Metal-catalyzed anaerobic disproportionation of hydroxylamine. Role of diazene and nitroxyl intermediates in the formation of N2, N 2O, NO+, and NH3

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The catalytic disproportionation of NH2OH has been studied in anaerobic aqueous solution, pH 6-9.3, at 25.0 °C, with Na 3[Fe(CN)5NH3]·3H2O as a precursor of the catalyst, [FeII(CN)5H2O] 3-. The oxidation products are N2, N2O, and NO+ (bound in the nitroprusside ion, NP), and NH3 is the reduction pro...

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Autor principal: Alluisetti, G.E
Otros Autores: Almaraz, A.E, Amorebieta, V.T, Doctorovich, F., Olabe, J.A
Formato: Capítulo de libro
Lenguaje:Inglés
Publicado: 2004
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ANAEROBIOSIS
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024 7 |2 scopus  |a 2-s2.0-6344227963 
024 7 |2 cas  |a ammonia, 14798-03-9, 51847-23-5, 7664-41-7; hydroxylamine, 7803-49-8; nitrogen oxide, 11104-93-1; nitrogen, 7727-37-9; nitroprusside sodium, 14402-89-2, 15078-28-1; Ammonia, 7664-41-7; Ferric Compounds; Ferrous Compounds; Free Radicals; Hydroxylamine, 7803-49-8; Nitrogen Oxides; Nitrogen, 7727-37-9; nitroxyl, 14332-28-6 
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100 1 |a Alluisetti, G.E. 
245 1 0 |a Metal-catalyzed anaerobic disproportionation of hydroxylamine. Role of diazene and nitroxyl intermediates in the formation of N2, N 2O, NO+, and NH3 
260 |c 2004 
270 1 0 |m Amorebieta, V.T.; Departamento de Química, Facultad de Ciencias Exactas, Univ. National de Mar del Plata, Funes y R. Peña, Mar del Plata B7602AYL, Argentina; email: amorebie@mdp.edu.ar 
506 |2 openaire  |e Política editorial 
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520 3 |a The catalytic disproportionation of NH2OH has been studied in anaerobic aqueous solution, pH 6-9.3, at 25.0 °C, with Na 3[Fe(CN)5NH3]·3H2O as a precursor of the catalyst, [FeII(CN)5H2O] 3-. The oxidation products are N2, N2O, and NO+ (bound in the nitroprusside ion, NP), and NH3 is the reduction product. The yields of N2/N2O increase with pH and with the concentration of NH2OH. Fast regime conditions involve a chain process initiated by the NH2 radical, generated upon coordination of NH2OH to [FeII(CN)5H 2O]3-. NH3 and nitroxyl, HNO, are formed in this fast process, and HNO leads to the production of N2, N 2O, and NP. An intermediate absorbing at 440 nm is always observed, whose formation and decay depend on the medium conditions. It was identified by UV-vis, RR, and 15NMR spectroscopies as the diazene-bound [Fe II(CN)5N2H2]3- ion and is formed in a competitive process with the radical path, still under the fast regime. At high pH's or NH2OH concentrations, an inhibited regime is reached, with slow production of only N2 and NH3. The stable red diazene-bridged [(NC)5FeHN=NHFe(CN)5] 6- ion is formed at an advanced degree of NH2OH consumption.  |l eng 
593 |a Departamento de Química, Facultad de Ciencias Exactas, Univ. National de Mar del Plata, Funes y R. Peña, Mar del Plata B7602AYL, Argentina 
593 |a Depto. Quim. Inorg./Analit./Quim. F., INQUIMAE, Universidad de Buenos Aires, Buenos Aires C1428EHA, Argentina 
690 1 0 |a CATALYSIS 
690 1 0 |a CATALYST ACTIVITY 
690 1 0 |a COORDINATION REACTIONS 
690 1 0 |a NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY 
690 1 0 |a OXIDATION 
690 1 0 |a PH EFFECTS 
690 1 0 |a REDUCTION 
690 1 0 |a ULTRAVIOLET SPECTROSCOPY 
690 1 0 |a CATALYTIC DISPROPORTIONATION 
690 1 0 |a DIAZENE 
690 1 0 |a AMINES 
690 1 0 |a AMMONIA 
690 1 0 |a AZO COMPOUND 
690 1 0 |a DIAZENE DERIVATIVE 
690 1 0 |a FREE RADICAL 
690 1 0 |a HYDROXYLAMINE 
690 1 0 |a NITROGEN 
690 1 0 |a NITROGEN OXIDE 
690 1 0 |a NITROPRUSSIDE SODIUM 
690 1 0 |a NITROXYL DERIVATIVE 
690 1 0 |a UNCLASSIFIED DRUG 
690 1 0 |a ABSORPTION SPECTROSCOPY 
690 1 0 |a ANAEROBIC METABOLISM 
690 1 0 |a AQUEOUS SOLUTION 
690 1 0 |a ARTICLE 
690 1 0 |a CATALYST 
690 1 0 |a CHEMICAL REACTION 
690 1 0 |a DISPROPORTIONATION REACTION 
690 1 0 |a GAS 
690 1 0 |a NITROGEN NUCLEAR MAGNETIC RESONANCE 
690 1 0 |a RAMAN SPECTROMETRY 
690 1 0 |a REDUCTION 
690 1 0 |a STOICHIOMETRY 
690 1 0 |a TEMPERATURE 
690 1 0 |a AMMONIA 
690 1 0 |a CATALYSIS 
690 1 0 |a FERRIC COMPOUNDS 
690 1 0 |a FERROUS COMPOUNDS 
690 1 0 |a FREE RADICALS 
690 1 0 |a HYDROGEN-ION CONCENTRATION 
690 1 0 |a HYDROXYLAMINE 
690 1 0 |a KINETICS 
690 1 0 |a NITROGEN 
690 1 0 |a NITROGEN OXIDES 
690 1 0 |a OXIDATION-REDUCTION 
690 1 0 |a SPECTRUM ANALYSIS, RAMAN 
650 1 7 |2 spines  |a PH 
650 1 7 |2 spines  |a ANAEROBIOSIS 
700 1 |a Almaraz, A.E. 
700 1 |a Amorebieta, V.T. 
700 1 |a Doctorovich, F. 
700 1 |a Olabe, J.A. 
773 0 |d 2004  |g v. 126  |h pp. 13432-13442  |k n. 41  |p J. Am. Chem. Soc.  |x 00027863  |w (AR-BaUEN)CENRE-19  |t Journal of the American Chemical Society 
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856 4 0 |u https://doi.org/10.1021/ja046724i  |y DOI 
856 4 0 |u https://hdl.handle.net/20.500.12110/paper_00027863_v126_n41_p13432_Alluisetti  |y Handle 
856 4 0 |u https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00027863_v126_n41_p13432_Alluisetti  |y Registro en la Biblioteca Digital 
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