- PREREQUISITE FOR OSCILLATORY BEHAVIOUR IN THE MALONIC ACID, BROMATE AND CATALYST REACTING SYSTEMS.
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The role of bromomalonic acid was investigated in Belousov-Zhabotinsky systems, in the preoscillatory period. It was established that the crucial bromomalonic acid concentration (at which the trasition from non-oscillatory behavior to the oscillatory one occurs) depends on the initial reactant concentrations. This relationship is closely connected to the rate equation describing the formation of bromomalonic acid in the preoscillatory period. On the basis of the solution of the rate equation the crucial bromomalonic acid concentration can be calculated. From the temperature dependence of the rate constants, the activation energy of the bromomalonic acid formation during the preoscillatory period was calculated.
- Burger,Koros
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- Effect of pulsed illumination on the belousov-zhabotinsky reaction catalyzed with tris(bipyridine) ruthenium(II) in continuous stirred tank reactor
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The photochemical response of BZ reaction with photosensitive Ru(bpy)32- has been studied under pulsed illumination in a continuous-flow stirred tank reactor, CSTR. Two types of photo-response, the advanced and delayed phase shifts of oscillation, are observed depending on the initial concentrations of malonic acid (MA) or Br- and the timing of a pulsed illumination.
- Matsumura-Inoue, Takeko,Nakamura, Tatsuhito,Mori, Yoshihito,Hanazaki, Ichiro
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- Perturbation mechanism and phase transition of AOT aggregates in the Fe(II)[batho(SO3)2]3 - catalyzed aqueous Belousov-Zhabotinsky reaction
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Surfactant AOT (sodium bis(2-ethylhexyl)sulfosuccinate) was introduced up to 200 mmol L-1 in the aqueous Belousov-Zhabotinsky (BZ) medium. Both the induction period (IP) and the oscillation period (τ) of the BZ waves decreased significantly, whereas the wave velocity (v) increased with the concentration of AOT. These tendencies were explained in terms of the perturbations to the FKN mechanism through the uptake of Br2 and BrO2· into the hydrophobic core of AOT aggregates. In addition, the structures and the phase transition of AOT aggregates were suggested based on the measurement of surface tension and the correlation analysis of the IP, τ and v values.
- Jahan, Rumana A.,Suzuki, Kosuke,Mahara, Hitoshi,Nishimura, Satoshi,Iwatsubo, Takashi,Kaminaga, Akiko,Yamamoto, Yasuhiko,Yamaguchi, Tomohiko
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- Electrical Pulses To Determine Chemical Phase Response Curves
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We report several series of single perturbation experiments in the Belousov-Zhabotinsky (BZ) reaction which have been carried out by applying an electrical current to a platinum electrode in the continuous flow stirred tank reactor (6.4 mL).When a single short current pulse is applied at the maximum of a chemical oscillation (high Ce4+ concentration) or at the minimum (low Ce4+), the response is a small advance or a significant delay of the original phase of oscillation (negative or positive phase shift), respectively.Thus we obtain phase response curves as a function of electrical current strength and duration of the pulses.These results show that the redox reactions occuring at the platinum electrodes involve mainly the Ce3+/Ce4+ redox couple as supported by pulsed additions of known Ce4+ solutions.Numerical simulations are in good agreement with the experiments.
- Dechert, G.,Lebender, D.,Schneider, F. W.
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- The Potentiometric Effect of As(III) Ion on a Belousov-Zhabotinskii Oscillating Chemical Reaction. Application to the Determination of As(III)
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A novel analytical method that builds on specific features of non-linear chemical systems far from thermodynamic equilibrium is described. The used oscillating chemical system is the BZ (Belousove-Zhabotinskii) reaction in a non-equilibrium stationary state close to a bifurcation point. The method uses a Pt electrode for monitoring the potential response to a perturbation caused by As(III) ion. A linear response, in which the oscillating amplitude varies versus the logarithm of the As(III) concentration, was found in the range of 1.99 * 10-6-1.27 * 10-4 M. Under optimum conditions, a detection limit of 2 * 10-6 M for As(III) was obtained. The relative standard deviation (%RSD) for As(III) 1.59 * 10-5 M is 7.1 (n = 6).
