- Mesoporous carbon supported platinum nanocatalyst: Application for hydrogen production by HI decomposition reaction in S-I cycle
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Platinum supported on carbon as a catalyst is widely reported and have a wide range of applications ranging from fuel cell application to hydrogenation reactions, where structure and properties of carbon support play an important role in the functioning of the catalyst. Mesoporous carbon supported platinum nanocatalyst was synthesized by hard templating route using mesoporous silica as template. The catalyst prepared has been characterized by X-ray diffraction, Raman, SEM, TEM, XPS and BET surface area. This catalyst has been employed for liquid phase HI decomposition reaction of sulfur iodine thermochemical cycle for production of hydrogen. The catalyst was evaluated for its activity for HI decomposition reaction and stability in the reaction environment. From present study we conclude that Pt supported on mesoporous carbon is a suitable and stable catalyst for liquid phase HI decomposition reaction.
- Tyagi, Deepak,Varma, Salil,Bharadwaj, Shyamala R.
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- Studies of chemical reactivity in the condensed phase. I. The dynamics of iodine photodissociation and recombination on a picosecond time scale and comparison to theories for chemical reactions in solution
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Picosecond transient absorption measurements from 1000-295 nm are used to monitor the recombination dynamics of iodine after photodissociation in a variety of inert solvents.The high time resolution and signal-to-noise ratio of these measurements permits the development of a detailed model of this reaction, which should resolve disagreements over the time scales of geminate recombination and vibrational relaxation and over the role of excited electronic state trapping.Most of the atoms which undergo geminate recombination do so in 15 ps, in agreement with the predictions of existzng molecular dynamics simulations.The subsequent vibrational and electronic energy relaxation of the recombined molecule is relatively slow and accounts for most of the transient absorption dynamics.The relaxing X state vibrational population distribution is extracted with an approximate method using calculated spectra of the excited vibrational levels and is compared to recent models.Vibrational relaxation times vary from ca. 15 ps near the middle of the ground state well to ca. 150 ps for complete relaxation to v = 0.The vibrational relaxation rates do not provide support for the predicted role of resonant vibration-to-vibration energy transfer to chlorinated methane solvents, but some evidence for this mechanism is found in alkane solvents.B-state predissociation times of 10-15 ps and A '-state lifetimes of 65-2700 ps are found depending on the solvent.Current theory is not able to satisfactorily explain the large variation of the A '-state lifetime in various solvents.
- Harris, A. L.,Berg, M.,Harris, C. B.
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- Photochemistry of alkyl halide dimers
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Dimers and other small clusters of CH3I, C2H5I, i- and n-C3H7I, HI, CF3I, CH3Br, and C2H5Br formed in a supersonic expansion are irradiated at 248 and 193 nm and the halogen molecule product probed via laser induced fluorescence spectroscopy.Both dimers and larger clusters of RI (R = H, alkyl) excited at each wavelength yield I2 in its ground electronic state with very little internal energy.Clusters of CF3I and those containing alkyl bromides do not give halogen molecule products after excitation at either wavelength.A model for the dynamics in the dimer excited state which explains these results is presented.
- Fan, Y. B.,Randall, K. L.,Donaldson, D. J.
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- Chlorite-Iodide Reaction: A Versatile System for the Study of Nonlinear Dynamical Behavior
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The autocatalytic reaction between chlorite and iodide ions exhibits a remarkable range of dynamical behavior.In a stirred tank reactor it shows bistability between steady states and between a steady and an oscillatory state.It forms the core of a large f
- Kepper, Patrick De,Boissonade, Jacques,Epstein, Irving R.
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- The Decomposition of Hydrogen Iodide and Separation of the Products by the Combination of an Adsorbent with Catalytic Activity and a Temperature-swing Method
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The decomposition of hydrogen iodide and the separation of the products by the combination of a column packed with an adsorbent with catalytic activity (platinum-supported active carbon, 2.3 wtpercent) and a temperature-swing method (450-900 K) are carried out, and the features and the problems of the method are examined.A one-step conversion of hydrogen iodide, 70percent, is obtained at 450 K, where the equilibrium conversion is 13percent.It is shown that the products of the decomposition of hydrogen iodide containing water are separated from each other.
- Oosawa, Yoshinao
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- Bi2(IO4)(IO3)3: A new potential infrared nonlinear optical material containing [IO4]3- anion
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A new potential infrared (IR) nonlinear optical (NLO) material Bi 2(IO4)(IO3)3 was synthesized by hydrothermal method. Bi2(IO4)(IO3)3 crystallizes in the chiral orthorhombic space group P212 121 (No. 19) with a = 5.6831(11) A, b = 12.394(3) A, and c = 16.849(3) A. It exhibits a threedimensional framework through a combination of the IO3, IO4, BiO8, and BiO9 polyhedra and is the first noncentrosymmetric (NCS) structure containing [IO4]3- anion. Bi2(IO 4)(IO3)3 has an IR cutoff wavelength of 12.3 ?m and belongs to the type 1 phase-matchable class with a moderately large SHG response of 5 × KDP, which is in good agreement with the theoretical calculations.
- Cao, Zhenbo,Yue, Yinchao,Yao, Jiyong,Lin, Zheshuai,He, Ran,Hu, Zhanggui
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- The Oscillatory Briggs-Rauscher Reaction. 1. Examination of Subsystems
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In acidic aqueous solution at 25 deg C, only slow or nonexistent reaction is observed for any two of three species iodate ion, hydrogen peroxide, and manganous ion.However, if all three species are present, 0.002 M Mn2+ catalyzes the iodate oxidation of peroxide at a rate almost 1000 times that in the absence of a catalyst! This remarkable observation, which has already been reported by Cooke, can be explained by postulating that the radical oxidant *IO2 is very sluggish at abstracting hydrogen atoms from the species like H2O2 but can oxidize Mn2+ by electron transfer.A detailed mechanism has been proposed that models semiquantitatively not only the manganous catalyzed iodate oxidation of peroxide but also the simultaneous induced disproportionation of the peroxide and the fact that the concentration of elementary iodine does not increase to a limiting value but rises to a maximum and then decreases toward a small value.Despite this single extremum, the subsystem does not exhibit oscillatory behavior.
- Furrow, Stanley D.,Noyes, Richard M.
