understand the difference between the two reactant sources (N 2 O and 2 : 1 N 2  : O 2 ; same stoichiometry).
Databáze: MEDLINE