- Ojani, Reza,Raoof, Jahanbakhsh,Mahdavi, Fathemeh
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- Stratification in a Thin-Layered Excitable Reaction-Diffusion System with Transverse Concentration Gradients
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Chemical waves propagate in thin gel layers saturated with Belousov-Zhabotinsky (BZ) reaction solution.When a layer is in contact with air, weakly interacting waves can propagate along the top and the bottom of the layer.Experiments on the ferrion-catalyzed BZ reaction with stepwise layers reveal a poorly excitable sublayer in the middle of the layer.We propose that in a BZ excitable layer open to air two opposite transverse concentration gradients are established, those of oxygen and bromine.The bromine gradient results in a parallel gradient of the total concentration of bromo derivatives of malonic acid (BrMAs).The threshold of excitability increases with the concentrations of oxygen and of BrMAs.As a result, the excitability threshold varies nonmonotonically, with a maximum in the middle of the layer.If this maximum of the excitability threshold is high enough, a poorly excitable sublayer appears between the two excitable sublayers at the top and bottom.The wave propagation and interaction have been simulated using an Oregonator-type model with a nonmonotonic vertical profile of the stoichiometric factor q that relates Br- production to ferriin reduction.The simulation confirms that the observed stratification of layers can be explained by the established mechanism of the BZ reaction supplemented with molecular diffusion.
- Zhabotinsky, Anatol M.,Gyoergyi, Laszlo,Dolnik, Milos,Epstein, Irving R.
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- Stoichiometry of Bromide Production from Ceric Oxidation of Bromomalonic Acid in the Belousov-Zhabotinskii Reaction
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We investigated the number of Ce4+ ions required to produce one Br- ion in the oxidation of bromomalonic acid by Ce4+ under conditions appropriate to the oscillating Belousov-Zhabotinskii (BZ) reaction.We found a ratio of 1:1, in agreement with earlier results by Jwo and Noyes (J.Am.Chem.Soc. 1975, 97, 5422), in the presence of oxygen.With oxygen excluded from the system, we found a ratio of 2:1.The presence of malonic acid in the system had no effect on the bromide production, contrary to the assumption of recent theoretical models of the Belousov-Zhabotinskii reaction.
- Foersterling, Horst-Dieter,Stuk, Linda,Barr, Alexander,McCormick, William D.
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- Kinetics of Chemical Waves in the Acidic Bromate-Malonic Acid-Ru(bpy)32+ System in Comparison with the Ferroin System
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Propagation of trigger waves investigated in the acidic bromate-malonic acid-Ru(bpy)32+ system.In excitable but not oscillatory solutions the concentration dependence of wave velocity ν follows the equation ν = 2(kR1Dx)1/2()1/2 - ν0.Concentration and temperature dependence of wave velocity coincide quantitatively with the corresponding results from BZ systems containing ferroin as catalyst.In solutions with coexisting phase and trigger waves the trigger wave velocities follow the empirical law ν ca. 1.261.68.
- Kuhnert, L.,Krug, H.-J.
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- Deuterium isotope effect on the induction period of the cerium catalyzed Belousov-Zhabotinsky reaction
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In this work we present results about the deuterium isotopic effect on the global kinetics of a cerium catalyzed Belousov-Zhabotinsky reaction. A nonlinear dependence of the induction period upon the percentage of deuterated reactants was found in batch conditions. In order to understand this result, we investigated two reaction pathways responsible for the length of the induction period, namely: (a) the reaction between the enolic form of the malonic acid with molecular bromine and (b) the oxidation of malonic acid by the Ce(IV) ion. In both cases we obtained a linear dependence of the kinetic constants on the percentage of deuterated reactants. Nevertheless, by inserting the experimental values in the MBM (Marburg-Budapest-Missoula) model, we were able to qualitatively simulate the observed trend of the induction period.
- Rossi, Federico,Simoncini, Eugenio,Marchettini, Nadia,Tiezzi, Enzo
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- Measurement of Convection Velocities in "Mosaic" Patterns
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Experimental evidence is given of the occurence of convection in a liquid layer of an oscillatory BZ reagent, sandwiched between two glass plates.Quantitative data on the hydrodynamic velocities are reported for three different layer depths.It is shown that convective motions result from inhomogeneities spontaneously occuring in the chemical reaction.
- Rodriguez, J.,Vidal, C.