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- Formation of volatile iodine compounds under hot concentrated acid conditions (nitric acid or aqua regia) and in diluted acid solutions with or without thiocyanate
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It is reported that iodine volatilization can occur in any elemental analysis of total iodine by ICP-MS. This problem affects the accuracy of the results, and it has been neither rationalized nor solved up to now. In this work, the formation of volatile iodine compounds in concentrated acid solutions (nitric acid or aqua regia) under microwave heating was studied by UV–Vis spectrophotometry, linear sweep voltammetry, and cyclic voltammetry. It was evidenced that molecular iodine (I2) can unexpectedly form in concentrated hot HNO3solutions, irrespective of the starting iodine compound (iodide, iodate, periodate, 3-iodo-L-tyrosine, 3,5-diiodo-L-tyrosine dehydrate). I2is produced by the nitrogen oxides existing in these conditions. The formation of volatile iodine is minimized in aqua regia, as chloride is able to keep iodine in solution due to the formation of charged chloro-iodo complexes (e.g. I2Cl?). The dilution of the concentrated acid solution, required prior to the ICP-MS analysis, causes the disruption of I2Cl?so that I2can again volatilize. To avoid this, 0.1 M thiocyanate can be added, as it forms a strong I2SCN?complex which keeps I2in solution as ion. Also other iodine species possibly occurring in the explored conditions, iodide and iodate, were demonstrated to be converted to I2SCN?in diluted HNO3solutions and in the presence of 0.1 M thiocyanate. Recovery tests demonstrated that iodine volatilization is minimized if samples containing iodine are treated in aqua regia and, after dilution, they are added with 0.1 M thiocyanate.
- Badocco, Denis,Romanini, Francesca,Di Marco, Valerio,Mondin, Andrea,Pastore, Paolo
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- Synthesis and Characterization of 2-Pyridinylmethylene-2-quinolyl Hydrazone Cobalt(III) Complexes. Reactivity Trends and Solvent Effect on the Initial and Transition States of Base Catalyzed Hydrolysis
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The complexes of pyridine-2-aldehyde-2-quinolylhydrazone Co(III) nitrate [Co(paqh)2](NO3)2, methyl-2-pyridylketone-2-quinolinhyrazone Co(III) nitrate [Co(mpkqh)2](NO3)2, and phenyl-2-pyridylketon-2-quinolinhyrazone Co(III) nitrate [Co(ppkqh)2](NO3)2 were prepared and characterized. Solubilities of Co(III)–hydrazone complexes were measured. Transfer chemical potentials were calculated from the measured solubilities of the Co(III) complexes in aqueous methanol mixtures at 25?°C. The reactivity trends in the transfer chemical potentials are discussed in terms of the nature of the bonded ligands. Kinetics of the base hydrolysis of Co(III)–hydrazone complexes in the aqueous methanol mixtures have been studied at 25?°C, and follow the rate law kobs?=?k2[OH?]. The solvent effects on the reactivity trends of Co(III) complexes are analyzed into initial state (is) and transition states (ts) components. The reaction rates are reduced by the increase of methanol content. The destabilization of the transition state is remarkable compared to the initial state in the aqueous methanol mixtures. The initial state is more hydrophobic in nature than the transition state for Co(III) complex reactions.
- Mohamad, Ahmad Desoky M.
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- Quantum yields for the photodissociation of iodine in compressed liquids and supercritical fluids
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Quantum yields of photodissociation were determined for iodine in compressed liquid n-alkanes and supercritical CO2 and xenon after laser excitation at 532 nm. The quantum yield decreases nearly linearly with increasing density. No cluster effe
- Schwarzer,Schroeder,Schroeder
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- Kinetics of the Oxidation of Substrate Ligands by Transition-metal Cations
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The kinetics of the oxidation of iodide ions by CeaqIV have been investigated.The reaction is found to be first order in each of IV>, and , in contrast to the oxidation of Br(1-) by CeaqIV, which is second order in both and .Nevertheless, the direct order of one in found for the CeIV + I(1-) reaction can only be interpreted by assuming the involvement of intermediate Ce(4+) - I(1-) complexes.The second-order rate constant for the oxidation of I(1-) by CoaqIII is shown to vary with ionic strength, so the entalphy ΔH* and entropy ΔS* of activation have been determined in conditions where the rate is invariant with ionic strength.These values for ΔH* and ΔS* are compared with the values for other substrates.The oxidation of iodide ions is discussed in relation to a general mechanism for the oxidation of substrate ligands by aquatransition-metal cations.
- Nazar, Abdul Fattah M.,Wells, Cecil F.
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- Iodine emission in the presence of humic substances at the water's surface
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Humic substances that preferentially adsorb at the air/water interfaces of water or aerosols consist of both fulvic and humic acid. To investigate the chemical reactivity for the heterogeneous reaction of gaseous ozone, O 3(g), with aqueous iodide, I-(aq), in the presence of standard fulvic acid, humic acid, or alcohol, cavity ring-down spectroscopy was used to detect gaseous products, iodine, I2(g) and an iodine monoxide radical, IO(g). Fulvic acid enhanced the I2(g) production yield, but not the IO(g) yield. Humic acid, n-hexanol, n-heptanol, and n-octanol did not affect the yields of I2(g) or IO(g). We can infer that the carboxylic group contained in fulvic acid promotes the I2(g) emission by supplying the requisite interfacial protons more efficiently than water on its surface.
- Hayase, Sayaka,Yabushita, Akihiro,Kawasaki, Masahiro
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- On-site detection of phosgene agents by surface-enhanced Raman spectroscopy coupled with a chemical transformation approach
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Phosgene and its analogs are greatly harmful to the public health, environmental safety and homeland security as widely used industrial substances with extremely high toxicity. In order to rapidly evaluate the emergency risk caused by these chemicals, a new highly sensitive method based on surface-enhanced Raman spectroscopy (SERS) technique for measurement of phosgene agents was developed for the first time. Coupled with a chemical transformation approach, the highly toxic phosgene was conveniently converted to a SERS-sensitive probe, i.e. iodine (I2), with low toxicity or non-toxicity. The characteristic SERS peak in 459 cm-1 was used for quantitation and was presumed as a formation of triiodide anion (I3-), which was induced in an iodide (I-)-aggregation Au NPs system. The total measurement can be completed in ~20 min with the limits of detection of ~60 μg/l (phosgene) and ~30 μg/l (diphosgene), respectively, on a portable Raman spectrometer. This work is the first report of SERS measurement on phosgene and diphosgene in a quantitative level. This method is expected to meet the requirements of on-site detection of phosgene agents, promote emergency responses and raise more opportunities for the portable SERS applications. A sensitive surface-enhanced Raman spectroscopy method for measurement of phosgene agents with a chemical transformation approach was reported for the first time. With the transformed product iodine, a more stable triiodide anion was formed in an iodide-aggregated Au nanoparticles system appeared as a characteristic ultraviolet-visible absorption peak at 352 nm and a surface-enhanced Raman spectroscopy peak of 459 cm-1. Three phosgene agents exhibit different reaction rates.
