Addition and redox reactivity of hydrogen sulfides (H2S/HS -) with nitroprusside: New chemistry of nitrososulfide ligands

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The nitroprusside ion [Fe(CN)5NO]2- (NP) reacts with excess HS- in the pH range 8.5-12.5, in anaerobic medium ("Gmelin" reaction). The progress of the addition process of HS - into the bound NO+ ligand was monitored by stopped-flow UV/Vis/EPR and FTIR spectroscopy, mass spectrometry, and c...

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Autor principal: Quiroga, S.L
Otros Autores: Almaraz, A.E, Amorebieta, V.T, Perissinotti, L.L, Olabe, J.A
Formato: Capítulo de libro
Lenguaje:Inglés
Publicado: 2011
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024 7 |2 scopus  |a 2-s2.0-79953189722 
024 7 |2 cas  |a ferrous ion, 15438-31-0; hydrogen sulfide, 15035-72-0, 7783-06-4; nitrogen oxide, 11104-93-1; nitroprusside sodium, 14402-89-2, 15078-28-1; Ferrous Compounds; Hydrogen Sulfide, 7783-06-4; Ligands; Nitrogen Oxides; Nitroprusside, 15078-28-1 
040 |a Scopus  |b spa  |c AR-BaUEN  |d AR-BaUEN 
030 |a CEUJE 
100 1 |a Quiroga, S.L. 
245 1 0 |a Addition and redox reactivity of hydrogen sulfides (H2S/HS -) with nitroprusside: New chemistry of nitrososulfide ligands 
260 |c 2011 
270 1 0 |m Amorebieta, V. T.; Departamento de Química, Facultad de Ciencias Exactas, Universidad Nacional de Mar Del Plata, Funes y Roca, Mar del Plata B7602AYL, Argentina; email: amorebie@mdp.edu.ar 
506 |2 openaire  |e Política editorial 
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504 |a The assignment of the reaction in Equation (4) as a spontaneous decomposition of the adduct is supported by our complementary experiments in excess of NP, in which a very similar rate of [Fe(CN)5NO] 3- production has been observed; Das, T.N., Huie, R.E., Neta, P., Padmaja, S., (1999) J. Phys. Chem. A, 103, p. 5221 
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504 |a Formation of dominant NH3 and other reduction products (N 2O, NO, NH2OH) in the reactions of free nitrosothiolates with an excess of thiolate allowed proposing diverse structures for the intermediates and their further reactivity modes.[51] We rely on our calculations of the atomic charges for AH, A and a related nitrosothiolate (see Table SI6 in the Supporting Information), revealing that the most positively charged N atom in the Fe-NOS(H) moieties should be the expected site for the nucleophilic attack of HS-. The attack on the S atom of the NOSR group has also been considered for free and protonated nitrosothiolates. [50, 51a]; Miranda, K.M., (2005) Coord. Chem. Rev., 249, p. 433 
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520 3 |a The nitroprusside ion [Fe(CN)5NO]2- (NP) reacts with excess HS- in the pH range 8.5-12.5, in anaerobic medium ("Gmelin" reaction). The progress of the addition process of HS - into the bound NO+ ligand was monitored by stopped-flow UV/Vis/EPR and FTIR spectroscopy, mass spectrometry, and chemical analysis. Theoretical calculations were employed for the characterization of the initial adducts and reaction intermediates. The shapes of the absorbance-time curves at 535-575 nm depend on the pH and concentration ratio of the reactants, R=[HS -]/[NP]. The initial adduct [Fe(CN)5N(O)SH]3- (AH, Î max≈570 nm) forms in the course of a reversible process, with kad=190±20 M-1 s-1, k -ad=0.3±0.05 s-1. Deprotonation of AH (pK a=10.5±0.1, at 25.0 °C, I=1 M), leads to [Fe(CN) 5N(O)S]4- (A, Î max=535 nm, ε=6000±300 M-1 cm-1). [Fe(CN) 5NO].3- and HS2. 