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- Malonic acid concentration as a control parameter in the kinetic analysis of the Belousov-Zhabotinsky reaction under batch conditions
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The influence of the initial malonic acid concentration [MA]0 (8.00 × 10-3≤ [MA]0≤ 4.30 × 10 -2 mol dm-3) in the presence of bromate (6.20 × 10-2 mol dm-3), bromide (1.50 × 10-5 mol dm-3), sulfuric acid (1.00 mol dm-3) and cerium sulfate (2.50 × 10-3 mol dm-3) on the dynamics and the kinetics of the Belousov-Zhabotinsky (BZ) reactions was examined under batch conditions at 30.0°C. The kinetics of the BZ reaction was analyzed by the earlier proposed method convenient for the examinations of the oscillatory reactions. In the defined region of parameters where oscillograms with only large-amplitude relaxation oscillations appeared, the pseudo-first order of the overall malonic acid decomposition with a corresponding rate constant of 2.14 × 10-2 min-1 was established. The numerical results on the dynamics and kinetics of the BZ reaction, carried out by the known skeleton model including the Br2O species, were in good agreement with the experimental ones. The already found saddle node infinite period (SNIPER) bifurcation point in transition from a stable quasi-steady state to periodic orbits and vice versa is confirmed by both experimental and numerical investigations of the system under consideration. Namely, the large-amplitude relaxation oscillations with increasing periods between oscillations in approaching the bifurcation points at the beginning and the end of the oscillatory domain, together with excitability of the stable quasi-steady states in their vicinity are obtained. the Owner Societies.
- Blagojevic, Slavica M.,Anic, Slobodan R.,Cupic, Zeljko D.,Pejic, Natasa D.,Kolar-Anic, Ljiljana Z.
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- Some Statements Concerning Oscillatory Phenomena
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This work attempts to provide a new theoretical model for oscillating chemical systems based on phase exchange and pulsating supersaturation.Phase exchange is of two types: one is steady exchange from the solution to the gas above it while the other is pulsating exchange between nucleations of bubbles of gas and the solution.The pulsating supersaturation allows nucleations of bubbles to form and oscillations to take place.We consider several variables, viz. temperature, bulk reaction, volume and size of the reactor, rate of stirring and pressure, and study their influence on the oscillations.The theoretical results are compared with some experimental results that can be explained by our new model.The system considered are the oxidation of malonic acid by bromate or iodate with cerium as catalyst and the oxidation of oxalic acid and formic acid.
- Alba, Francesca D',Lorenzi, Sergio Di
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- Quantitative Measurement of Intermediate Species in Sustained Belousov-Zhabotinsky Oscillations
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Sustained Belousov-Zhabotinsky oscillations have been performed in an open continuous-fed reactor, controlled by a computer.A procedure of repeated storage and accumulation of the signal given by any kind of detector allows the identification of several intermediate species and their concentration measurement with a good accuracy.By means of spectrophotometric as well as potentiometric techniques we have so obtained the concentration time dependence of Ce3+, Ce4+, Br2, Br-, bromomalonic compounds (BrMA), O2, and CO2.These species cannot account for the overall ligh t absorption in the UV range (280-320nm), so that at least another one, which we could not identify, is involved.A detailed analysis of our experimental results points out for a general agreement with the mechanism already proposed by Field, Koeros, and Noyes.
- Vidal, C.,Roux, J. C.,Rossi, A.
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- Spiral Waves in the Homogeneous and Inhomogeneous Belousov-Zhabotinsky Reaction
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The model of the ferroin-catalyzed Belousov-Zhabotinsky reaction is modified for the temperature range 10-30 deg C, which is more appropriate for experiments.In the concentration range explored, a vortex rotates around a stationary circular core.However, in an inhomogeneous medium, it drifts along the boundary of the inhomogeneity.The computations fit experiments well for all measured spiral wave parameters.
- Aliev, R. R.,Rovinsky, A. B.
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- Experimental Study of Spiral Waves in the Ce-Catalyzed Belousov-Zhabotinskii Reaction
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Systematic measurements of spiral wave characteristics (rotation period, normal velocity, wavelength, and wave form) in the cerium-catalyzed BZ reaction were carried out over a wide range of reagent concentrations.These data provide a stringent test for theoretical models of the reaction.Numerical calculations of spiral wave solutions to modified Oregonator equations are in satisfactory agreement with the experimental results.