- Gao, Haiyue,Wu, Jianfeng,Zhu, Yingjie,Guo, Lei,Xie, Jianwei
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- Photochemistry of trimethyltin iodide in polar media: Orbital parentage and observed reactivity
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(CH3)3Snl exists as individual tetrahedral molecules in hexane but reacts with the silanol moieties present on the surface of porous glass and with the hydroxyl group of ethanol and hexanol to form five-coordinate adducts. With the exception of slight shifts to higher energy, formation of the adduct has little effect on the electronic spectrum of the complex, and the wavelength and O2 dependencies of the quantum yield of (CH3)3Snl disappearance indicate that the photochemistry of the complex initiates from the ligand-to-metal charge-transfer (LMCT) state populated on absorption in each medium. Nevertheless, 254 nm excitation in hexane leads to l2 and ((CH3)3Sn)2, whereas excitation of the five-coordinate adduct on the glass surface leads to l2, l3-, ((CH3)3Sn)2, and (CH3)3Sn-OSi≡ (OSi≡ represents a surface siloxyl), while in ethanol, l3- is the only detectable product. Regardless of the medium, the ground state is polarized and population of the LMCT state creates a more uniform charge distribution from which homolytic cleavage of the (CH3)3Sn-l bond is the dominant reaction pathway in each medium. In hexane, the (CH3)3Sn? and l? radicals couple to form ((CH3)3Sn)2 and l2, whereas adsorbed onto the glass, a fraction of the radical pairs thermalize via electron transfer to form l3- and a surface-bound (CH3)3Sn-OSi≡ species. In ethanol, excitation of the solvent adduct (CH3)3Sn-OHC2H5 leads to homolytic cleavage and l2 formation, which reacts thermally with (CH3)3Sn-OHC2H5 to form an [(CH3)3Sn+, l3-] ion pair.
- Dong, Jinquan,Devi, P. Sujatha,Sunil,Mendoza, Edgar,Gafney, Harry D.
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- Experimental and modeling study of oscillations in the chlorine dioxide-iodine-malonic acid reaction
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At pH 0.5-5.0, a closed system containing an aqueous mixture of chlorine dioxide, iodine, and a species such as malonic acid (MA) or ethyl acetoacetate, which reacts with iodine to produce iodide, shows periodic changes in the light absorbance of I3-. This behavior can be modeled by a simple scheme consisting of three component reactions: (1) the reaction between MA and iodine, which serves as a continuous source of I-; (2) the reaction between ClO2? and I-, which acts as a source of ClO2-; and (3) the self-inhibited reaction of chlorite and iodide that kinetically regulates the system. The fast component reaction between chlorine dioxide and iodide ion was studied by stopped-flow spectrophotometry. The rate law is -[ClO2?]/df = 6 × 103 (M-2 s-1)[ClO2?][I-]. A two-variable model obtained from the empirical rate laws of the three component reactions gives a good description of the dynamics of the system. The oscillatory behavior results not from autocatalysis but from the self-inhibitory character of the chlorite-iodide reaction.
- Lengyel, István,Rábai, Gyula,Epstein, Irving R.
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- Weak acids enhance halogen activation on atmospheric waters surfaces
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We report that rates of I2(g) emissions, measured via cavity ring-down spectroscopy, during the heterogeneous ozonation of interfacial iodide: I-(surface, s) + O3(g) + H+(s) →→ I2(g), are enhanced several-fold, whereas those of IO · (g) are unaffected, by the presence of undissociated alkanoic acids on water. The amphiphilic weak carboxylic acids appear to promote I2(g) emissions by supplying the requisite interfacial protons H+(s) more efficiently than water itself, at pH values representative of submicrometer marine aerosol particles. We infer that the organic acids coating aerosol particles ejected from oceans topmost films should enhance I2(g) production in marine boundary layers.
- Hayase, Sayaka,Yabushita, Akihiro,Kawasaki, Masahiro,Enami, Shinichi,Hoffmann, Michael R.,Colussi, Agustin J.
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- Spontaneous Formation of Cellular Chemical System that Sustains Itself far from Thermodynamic Equilibrium
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We report the observation of the spontaneous formation of a cellular structure in a simple inorganic system. The system is obtained by immersing a pellet of calcium and copper chlorides in an alkali solution containing sodium carbonate, sodium iodide, and hydrogen peroxide. The system produces a cell surrounded by a semipermeable membrane. Reactants diffuse and react inside the cell with copper ions serving as catalyst. The products diffuse out of the cell. The system sustains itself far from thermodynamic equilibrium.
- Maselko, Jerzy,Strizhak, Peter
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- resonance enhanced multiphoton ionization of I and Br formed from the infrared multiphoton decomposition of CF3I and CF3Br
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Resonance enhanced multiphoton ionization (REMPI) has been used to study the products of the infrared multiphoton decomposition (IRMPD) of CF3I in a very low-pressure photolysis (VLPΦ) cell.The strongest REMPI signals are due to the ground state I(2P3/2) and the spin-orbit excited state I*(2P1/2).The origins of I and I* were determined from the time and IR laser fluence dependences of the REMPI signal.I* is formed by visible single photon dissociation of vibrationally excited CF3I and by visible multiphoton dissociation of I2 and thermal CF3I.The ionization efhciency of I has been determined relative to NH3 for our probe laser conditions, and the sticking coefhcient of I with gold surfaces has been determined.The REMPI spectra of the products of the IRMPD of CF3Br is also presented.
- Robertson, Robert M.,Golden, David M.,Rossi, Michel J.
