The explosive nitramine RDX (1,3,5-trinitrohexahydro-s-triazine) is thought to decompose largely by homolytic N-N bond cleavage, among other possible initiation reactions. Density-functional theory (DFT) calculations indicate that the resulting secondary aminyl (R2N·) radical can abstract an oxygen atom from NO2 or from a neighboring nitramine molecule, producing an aminoxyl (R2NO·) radical. Persistent aminoxyl radicals have been detected in electron-spin resonance (ESR) experiments and are consistent with autocatalytic "red oils" reported in the experimental literature. When the O-atom donor is a nitramine, a nitrosamine is formed along with the aminoxyl radical. Reactions of aminoxyl radicals can lead readily to the "oxy-s-triazine" product (as the s-triazine N-oxide) observed mass-spectrometrically by Behrens and co-workers. In addition to forming aminoxyl radicals, the initial aminyl radical can catalyze loss of HONO from RDX.
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http://dx.doi.org/10.1021/jp310247z | DOI Listing |
Nat Commun
January 2025
Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, P.R. China.
Electrochemical alcohol oxidation (EAO) represents an effective method for the production of high-value carbonyl products. However, its industrial viability is hindered by suboptimal efficiency stemming from low reaction rates. Here, we present a synergistic electrocatalysis approach that integrates an active electrode and aminoxyl radical to enhance the performance of EAO.
View Article and Find Full Text PDFJ Phys Chem B
January 2025
Department of Chemistry and Biochemistry, Thapar Institute of Engineering and Technology, Patiala 147001, Punjab, India.
This study presents a detailed density functional theory (DFT) investigation into the mechanism and energetics of C-H activations catalyzed by bioinspired Fe(IV)O complexes, particularly in the presence of -hydroxy mediators. The findings show that these mediators significantly enhance the reactivity of the iron-oxo complex. The study examines three substrates with varying bond dissociation energies─ethylbenzene, cyclohexane, and cyclohexadiene─alongside the [Fe(IV)O(N4Py)] complex.
View Article and Find Full Text PDFDalton Trans
January 2025
Department of Material Science, Graduate School of Science, University of Hyogo, 3-2-1 Kouto, Kamigori-cho, Ako-gun, Hyogo 678-1297, Japan.
Stable radicals have attracted increasing attention in recent years because of their unique electronic and optical characteristics. Aminoxyl radicals are one of the most widely studied stable radicals to date, but their applications in opto-functional materials have yet to be explored in detail. Our group previously reported the boron complexes of aminoxyl radicals exhibit near-infrared (NIR) absorption.
View Article and Find Full Text PDFInorg Chem
November 2024
Department of Chemistry, The University of Manchester, Oxford Road, Manchester M13 9PL, U.K.
Modulation of the crystal field (CF) in lanthanide (Ln) complexes can enhance optical and magnetic properties, and large CF splitting can be achieved with low coordination numbers in specific geometries. We previously reported that the homoleptic near-linear Sm complex [Sm{N(SiPr)}] () is oxidized by the 2,2,6,6-tetramethylpiperidinyl-1-oxy (TEMPO) radical to give the heteroleptic, approximately trigonal planar Sm complex, [Sm{N(SiPr)}(TEMPO)] (). Here, we report the synthesis of homologous [Ln{N(SiPr)}(TEMPO)] (; Ln = Tm, Yb) complexes by the oxidation of the parent [Ln{N(SiPr)}] (; Ln = Tm, Yb) with TEMPO; complexes all contain TEMPO anions.
View Article and Find Full Text PDFPolymers (Basel)
May 2024
Faculty of Chemistry, Lomonosov Moscow State University, Leninskie Gory 1, bld. 3, 119991 Moscow, Russia.
Polymerization-induced self-assembly (PISA) is a powerful and versatile technique for producing colloidal dispersions of block copolymer particles with desired morphologies. Currently, PISA can be carried out in various media, over a wide range of temperatures, and using different mechanisms. This method enables the production of biodegradable objects and particles with various functionalities and stimuli sensitivity.
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