- Nagy-Ungvarai, Zs.,Tyson, J. J.,Mueller, S. C.,Watson, L. T.,Hess, B.
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- Synthesis and properties of dipyridemium betaines of derivatives of 1,4-benzoquinone and tetracyanoquinodimethane
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Reaction of chloranil with excess pyridine gives the poorly stable 2,5-di(N-pyridinium)-3,6-dichloro-1,4-benzoquinone dichloride which is readily hydrolyzed to give the bisbetaine of 2,5-di(N-pyridinium)-1,4-benzoquinone-3,6-dioxide. Treatment with acid g
- Yanchishin,Karlivan,Valter
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- Optical Communication among Oscillatory Reactions and Photo-Excitable Systems: UV and Visible Radiation Can Synchronize Artificial Neuron Models
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Neuromorphic engineering promises to have a revolutionary impact in our societies. A strategy to develop artificial neurons (ANs) is to use oscillatory and excitable chemical systems. Herein, we use UV and visible radiation as both excitatory and inhibitory signals for the communication among oscillatory reactions, such as the Belousov–Zhabotinsky and the chemiluminescent Orban transformations, and photo-excitable photochromic and fluorescent species. We present the experimental results and the simulations regarding pairs of ANs communicating by either one or two optical signals, and triads of ANs arranged in both feed-forward and recurrent networks. We find that the ANs, powered chemically and/or by the energy of electromagnetic radiation, can give rise to the emergent properties of in-phase, out-of-phase, anti-phase synchronizations and phase-locking, dynamically mimicking the communication among real neurons.
- Gentili, Pier Luigi,Giubila, Maria Sole,Germani, Raimondo,Romani, Aldo,Nicoziani, Andrea,Spalletti, Anna,Heron, B. Mark
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p. 7535 - 7540
(2017/06/13)
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- 1-Malonyl-1,4-dihydropyridine as a novel carrier for specific delivery of drugs to the brain
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A group of 1-malonyl-1,4-dihydropyridine derivatives were synthesized as novel carrier systems for site-specific and sustained drug delivery to the brain. Such carriers are expected to be stable against air oxidation due to the presence of the carbonyl group close to nitrogen of the dihydropyridine. These carrier systems were attached to a group of different aldehydes to afford novel quaternary pyridinium derivatives 9a-e, 11a-d, 13 and 18a-b. Reduction of the prepared quaternary pyridinium derivatives with sodium dithionite afforded a novel group of 1-malonyl-1,4-dihydropyridine chemical delivery systems (CDSs) 10a-e, 12a-d, 14 and 19a-b. The synthesized 1-malonyl-1,4-dihydropyridine CDSs were subjected to various chemical and biological investigations to evaluate their ability to cross the blood-brain barrier, and to be oxidized biologically into their corresponding quaternary derivatives. The in vitro oxidation studies showed that most of the 1-malonyl-1,4-dihydropyridine CDSs could be oxidized into their corresponding quaternary derivatives at an adequate rate. The in vivo studies showed that compounds 10c and 14 were able to cross the blood-brain barrier at detectable concentrations. Moreover, the pyridinium quaternary intermediates 9a, 9c, 13, 18a and their corresponding dihydro derivatives 10a, 10c, 14 and 19a were screened for their antidepressant activity using tail suspension behavioral despair test compared to imipramine as a reference at a dose level of 10 mg/kg. The results indicated that compounds 13, 14 and 19a induced remarkable antidepressant activity comparable to imipramine. Compounds 10a, 10c and 18a exhibited good antidepressant activity, their activities nearly equal to 92.8%, 86.7% and 90.20% of the activity of imipramine, respectively. The other derivatives 9a and 9c exhibited moderate antidepressant activity compared with imipramine.
- Hassan, Heba A.,Abdel-Aziz, Mohamed,Abuo-Rahma, Gamal El-Din A.A.,Farag, Hassan H.