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- Synthesis, structural and magnetic characterizations of a dinuclear copper(II) complex with an (N,S,O) donor ligand: Catecholase and phenoxazinone synthase activities
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A new dinuclear Cu(II) complex (1) was synthesized and crystallographically characterized. Each of the Cu(II) centres has penta coordination and been found to adopt square pyramidal geometry. Variable temperature magnetic measurements showed that there is weak ferromagnetic interaction between the Cu(II) centres in 1. 1 shows catecholase as well as phenoxazinone synthase activities in different solvents. The turn over numbers for the catecholase activity were 4.02 × 103 h?1 (MeOH) and 9.57 × 103 h?1 (MeCN), and that of phenoxazinone synthase activity were 1.065 × 103 h?1 (MeOH), 2.13 × 102 h?1 (MeCN) and 2.844 × 103 h?1 (DCM).
- Ghosh, Ayon Kanti,Ali, Anzar,Singh, Yogesh,Purohit, Chandra Shekhar,Ghosh, Rajarshi
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p. 156 - 163
(2018/02/20)
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- Molecular Thorium Compounds with Dichalcogenide Ligands: Synthesis, Structure, 77Se NMR Study, and Thermolysis
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A series of dimeric thorium disulfides and diselenides have been prepared with sterically undemanding ancillary ligands. Five complexes, (py)6Th2I4(μ2-S2)2, (py)6Th2Br2(SC6F5)2(μ2-S2)2, (py)6Th2I4(μ2-Se2)2, (py)6Th2I2(SC6F5)2(μ2-Se2)2, and (py)6Th2Br2(SC6F5)2(μ2-Se2)2, were isolated in high yields by first reducing mixtures of I2, F5C6SSC6F5, PhSeSePh, or PhSSPh, and PhSeBr with elemental Th, followed by in situ ligand-based redox reactions with elemental sulfur or selenium. These are the first examples of thorium compounds with bridging dichalcogenide ligands. Attempts to prepare chloride derivatives gave mixtures of (py)4ThCl4 and either (py)6Th2Cl2(SC6F5)2(μ2-S2)2 or (py)8Th4Se4(SePh)4(SC6F5)4. All products were characterized by single-crystal and powder X-ray diffraction and IR, UV-visible, and NMR spectroscopy. A computational analysis of experimental 77Se NMR chemical shifts reveals that the solvated dimeric structures with two bridging dichalcogenides are maintained in solution. Thermolysis of (py)6Th2I4(μ2-Se2)2 leads to reduction of the bridging Se22- moieties, oxidation of the I- ligand, and formation of solid-state ThSe2 and I2.
- Wu, Wen,Rehe, David,Hrobárik, Peter,Kornienko, Anna Y.,Emge, Thomas J.,Brennan, John G.
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p. 14821 - 14833
(2018/12/13)
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- Compatible Mechanism for a Simultaneous Description of the Roebuck, Dushman, and Iodate-Arsenous Acid Reactions in an Acidic Medium
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The iodine-arsenous acid (Roebuck), iodide-iodate (Dushman), and iodate-arsenous acid reactions have been studied simultaneously by a stopped-flow technique by monitoring the absorbance-time profiles at the isosbestic point of the I2/I3- system (468 nm). Using the well-accepted rate coefficients of iodine hydrolysis, we have proven that iodine is the kinetically active species of the iodine-arsenous acid reaction. Strong iodide inhibition of this system is explained by a rapidly established equilibrium between iodine and arsenous acid to produce an iodide ion, a hydrogen ion, and a short-lived intermediate H2AsO3I, which is shifted far to the left. Taking into consideration the generally accepted kinetic model of the Dushman reaction where I2O2 plays a key role to account for all of the most important observations in this subsystem and a sequence of simple formal oxygen-transfer reactions between arsenous acid and iodic acid as well as iodous acid and hypoiodous acid, we propose a 13-step comprehensive kinetic model, including seven rapidly established equilibria with only six fitted parameters, that is able to explain all of the most important characteristics of the kinetic curves of all of the title systems both individually and simultaneously.
- Valkai, László,Horváth, Attila K.
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p. 1595 - 1603
(2016/02/27)
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- Facile synthesis of a rare example of an iron(III) iodide complex, [FeI3(AsMe3)2], from the reaction of Me 3AsI2 with unactivated iron powder
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The reaction of Me3AsI2 with unactivated iron powder provides a synthetic entry into the coordination chemistry of iron(III) iodide, which is inaccessible by traditional routes due to the low stability of the parent halide FeI3. The reaction of iron powder with Me 3AsI2 results in the formation of a trigonal bipyramidal complex, [FeI3(AsMe3)2], which features the iodide ligands in the equatorial positions, and the Me3As groups occupying the axial positions. This complex is a rare example of an iron(III) iodide complex, and is the first iron(III) complex of a monodentate tertiary arsine ligand. The preparation of [FeI3(AsMe3) 2] via the direct oxidation of iron powder further demonstrates that complexes of soft donor ligands can be prepared with hard transition metal centres, such as iron(III), in direct contravention of the HSAB principle. The structure of [FeI3(AsMe 3)2] is isomorphous with all previously reported [MX 3(EMe3)2] (M = main group or transition metal, X = halide, E = N, P, As) trigonal bipyramidal structures.
- Barnes, Nicholas A.,Godfrey, Stephen M.,Ho, Nicholas,McAuliffe, Charles A.,Pritchard, Robin G.
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- CONTINUOUS PROCESS FOR CONVERTING NATURAL GAS TO LIQUID HYDROCARBONS
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A method comprising: providing a first halogen stream; providing a first alkane stream; reacting at least a portion of the first halogen stream with at least a portion of the first alkane stream in a first reaction vessel to form a first halogenated stream; providing a second alkane stream comprising C2 and higher hydrocarbons; providing a second halogen stream; and reacting at least a portion of the second halogen stream with at least a portion of the second alkane stream in a second reaction vessel to form a second halogenated stream.
