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Pinakoulaki E Ohta T Soulimane T Kitagawa T Varotsis C 《Journal of the American Chemical Society》2005,127(43):15161-15167
Reaction pathways in the enzymatic formation and cleavage of the N-N and N-O bonds, respectively, are difficult to verify without the structure of the intermediates, but we now have such information on the heme a(3)(2+)-NO species formed in the reaction of ba(3)-oxidase with NO from resonance Raman spectroscopy. We have identified the His-heme a(3)(2+)-NO/Cu(B)(1+) species by its characteristic Fe-NO and N-O stretching frequencies at 539 and 1620 cm(-)(1), respectively. The Fe-NO and N-O frequencies in ba(3)-oxidase are 21 and 7 cm(-)(1) lower and higher, respectively, than those observed in Mb-NO. From these results and earlier Raman and FTIR measurements, we demonstrate that the protein environment of the proximal His384 that is part of the Q-proton pathway controls the strength of the Fe-His384 bond upon ligand (CO vs NO) binding. We also show by time-resolved FTIR spectroscopy that Cu(B)(1+) has a much lower affinity for NO than for CO. We suggest that the reduction of NO to N(2)O by ba(3)-oxidase proceeds by the fast binding of the first NO molecule to heme a(3) with high-affinity, and the second NO molecule binds to Cu(B) with low-affinity, producing the temporal co-presence of two NO molecules in the heme-copper center. The low-affinity of Cu(B) for NO binding also explains the NO reductase activity of the ba(3)-oxidase as opposed to other heme-copper oxidases. With the identification of the His-heme a(3)(2+)-NO/Cu(B)(1+) species, the structure of the binuclear heme a(3)-Cu(B)(1+) center in the initial step of the NO reduction mechanism is known. 相似文献
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M.?Koubaa W.?Prellier R.?Soulimane W.?Boujelben A.?Cheikh-RouhouEmail author Ph.?Lecoeur A.-M.?Haghiri-Gosnet 《The European Physical Journal B - Condensed Matter and Complex Systems》2005,47(1):29-35
The magneto-transport properties of thick relaxed A-site deficient films
having the composition Pr
Sr0.3MnO3 (P□SMO
with the □ symbol for the Pr vacancy) and Pr0.7Sr
MnO3 (PS□MO) are studied. A
direct comparison with a Pr0.7Sr0.3MnO3 (PSMO)completely relaxed film, deposited under the same growth conditions, shows
a reduction of the in-plane parameter a100 associated to an enhancement
of the out-plane parameter. The strains (bulk strain εB
and biaxial Jahn-Teller strain εJ-T) do vary with the
nature of the cationic vacancy. For example, an enhancement of εB of 9% in the PS□MO film (Sr deficient) produces a decrease
of TC of 30 K, whereas the Pr deficient P□SMO film exhibits a
large reduction of both εB (-16%) and εJ-T (divided by a factor of 5), which enhances TC of 12 K, similarly to previous observations on bulk ceramics. With a reduced
resistivity (ρ<0.02 Ω cm), the obtained Pr-deficient film,
P□SMO, exhibits the best magneto-transport properties with a decreasing
magnetoresistance sensitivity at low field. 相似文献
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In this paper we study boundary value problems for perturbed second-order linear difference equations with a small parameter. The reduced problem obtained when the parameter is equal to zero is a first-order linear difference equation. The solution is represented as a convergent series in the small parameter, whose coefficients are given by means of solutions of the reduced problem. 相似文献
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Boudraa Kamel Bouchaour Tewfik Maschke Ulrich 《Journal of Thermal Analysis and Calorimetry》2020,140(4):1845-1857
Journal of Thermal Analysis and Calorimetry - In this work, we verified the synthesis of a novel sequential interpenetrating polymer network, composed of poly(2-hexyl-ethylacrylate) and... 相似文献
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Z.?Gabelica A.?Charmot R.?Vataj R.?Soulimane J.?Barrault S.?ValangeEmail author 《Journal of Thermal Analysis and Calorimetry》2009,95(2):445-454
Nanometric Fe2O3 particles could be inserted inside the internal pore volume of SBA-15 mesoporous silica and mesoporous alumina supports,
when Fe(III) chelates (EDTA, gluconate or citrate) were used as impregnating precursors. The oxidative degradation of the
chelating anions was followed by combined TG-DTA. Strong chelate-SiOH interactions (case of bulky EDTA), favored by the mesopore
curvature, yield sub-nanometric extremely well dispersed Fe2O3 particles preferentially located at the micropore mouths (confinement effect). Fe2O3 even more strongly interacts with alumina walls, generating either (Fe,Al)2O3 mixed phases or Fe-aluminate micro domains. These iron-based mesoporous alumina composites proved very active catalysts in
total oxidation of phenol at ambient conditions, with extremely low iron leaching (0.2%). 相似文献
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We study the stability loss delay phenomenon in a dynamic transcritical bifurcation in a class of three-dimensional prey and predator systems. The dynamics of the predator is assumed to be slow comparatively to the dynamics of the prey. As an application, a well-known model considered by Clark will be discussed. 相似文献
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Summary: The swelling properties of photochemically crosslinked poly(n-butyl acrylate) (PABu) networks in isotropic and anisotropic solvents were investigated experimentally. The purpose of this study was to examine the swelling kinetics of PABu networks in isotropic solvents and to compare the results obtained which those observed in the case of the low molecular weight liquid crystal 4-cyano-4′-n-pentyl-biphenyl known as 5CB. The phase diagrams were established in terms of composition and temperature for isotropic solvents, as toluene, acetone, cyclohexane, and methanol, and 5CB, using the plateau values corresponding to equilibrium states of swelling. The polymer networks were prepared via free radical polymerization/crosslinking processes by ultraviolet (UV) radiation of initial mixtures made up from a monomer, a crosslinker, and a photoinitiator. PABu networks with several crosslinking densities were formed using different quantities of difunctional monomer hexanedioldiacrylate (HDDA). Immersion of these networks in excess solvent allows measuring the solvent uptake by determination of the weight in isotropic solvents and diameter in an anisotropic solvent (5CB). Swelling data were rationalized by calculating weight and diameter ratios considering swollen to dry network states of the samples. 相似文献
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Frank Seela Tewfik Soulimane Kann Mersmann Thomas Jürgens 《Helvetica chimica acta》1990,73(7):1879-1887
Nucleobase-anion glycosylation (KOH, tris[2-(2-methoxyethoxy)ethyl]amine (TDA-1), MeCN) of the pyrrolo[2,3-d]pyrimidines 4a – d with 5-O-[(1,1-dimethylethyl)dimethylsilyl]-2,3-O-(1-methylethylidene)-α-D -ribo-furanosyl chloride ( 5 ) gave the protected β-D -nucleosides 6a – d stereoselectively (Scheme 1). Contrary, the β-D -halogenose 8 yielded the corresponding α-D -nucleosides ( 9a and 9b ) apart from minor amounts of the β-D -anomers. The deprotected nucleosides 10a and 11a were converted into 4-substituted 2-aminopyrrolo[2,3-d]-pyrimidine β-D -ribofuranosides 1 . 10c , 12 , 14 , and 16 and into their α-D -anomers, respectively (Scheme 2). From the reaction of 4b with 5 , the glycosylation product 7 was isolated, containing two nucleobase moieties. 相似文献