NDLI: Intermediates Involved in the Oxidation of Nitrogen Monoxide: Photochemistry of the $cis-N_{2}O_{2}⋅O_{2}$ complex and of $sym-N_{2}O_{4}$ in Solid Ne Matrices

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Intermediates Involved in the Oxidation of Nitrogen Monoxide: Photochemistry of the $cis-N_{2}O_{2}⋅O_{2}$ complex and of $sym-N_{2}O_{4}$ in Solid Ne Matrices

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Intermediates Involved in the Oxidation of Nitrogen Monoxide: Photochemistry of the $cis-N_{2}O_{2}⋅O_{2}$ complex and of $sym-N_{2}O_{4}$ in Solid Ne Matrices

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Beckers, Helmut Zeng, Xiaoqing Willner, Helge
Description	Author Affiliation: Beckers H ( Fachbereich C-Anorganische Chemie, Bergische Universität Wuppertal, 42097 Wuppertal, Germany. beckers@uni-wuppertal.de)
Abstract	Pure $sym-N_{2}O_{4}$ isolated in solid Ne was obtained by passing cold neon gas over solid $N_{2}O_{4}$ at −115 °C and quenching the resulting gaseous mixture at 6.3 K. Filtered UV irradiation (260–400 nm) converts $sym-N_{2}O_{4}$ into $trans-ONONO_{2},$ a weakly interacting $(NO_{2})_{2}$ radical pair, and traces of the $cis-N_{2}O_{2}⋅O_{2}$ complex. Besides the weakly bound $ON⋅O_{2}$ complex, $cis-N_{2}O_{2}⋅O_{2}$ was also obtained by co-deposition of NO and $O_{2}$ in solid Ne at 6.3 K, and both complexes were characterised by their matrix IR spectra. Concomitantly formed $cis-N_{2}O_{2}$ dissociated on exposure to filtered IR irradiation $(400–8000 cm^{−1}),$ and the $cis-N_{2}O_{2}⋅O_{2}$ complex rearranged to $sym-N_{2}O_{4}$ and $trans-ONONO_{2}.$ Experiments using $^{18}O_{2}$ in place of $^{16}O_{2}$ revealed a non-concerted conversion of $cis-N_{2}O_{2}⋅O_{2}$ into these species, and gave access to four selectively $di-^{18}O-substituted$ $trans-ONONO_{2}$ isotopomers. No isotopic scrambling occurred. The IR spectra of $sym-N_{2}O_{4}$ and of $trans-ONONO_{2}$ in solid Ne were recorded. IR fundamentals of $trans-ONONO_{2}$ were assigned based on experimental $^{16/18}O$ isotopic shifts and guided by DFT calculations. Previously reported contradictory measurements on cis- and $trans-ONONO_{2}$ are discussed. Dinitroso peroxide, ONOONO, a proposed intermediate in the IR photoinduced rearrangement of $cis-N_{2}O_{2}⋅O_{2}$ to the various $N_{2}O_{4}$ species, was not detected. Its absence in the photolysis products indicates a low barrier $(≤10 kJ mol^{−1})$ for its exothermic OO bond homolysis into a $(NO_{2})_{2}$ radical pair.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	5
Volume Number	16
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2010-02-01
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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