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Page/Page column 78
(2010/04/03)
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- Organosulfur oxoacids. Part 2. A novel dimethylthiourea metabolite - Synthesis and characterization of the surprisingly stable and inert dimethylaminoiminomethane sulfonic acid
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A new metabolite of the biologically active thiocarbamide dimethylthiourea (DMTU) has been synthesized and characterized. DMTU's metabolic activation in the physiological environment is expected to be dominated by S-oxygenation, which produces, successively, the sulfenic, sulfinic, and sulfonic acids before forming sulfate and dimethylurea. Only the sulfinic and sulfonic acids are stable enough to be isolated. This manuscript reports on the first synthesis, isolation, and characterization of the sulfonic acid: dimethylaminoiminomethanesulfonic acid (DMAIMSOA). It crystallizes in the orthorhombic Pbca space group and exists as a zwitterion in its solid crystal form. The negative charge is delocalized over the sulfonic acid oxygens and the positive charge is concentrated over the planar N-C-N framework rather than strictly on the sp2-hybridized cationic carbon center. As opposed to its sulfinic acid analogue, DMAIMSOA is extremely inert in acidic environments and can maintain its titer for weeks at pH 6 and below. It is, however, reasonably reactive at physiological pH conditions and can be oxidized to dimethylurea and sulfate by mild oxidants such as aqueous iodine.
- Petersen, Jeffrey L.,Otoikhian, Adenike A.,Morakinyo, Moshood K.,Simoyi, Reuben H.
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p. 1247 - 1255
(2011/02/24)
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- Kinetics of oxidation of iodide by vanadium (V): Catalysis by the water pools of CTAB reverse micelles
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The kinetic study of the oxidation of iodide ion by V(V) has been carried out in the water pools of cetyl trimethyl ammonium bromide(CTAB) reverse micelles in a mixture of chloroform-hexane (3 : 2). The study of the effect of concentration of V(V) and I- on rate show that the reaction obeys first order kinetics with each of the reactants. A plot of k′ (pseudo first order rate constant) versus [H+] is linear with a positive intercept at constant concentrations of iodide and bromide. The rate of the reaction is markedly increased in the reverse micellar medium compared to conventional aqueous medium under identical conditions. The pronounced acceleration in reverse micelles has been accounted for by the concentration effect in the water pool which have an effect on kinetics.
- Shyamala,Subba Rao
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p. 207 - 210
(2010/09/04)
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- Novel and highly effective method for the trimethylsilylation of alcohols and phenols with hexamethyldisilazane (HMDS), catalyzed by I2 generated in situ using Fe(NO3)3 · 9 H 2O/NaI under heterogeneous and neutral conditions
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Structurally diverse alcohols and phenols were trimethylsilylated in a clean and efficient reaction with hexamethyldisilazane (HMDS) based on the use of I2 generated in situ from Fe(NO3)3 · 9 H2O/NaI. The reaction occurs very rapid in good-to-high yield in CH2Cl2 at room temperature, and the use of toxic and corrosive molecular I2 is avoided.
- Khazaei, Ardeshir,Rahmati, Sadegh,Rostami, Amin
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p. 1434 - 1438
(2009/10/16)
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- Oxyhalogen-sulfur chemistry - Kinetics and mechanism of oxidation of methionine by aqueous iodine and acidified iodate
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The oxidation of methionine (Met) by acidic iodate and aqueous iodine was studied. Though the reaction is a simple two-electron oxidation to give methionine sulfoxide (Met-S=O), the dynamics of the reaction are, however, very complex, characterized by clock reaction characteristics and transient formation of iodine. In excess methionine conditions, the stoichiometry of the reaction was deduced to be IO3- + 3Met → I- + 3Met-S=O. In excess iodate, the iodide product reacts with iodate to give a final product of molecular iodine and a 2:5 stoichiometry: 2IO3 - + 5Met + 2H+ → I2 + 5Met-S=O + H 2O. The direct reaction of iodine and methionine is slow and mildly autoinhibitory, which explains the transient formation of iodine, even in conditions of excess methionine in which iodine is not a final product. The whole reaction scheme could be simulated by a simple network of 11 reactions.
- Chikwana, Edward,Davis, Bradley,Morakinyo, Moshood K.,Simoyi, Reuben H.
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p. 689 - 697
(2009/12/04)
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- Mechanism of enhancement of sonochemical-reaction efficiency by pulsed ultrasound
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The enhancement of sonochemical-reaction efficiency by pulsed ultrasound at 152 kHz has been studied experimentally through absorbance measurements of triiodide ions from sonochemical oxidation of potassium iodide at different liquid volumes to determine
- Tuziuti, Toru,Yasui, Kyuichi,Lee, Judy,Kozuka, Teruyuki,Towata, Atsuya,Iida, Yasuo
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p. 4875 - 4878
(2009/03/11)
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- Generation of atomic iodine via fluorine for chemical oxygen-iodine laser
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A method of the chemical generation of atomic iodine for a chemical oxygen-iodine laser (COIL) using atomic fluorine as a reaction intermediate was studied experimentally. This method is based on the reaction between F2 and NO providing F atoms, and the reaction of F with HI resulting in iodine atoms generation. Atomic iodine was produced with efficiency exceeding 40% relative to initial F2 flow rate. This efficiency was nearly independent on pressure and total gas flow rate. The F atoms were stable in the reactor up to 2 ms. An optimum ratio of the reactants flow rates was F2:NO:HI = 1:1:1. A rate constant of the reaction of F2 with HI was determined. The numerical modelling showed that remaining HI and IF were probably consumed in their mutual reaction. The reaction system was found suitable for employing in a generator of atomic iodine with its subsequent injection into a supersonic nozzle of a COIL.
- Jirásek, Vít,?palek, Otomar,?ensky, Miroslav,Picková, Irena,Kodymová, Jarmila,Jakubec, Ivo
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p. 167 - 174
(2008/10/09)
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- Semiconductor-catalyzed solar photooxidation of iodide ion
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With natural sunlight TiO2 (anatase), ZrO2, MoO3, Fe2O3, ZnO, CeO2 and Al2O3 microparticles photocatalyze the oxidation of iodide ion but CuO, ZnS, CdO, CdS, HgO, PbO,
- Karunakaran,Anilkumar
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p. 153 - 158
(2008/10/09)
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- Freezing halide ion solutions and the release of interhalogens to the atmosphere
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The effect of freezing on a variety of acidified and neutral, nitrite ion and halide-containing mixtures has been investigated using UV/vis spectroscopy. Several trihalide ions were formed and monitored, including I2Cl -, I2Br-, ICI2- and IBr2-. A mechanism to explain the observations is given in terms of steps involving INO and the nitroacidium ion, [H2ONO] +. The transformation of sea salt components to specific trihalide ions by freezing represents a potentially important process in a polar atmospheric context. This is because the dichloro- and dibromo-trihalide ions can release chlorine- and bromine-containing gases, which are key intermediates in ozone destruction.