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p. 1681 - 1692
(2009/08/07)
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- New chaotic behavior and its effective control in Belousov-Zhabotinsky reaction
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A new "spiral-in-to-spiral-out" mixed-mode type chaos of the Belousov-Zhabotinsky (BZ) reaction in a continuous flow stirred tank reactor (CSTR) is observed. We discussed its evolution and characterization in detail. We controlled the new chaos into steady periodic behavior by two control methods: (i) a self-adaptive delayed feedback controlling scheme; and (ii) a linear self-interacting feedback controlling scheme.
- Li,Song,Cai,Chen,Hou,Wei,Wu,Zhao
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- Halogenation of malonic acid and malonic acid monomethyl ester. Enolisation pathways and enol reactivity.
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Reactions of iodine (2 * 10-5 mol dm-3) and bromine (5 * 10-5 mol dm-3) in water with malonic acid (MAL) (in large excess) are first-order in and in and are independent of acidity in the range 0.02-0.16 mol dm-3 H+.These results are consistent only with a rate-limiting reaction between the halogen and the enol form of MAL.Evidence is presented that these reactions occur at the diffusion limit and the results enable a value for KE (the equilibrium constant for enolisation) of 7.4 * 10-9 to be deduced.At a much higher bromine concentration (ca. 2 * 10-3 mol dm-3) the reaction is zero-order in , consistent with a rate-limiting enolisation.Values of ke (the rate constant for enolisation) for MAL and for malonic acid monomethyl ester (EHM) are reasonably similar (4.0 * 10-3 and 1.1 * 10-3 s-1, respectively) and are about 102 greater than the value for diethyl malonate, supporting a mechanism of enolisation involving internal H+ transfer for both MAL and EHM.Under conditions zero-order in , the dependence of the observed rate constant upon the total stoichiometric concentration of malonic acid T over the pH range 1.0-4.3 enables the kinetic identification of a reaction pathway involving base catalysis by malonate ion in addition to the solvent promoted reaction which is dominant at lower pH.At higher pH values there is evidence of a third pathway involving malonate ion catalysis of enolisation of the malonate ion.
- Eberlin, Alex L.,Williams, D. Lyn H.
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p. 883 - 888
(2007/10/03)
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- Characteristics of the effect of acoustic waves at different frequencies on the reduction of bromate ions by malonic acid
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The influence of ultrasonic waves at frequencies of 22 kHz and 1 MHz as well as low-frequency acoustic fields on the malonic acid - bromate ions - cerium ions - sulphuric acid chemical system was examined.It was noted that the nature of the effect of acoustic fields at different frequencies on the principal parameters of the autooscillations of the reactions is identical but the effectiveness of their action varies.It was shown that the observed increase in the effectiveness of acoustic vibrations with increase in frequency is associated with increase in the initial chemical-acoustic yield of H2O2 as the frequency of the acoustic waves increases.
- Maksimenko, N. A.,Margulis, M. A.
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p. 1174 - 1176
(2007/10/02)
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- Investigation of Radical Reactions Important in the Gyoergyi-Turanyi-Field Model of the Belousov-Zhabotinskii Reaction
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In the Gyoergyi-Turanyi-Field (GTF) model of the Belousov-Zhabotinskii (BZ) reaction, malonyl radicals (MA.) and bromomalonyl radicals (BrMA.) are assumed to be important intermediates.The hydrogen abstraction reactions MA. + BrMA -> MA + BrMA. (a) and BrMA. + MA -> BrMA + MA. (b) (MA, malonic acid; BrMa, bromomalonic acid) transfer from free-radical nature of the malonyl species to the bromomalonyl species and vice versa.The rates of these two reactions determine in part the relative importance of these radical intermediates.Another key radical reaction is BrMA. + Ce4+ + H2O -> BrTTa + Ce3+ (c) (BrTTA, bromotartronic acid), which is a source of Br- through decomposition of BrTTA in the model.It has been deduced from ESR and spectrophotometric experiments that reactions a-c do not contribute to the chemistry of the BZ reaction.Numerical integration of the GTF rate equations, omitting reactions a-c, shows no oscillation in BZ systems with high initial concentrations of BrMA.Experimentally, these systems exhibit oscillations with no induction period.