2- radicals form through the spontaneous decomposition of AH and A. The minor formation of the [Fe(CN)5NO]3- ion equilibrates with [Fe(CN)4NO]2- through cyanide labilization, and generates the "g=2.03" iron-dinitrosyl, [Fe(NO)2(SH) 2]-, which is labile toward NO release. Alternative nucleophilic attack of HS- on AH and A generates the reactive intermediates [Fe(CN)5N(OH)(SH)2]3- and [Fe(CN)5N(OH)(S)(SH)]4-, respectively, which decompose through multielectronic nitrosyl reductions, leading to NH3 and hydrogen disulfide, HS2-. N2O is also produced at pH≥11. Biological relevance relates to the role of NO, NO-, and other bound intermediates, eventually able to be released to the medium and rapidly trapped by substrates. Structure and reactivity comparisons of the new nitrososulfide ligands with free and bound nitrosothiolates are provided. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.  |l eng 
593 |a Departamento de Química, Facultad de Ciencias Exactas, Universidad Nacional de Mar Del Plata, Funes y Roca, Mar del Plata B7602AYL, Argentina 
593 |a Departamento de Química Inorgánica, Analítica y Química Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires/INQUIMAE/CONICET, Pabellõn 2, C1428EHA Buenos Aires, Argentina 
690 1 0 |a ADDITION REACTION 
690 1 0 |a IRON 
690 1 0 |a N LIGANDS 
690 1 0 |a NITROSOSULFIDE LIGANDS 
690 1 0 |a NITROSYL 
690 1 0 |a SULFUR 
690 1 0 |a ABSORBANCE-TIME CURVES 
690 1 0 |a CONCENTRATION RATIO 
690 1 0 |a FTIR SPECTROSCOPY 
690 1 0 |a N LIGANDS 
690 1 0 |a NITROSOSULFIDE LIGANDS 
690 1 0 |a NITROSYL 
690 1 0 |a NO RELEASE 
690 1 0 |a NUCLEOPHILIC ATTACK 
690 1 0 |a PH RANGE 
690 1 0 |a REACTIVE INTERMEDIATE 
690 1 0 |a REDOX REACTIVITY 
690 1 0 |a REVERSIBLE PROCESS 
690 1 0 |a STOPPED FLOW 
690 1 0 |a THEORETICAL CALCULATIONS 
690 1 0 |a ADDITION REACTIONS 
690 1 0 |a CHEMICAL ANALYSIS 
690 1 0 |a CYANIDES 
690 1 0 |a FOURIER TRANSFORM INFRARED SPECTROSCOPY 
690 1 0 |a HYDRAULIC STRUCTURES 
690 1 0 |a HYDROGEN 
690 1 0 |a MASS SPECTROMETRY 
690 1 0 |a REACTION INTERMEDIATES 
690 1 0 |a REACTION KINETICS 
690 1 0 |a SULFUR 
690 1 0 |a LIGANDS 
690 1 0 |a FERROUS ION 
690 1 0 |a HYDROGEN SULFIDE 
690 1 0 |a LIGAND 
690 1 0 |a NITROGEN OXIDE 
690 1 0 |a NITROPRUSSIDE SODIUM 
690 1 0 |a ARTICLE 
690 1 0 |a CHEMICAL STRUCTURE 
690 1 0 |a CHEMISTRY 
690 1 0 |a KINETICS 
690 1 0 |a OXIDATION REDUCTION REACTION 
690 1 0 |a STEREOISOMERISM 
690 1 0 |a ULTRAVIOLET SPECTROPHOTOMETRY 
690 1 0 |a FERROUS COMPOUNDS 
690 1 0 |a HYDROGEN SULFIDE 
690 1 0 |a HYDROGEN-ION CONCENTRATION 
690 1 0 |a KINETICS 
690 1 0 |a LIGANDS 
690 1 0 |a MOLECULAR STRUCTURE 
690 1 0 |a NITROGEN OXIDES 
690 1 0 |a NITROPRUSSIDE 
690 1 0 |a OXIDATION-REDUCTION 
690 1 0 |a SPECTROPHOTOMETRY, ULTRAVIOLET 
690 1 0 |a STEREOISOMERISM 
650 1 7 |2 spines  |a PH 
650 1 7 |2 spines  |a PH 
700 1 |a Almaraz, A.E. 
700 1 |a Amorebieta, V.T. 
700 1 |a Perissinotti, L.L. 
700 1 |a Olabe, J.A. 
773 0 |d 2011  |g v. 17  |h pp. 4145-4156  |k n. 15  |p Chem. Eur. J.  |x 09476539  |w (AR-BaUEN)CENRE-83  |t Chemistry - A European Journal 
856 4 1 |u https://www.scopus.com/inward/record.uri?eid=2-s2.0-79953189722&doi=10.1002%2fchem.201002322&partnerID=40&md5=7f88afd8e9903201d87f82a663c8b0e0  |y Registro en Scopus 
856 4 0 |u https://doi.org/10.1002/chem.201002322  |y DOI 
856 4 0 |u https://hdl.handle.net/20.500.12110/paper_09476539_v17_n15_p4145_Quiroga  |y Handle 
856 4 0 |u https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_09476539_v17_n15_p4145_Quiroga  |y Registro en la Biblioteca Digital 
961 |a paper_09476539_v17_n15_p4145_Quiroga  |b paper  |c PE 
962 |a info:eu-repo/semantics/article  |a info:ar-repo/semantics/artículo  |b info:eu-repo/semantics/publishedVersion 
999 |c 71635 

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