- O'Driscoll, Paul,Lang, Kathrin,Minogue, Nicholas,Sodeau, John
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p. 4615 - 4618
(2008/10/09)
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- Heterogeneous reactions of HX + HONO and I2 on ice surfaces: Kinetics and linear correlations
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Reaction probabilities of gaseous nitrous acid, HONO, with HCl, HBr, and HI treated ice surfaces have been investigated in a fast flow-tube reactor coupled with a differentially pumped quadrupole mass spectrometer (QMS) at 191 K. The reaction probability increases with the HX surface coverage, and the rate is the highest for the HONO reaction on the Hi-treated ice surface. Relative rate constants are correlated to the nucleophilic parameter, according to the linear free-energy relationship for this series of heterogeneous reactions on ice surfaces. The correlation was also extended to HOCl + HX(ad) reactions on the ice surface, and it can be used to treat other heterogeneous atmospheric and catalytic reactions. The reaction products ClNO and BrNO were determined by the QMS. INO was found to rapidly convert to I2 on surfaces, and I2 was observed from the reaction of HONO + HI. The uptake coefficient of I2 on the HI-treated ice surface is higher than that for I2 on the water-ice surface.
- Diao, Guowang,Chu, Liang T.
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p. 1364 - 1373
(2007/10/03)
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- METHOD OF PROCESSING OF HYDROGEN FOR REDUCTIVE ACYLATION OF NITRO, AZIDO AND CYANO ARENES
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The present invention relates to a method for processing of hydrogen for the reductive acylation of nitro, azido and cyano arenes. More particularly, this invention relates to an improved process for the preparation of amides and anilides using C3-C7 carboxylic acids as proton source/acylating agents employing Fe3+-montmorillonite as a catalyst.
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- Method of processing of hydrogen for reductive acylation of nitro, azido and cyano arenes
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A method for processing of hydrogen for the reductive acylation of nitro, azido and cyano arenes is disclosed. More particularly, improved process for the preparation of amides and anilides using C3-C7carboxylic acids as proton source/acylating agents employing Fe3+-montmorillonite as a catalyst is disclosed.
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Page column 4
(2008/06/13)
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- Two- and three-body photodissociation of gas phase I3 -
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The photodissociation dynamics of gas phase I-3 by using a fast beam photofragment translational spectrometer was examined. It was stated that the photofragment translational spectrometer was coupled to a coincidence imaging detector that enabled the direct detection and analysis of two and three neutron or anion fragments from single dissociation events. The three-body dissociation yielding I-+2I(2P3/2) photofragments was also seen throughout the energy range probed. Analysis shows that the three-body decay dynamics was dominated by synchronous concerted dissociation.
- Hoops, Alexandra A.,Gascooke, Jason R.,Faulhaber, Ann Elise,Kautzman, Kathryn E.,Neumark, Daniel M.
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p. 7901 - 7909
(2007/10/03)
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- Method and composition for the generation of chlorine dioxide using Iodo-Compounds, and methods of use
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The present invention relates to a biocidal composition, designed for the generation of chlorine dioxide, comprising at least one iodo-compound having at least one iodine atom and a source of chlorite ions. The molar ration of chlorite ions to iodine atoms is 2 or greater. The composition finds use in a variety of applications including methods of cleaning, sanitizing, deodorizing, and disinfecting various surfaces.
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Page column 17-21
(2008/06/13)
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- Spectrofluorimetric determination of both hydrogen peroxide and -O-O-H in polyethylene glycols (PEGs) using 2-hydroxy-1-naphthaldehyde thiosemicarbazon (HNT) as the substrate for horseradish peroxidase (HRP)
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2-Hydroxy-1-naphthaldehyde thiosemicarbazon (HNT) had been synthesized and used as a new kind of substrate for horseradish peroxidase (HRP) in spectrofluorimetric determination of hydrogen peroxide (H2O 2). The oxidation reaction of HNT with H2O2 under the catalysis of HRP was studied in detail. The possible reaction mechanism was discussed. Under optimum experimental conditions, the oxidized product of HNT had excitation and emission maxima at 260 and 450 nm, respectively. The linear range of this method was 1.30 × 10-9 -1.25 × 10-5 mol 1-1 with a detection limit of 3.89 × 10-10 mol 1-1. The effect of interferences, surfactants and organic solvents on the determination of H2O 2 had been investigated. A study to prove the existence of -O-O-H in PEGs was carried out. The proposed method was successfully applied to the determination of -O-O-H in polyethylene glycols.
- Tang, Bo,Wang, Yan
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p. 2867 - 2874
(2008/10/08)
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- Inhibitors of IMPDH enzyme
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The present invention relates to a novel class of compounds which are IMPDH inhibitors. This invention also relates to pharmaceutical compositions comprising these compounds. The compounds and pharmaceutical compositions of this invention are particularly well suited for inhibiting IMPDH enzyme activity and consequently, may be advantageously used as therapeutic agents for IMPDH mediated processes. This invention also relates to methods for inhibiting the activity of IMPDH using the compounds of this invention and related compounds.
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Page column 30
(2010/02/04)
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- Formation of Pd2X2(μ-S)(μ-dpm)2 by reaction of PdX2(dpm) with H2S in the presence of alumina (X = halogen, dpm - diphenylphosphinomethane)
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Alumina promotes the reaction of PdX2(dpm) (3) (X = Cl, Br, I) with H2S to form Pd2X2(μ-S)(dpm)2 (2) and HX, with chemisorption of the HX (quantified by titration) providing the driving force; althoug
- Wong, Terrance Y.H.,James, Brian R.,Wong, Philip C.,Mitchell, Keith A.R.
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p. 159 - 169
(2008/10/09)
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- Kinetics of the molybdate and tungstate catalyzed oxidation of iodide by hydrogen peroxide
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Several studies of the Mo(VI) and W(VI) catalyzed reaction of H2O2 with various substrates have been documented previously. The experiments described herein attempt to settle some apparent contradictions in these reports. Specificall
- Copper, Christine L.,Koubek, Edward
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p. 229 - 232
(2008/10/08)
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- The Effect of Iron(III) Sulfate on the Interaction of Hydrogen Peroxide with Potassium Iodide in Solution
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Iron(III) sulfate is shown to accelerate iodide oxidation by hydrogen peroxide in aqueous solution.