- Foersterling, Horst-Dieter,Stuk, Linda
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p. 7320 - 7325
(2007/10/02)
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- Thermodynamics of Protonation and Copper(II) Complex Formation of α-Aminomalonic acid
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The thermodynamic function (ΔG0, ΔH0 and ΔS0) for the protonation of α-aminomalonic acid were determined in aqueous solution (25 deg C, I=0.1 mol dm-3 NaCl).The basicity constants and enthalpy changes were evaluated from potentiometric and calorimetric data for both the primary amino and the carboxylate groups.On the basis of the thermodynamic changes a closed structure is hypothesized with the protonated amino nitrogen hydrogen-bonded to both the carboxylate groups to form two five-membered rings.The protonation of the CO2- groups provokes opening of the ring s.A relatively high stability constant for complexation with Cu2+ was determined, however in a narrow range of low pH.The co-ordination to the copper(II) occurs both with nitrogen and the two oxygen donor atoms, to form two five-membered chelate rings.
- Barbucci, Rolando,Casolaro, Mario,Fini, Adamo
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p. 207 - 211
(2007/10/02)
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- CHEMICAL TEMPORAL AND SPATIAL STRUCTURES IN STRONG MAGNETIC FIELD
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Temporal and spatial structures in the Belousov-Zhabotinskii systems in constant electric and strong magnetic fields are studied in this paper.Unlike a random generation of chemical wave center in a system without the influence of an electromagnetic field we have observed that only one wave forms in the presence of electric and magnetic fields of suitable intensity and induction.Its speed of propagation depends on the connected fields.A theory of this phenomenon has been developed and the obtained results are in a good agreement with experimentally measured dependences of the temporal period of chemical waves on electric field intensity and magnetic field induction.
- Krempasky, Julius,Smrcinova, Miroslava
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p. 1232 - 1243
(2007/10/02)
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- New Strategies for Studies on the Kinetics and Energetics of the Belousov-Zhabotinskii Reaction
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The oscillatory Belousov-Zhabotinskii reaction and its subsystems were studied by ca. 1700 DTA and UV experiments performed at linearly increased temperature.The starting concentrations of bromate, bromide, catalyst, and malonic acid were varied in order to obtain "concentration codes" of such series.These represent the dependence of any parameters in discrete ranges of the starting concentrations of the different components.Particularly adequate for a model check are the mechanistic codes (= MCC's), which concern the shape index and reaction type index: If these mechanistic coordinates remain constant in such a concentration interval, other data, e.g. activation energies, can be attributed to a rate-determining process. - The results led to a nine-step model which is based on the FKN mechanism and is capable of roughly reproducing the influence of the initial concentrations and heating rate on 11 parameters characteristic of the envelope and of the oscillations of the experimental signals.The MCC's of the experimental and theoretical series are similar, revealing 4-5 rate-determining steps in the different concentration ranges. - The activation energies agree with values from the literature, cited for three steps; these and further resulting activation energies are consistent with our studies with subsystems. - Key words: Catalysis / Chemical Kinetics / Computer Experiments / Oscillatory Chemical Reactions / Thermal Analysis
- Koch, E.,Nagy-Ungvarai, Zs.
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p. 1375 - 1386
(2007/10/02)
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- Thorough Study of Bromine Control in Bromate Oscillators. 4. A Quantitative and Comparative Study on Silver Ion Perturbed Belousov-Zhabotinsky Systems
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The distribution of bromine between bromoorganics and bromide was followed in Ag(1+)-perturbed Belousov-Zhabotinsky (BZ) systems and the rate of the Br(1-) removing reaction (Ag(1+) + Br(1-) --> AgBr) was measured.A rate constant in the order of 1E-4 M-1s-1 was obtained for the reaction.A comparision of bromine distribution in Ag(1+)-perturbed malonic acid and and malic acid containing BZ systems revealed the difference in their oscillatory behavior.
- Varga, Margit,Koeroes, Endre
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p. 4373 - 4376
(2007/10/02)
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- STUDY OF THE PREOSCILLATORY PERIOD OF THE BELOUSOV-ZHABOTINSKY SYSTEM
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The conditions for the onset of chemical oscillation were investigated in the bromate, malonic acid, sulphuric acid (or nitric acid) and catalyst reacting systems.We determined the critical bromomalonic acid concentration and established how this value depends on the bromate-, malonic acid- and catalyst concentrations.On the basis of kinetic measurements we described the rate equations for the formation of bromomalonic acid in te preoscillatory period.
- Ungvarai-Nagy, Zs.,Koeroes, E.
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