- Danilov,Krasnobaeva,Nosova,Fedulov,Georgievskaya
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p. 660 - 661
(2008/10/08)
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- Kinetics and Mechanism of the Copper(II)-Catalyzed Oxidation of the Iodide Ion by Chromate(VI) Ion in an Aqueous Solution
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Although the chromate(VI) ions, CrO42- and HCrO4- , which are described as CrVI herein, could hardly oxidize the iodide ion to iodine above pH 3.0, it was catalytically oxidized by adding traces of copper(II) ion. When a copper(II) solution of 10-7-10-5 mol dm-3 was mixed with an iodide solution, after a fast formation of iodine, the iodine concentration remained constant. After such an iodine formation had occurred, if a chromate solution was added into the reacting mixture, the iodine began to form again in accordance with a rate law of 2/3(d[I2]/dt)= -d[CrVI]/dt=k[CuI][CuvI], in which [CuI] is the steady-state concentration in the chain cycle CuI+/CuI. The rate of the chain reaction was independent of the time to add chromate, and the formation of iodine I2 (or triiodide ion I3-) stopped at the time when all of the chromate was consumed by the chain reaction. The stoichiometry was 3I- +CrVI→1.5I2+CrIII. The iodine formation was extremely inhibited by the presence of either radical scavengers or complex-forming reagents as well as by increasing pH. Although addition of alcohols to the reaction mixture extremely accelerated the iodine formation before adding chromate, it hardly affected on this process after the addition of chromate. The reaction mechanisms are presented in order to account for the observed results.
- Kimura, Masaru,Ikawa, Rie,Shiota, Yuko,Tsukahara, Keiichi
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p. 893 - 897
(2007/10/03)
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- Synthesis, properties, and structure of LiAuI4 and KAuI4 with a discussion of the crystal chemical relationship between the halogenoaurates RbAuCl4, AgAuCl4, RbAuBr4 and LiAuI4
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The alkalimetal iodo aurates(III) MAuI4 (M = Li, K) are obtained in form of single crystals from MI, Au and I2 in a sealed glass ampoule by heating to 550°C and slow cooling to 300°C. KAuI4 crystallizes in the monoclinic space group P21/c with a = 968.6(4); b = 704.5(2), c = 1393.2(7) pm; β = 100.95(2)° and Z = 4. The crystal structure is built up from square planar AuI4- anions and K+ cations. The cations are coordinated by eight I atoms of neighbouring AuI4- anions with distances K-I between 350.0 and 369.6 pm. At 100°C KAuI4 is reduced to form K3Au3I8, which at 180°C decomposes to KI, Au and I2. LiAuI4 forms black, moisture sensitive needles, decomposing in the absence of iodine at 20°C to LiI, Au and I2. It crystallizes in a variant of the RbAuBr4 type structure with the space group P21/a and a = 1511.7(4); b = 433.9(4); c = 710.0(2) pm; β = 121.50(2)°; Z = 2. The crystal chemical relationship between the structures of RbAuCl4, RbAuBr4, AgAuCl4 and LiAuI4 is discussed.
- Lang, E. Schulz,Abram,Str?hle
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p. 1791 - 1795
(2008/10/09)
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- Kinetics and Mechanisms of the Copper(II)-Catalyzed Oxidation of Iodide Ion in the Presence of Molecular Oxygen in Aqueous Acid Media
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Traces of copper(II) ions in 10-7 - 10-5 M (M=mol dm-3) catalytically accelerated the oxidation reactions of iodide ion to iodine in relatively strong acid solutions (pH2) in the presence of molecular oxygen under conditions containing relatively high concentrations of I-.When a copper(II) solution was mixed with an iodide solution, after a rapid formation of iodine, it gradually increased according to the reaction times.For about 5 min after mixing, plots of ->formed vs. t showed a good straight line; the formation rate of I2 (or I3-) increased proportionally with increasing concentrations of copper(II) ion and oxygen, with increasing concentrations of hydrogen ion and iodide ion, and with increasing temperature and with decreasing the ionic strength in the reaction solution.The formation rate of I2 was extremely inhibited by the presence of either radical scavengers or ethylenediaminetetraacetic acid (EDTA).A chain mechanism is presented to account for the obtained results.
- Kimura, Masaru,Tokuda, Mari,Tsukahara, Keiichi
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p. 2731 - 2735
(2007/10/02)
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- The Role of Adsorption of Iodine on the Reactor Wall in Photoinduced Nonequilibrium Phase Transition in the Briggs-Rausher Reaction
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The lengths of the induction periods for the photoinduced nonequilibrium (I) -> (II) phase transition in the Briggs-Rausher reaction were measured both in a well-stirred reactor and in artificially created unstirred regions of the reactor.In the absence of stirring, the new phase, (II), is generated irregularly at a random point in the bulk and is not initiated by the reactor walls.The magnitude of iodine adsorption from an aqueous solution on a glass surface was experimentally determined.The experimental results preclude the earlier assumption that in the nonequilibrium (I) -> (II) phase transition iodine adsorption on the reactor walls is the primary cause of the stirring effects.
- Melikhov, D. P.,Vanag, V. K.
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p. 1019 - 1022
(2007/10/02)
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- Destructive or cooperative attack of iodide anions on alkyltriiodophospbonium cations: Elimination of iodine in solution and layer structures in the solid state
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Solid-state and solution 31P NMR shifts of t-BuPI4 and crystal structure determinations of t-BuPI4, i-PrPI4, and MePI4 reveal that alkyltetraiodophosphorus compounds RPI4 (R = t-Bu (1), i-Pr (2), Me3SiCH2 (3), Me (4)) in the solid state involve μ3-bridging I?I interactions between RPI3+ cations and I- anions (leading to the formation of layer structures (2,4) or a 3-dimensional network (1)) whereas, in CS2CD2Cl2 solutions, deiodination by nucleophilic I- anions causes all RPI4 compounds and PI5 to decompose into the iodophosphanes RPI2 or PI3 and molecular iodine. 1 crystallizes in the cubic space group I213, with a = 13.613(2) A?, V = 2522.7(6) A?3, and Z = 8. 2 crystallizes in the monoclinic space group P21/c, with a = 6.686(2) A?, b = 19.918(5) A?, c = 8.961(3) A?, β = 97.41(2)°, V = 1183.4(6) A?3, and Z = 4. 4 crystallizes in the orthorhombic space group Pbcm, with a = 6.031 (2) A?, b = 18.426(7) A?, c = 8.741(5) A?, V = 971.4(3) A?3, and Z = 4. Cation-anion I?I interactions of solid RPI4 are stronger than molecule-ion interactions within the related anion network of solid PhCH2NMe3+HCl4- (5), which crystallizes in the monoclinic space group P21/c, with a = 8.200(1) A?, b = 13.723(1) A?, c = 16.216(1) A?, β = 91.32(2)°, V = 1824.3(3) A?3, and Z = 4.
- Du Mont, Wolf-Walther,Stenzel, Volkmar,Jeske, J?rg,Jones, Peter G.,Sebald, Angelika,Pohl, Siegfried,Saak, Wolfgang,B?tcher, Michael
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p. 1502 - 1505
(2008/10/08)
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- A pulse radiolysis study of the reaction of OH with I2 and the decay of I2-
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The rate constant for the reaction of the hydroxyl radical with iodine was estimated to be (9.5 +/- 1.0) * 10-9 dm3 mol-1 s-1 at 20 deg C from fitting the time dependence of the decrease in the absorption of iodine at 460 nm.A number of rate constants associated with the decay of I2- that were required for this fitting process were also determined.They were the reaction of I2- with I2- (2k = (4.60 +/- 0.05) * 10-9 dm3 mol-1 s-1) at an ionic strength of 1.2 * 10-2 mol dm-3; I2- with I (k = 4.6 +/- 1.6) * 10-9 dm3 mol-1 s-1); and I with I (2k = (3.0 +/- 1.0) * 10-10 dm3 mol-1 s-1).
- Elliot, A. John
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p. 1658 - 1661
(2007/10/02)
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- A SIMPLE METHOD TO LOCATE TRANSITION STATES OF CHEMICAL REACTIONS
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By using an appropriate coordinate system the arc length between two points on the geodesic reaction path is equal to the absolute difference between the function values (energies) belonging to the same points.This gives the possibility to avoid the tedious integration procedure necessary to get a measure of the position of the saddle point (or any other point) in the one-dimensional space of the reaction path.The method is illustrated by reaction coordinate values of transition states for a number of atom transfer reactions in comparison with those calculated by an independent method.Reaction coordinates also computed by using analytical functions are compared with those obtained by direct integration.
- Balint, Imre,Ban, Miklos I.
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p. 431 - 438
(2007/10/02)
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- Large Amplitude pH Oscillation in the Oxidation of Hydroxylamine by Iodate in a Continuous-Flow Stirred Tank Reactor
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Large amplitude pH oscillation occurs in the iodate oxidation of hydroxylamine in a continuous-flow tank reactor (CSTR) in a narrow range of flow rates and input concentrations.In addition to pH, the redox potential, the iodide ion concentration, the rate of gas (N2O) formation, and the color of the solution (I2) change periodically.The oscillatory period is extremely long, 2-6 h.The dynamical behaviour of the reaction was modeled by a scheme that takes into account the following component processes: the protonation equilibrium of NH2OH, the dissociation of water,the direct redox reaction between IO3- and NH3OH+, the Dushman reaction between IO3- and I-, the autoinhibitory reaction between I2 and NH3OH+, the fast dimerization of NOH to N2O, the reaction of NOH with NH2OH, and the volatility of iodine.Empirical rate laws of the component reactions were used successfully to calculate the kinetic behaviour in a closed system, as well as in the CSTR.
- Rabai, Gyula,Epstein, Irving R.
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p. 6361 - 6365
(2007/10/02)
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- Complex Dynamical Behavior in the Oxidation of Thiocyanate by Iodate
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Complex dynamical behavior including oligooscillation (multiple extrema in concentration as a function of time) has been observed in the oxidation of thiocyanate in acidic medium.The stoichiometry of the reaction when thiocyanate is in stoichiometric excess over iodate is IO3- + SCN- + H2O SO42- + CN- + I- + 2H+.In excess iodate the stoichiometry is 7IO3- + 5SCN- + 2H+ I2 + 5ICN + 5SO42- + H2O.In high acidic concentrations the reaction initially produces iodine, and then later the iodine is consumed.In excess thiocyanate all the iodine produced is subsequently consumed, while in excess iodate some iodine is left at the end of the reaction.This behavior is explained via a network of nine reactions which are viable in acidic mixtures of iodate and thiocyanate.
- Simoyi, Reuben H.,Epstein, Irving R.,Kustin, Kenneth
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p. 1689 - 1691
(2007/10/02)
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- Oxidation of Hydroxylamine by Periodate in a Continuous-Flow Stirred Tank Reactor: A New pH Oscillator
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The periodate oxidation of hydroxylamine exhibits a complex and variable stoichiometry at pH 5.There are two limiting cases.In excess periodate the products are nitrate and iodate, while in a large excess of hydroxylamine IO4- is reduced to I-, and the nitrogen-containing product is N2O.The formation of nitrite ion and iodine is important when neither of the reactants is present in large excess.The reaction shows clock type kinetics in closed conditions if no buffer is present.In a flow reactor sustained oscillations in +>, in color, and in redox potential are found experimentally in a narrow range of flow rate and input concentrations.A simple model is proposed to explain the oscillation.
- Rabai, Gyula,Epstein, Irving R.
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p. 7556 - 7559
(2007/10/02)
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- PHOTOCATALYTIC OXIDATION OF IODIDE IONS BY TITANIUM DIOXIDE
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The photocatalytic oxidation of aqueous I(-), usually as neutral 0.1 mol kg-1 KI, has been investigated using suspensions of pure anatase and rutile, five doped rutiles and two commercial anatase pigments.Reaction only proceeded in the presence of both O2 and u.v. radiation to yield I2, which reacted with excess I(-) to form I(-)3; there was no evidence for IO(-) or IO(-)3 formation.The dependence of initial reaction rate on the square root of the intensity of the incident 366 nm radiation, together with low quantum yields, reflect the recombinative loss of photoelectrons and photoholes greatly exceeding their consumption in productive reaction steps.No activation energy for I2 formation was observed with any of the catalysts, and in this respect the photo-oxidation of I(-) differs from that of liquid alcohols on the identical catalysts.A mechanism is proposed in which I2 and OH(-) result from electron transfer between charged and neutral species adsorbed on the TiO2 surface, leading to an overall reaction: .
- Harvey, Paul R.,Rudham, Robert
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p. 4181 - 4190
(2007/10/02)
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