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In Situ Observation of Surface Species on Iridium Oxide Nanoparticles during the Oxygen Evolution Reaction 下载免费PDF全文
Hernan G. Sanchez Casalongue Dr. May Ling Ng Dr. Sarp Kaya Dr. Daniel Friebel Dr. Hirohito Ogasawara Dr. Anders Nilsson 《Angewandte Chemie (International ed. in English)》2014,53(28):7169-7172
An iridium oxide nanoparticle electrocatalyst under oxygen evolution reaction conditions was probed in situ by ambient‐pressure X‐ray photoelectron spectroscopy. Under OER conditions, iridium undergoes a change in oxidation state from IrIV to IrV that takes place predominantly at the surface of the catalyst. The chemical change in iridium is coupled to a decrease in surface hydroxide, providing experimental evidence which strongly suggests that the oxygen evolution reaction on iridium oxide occurs through an OOH‐mediated deprotonation mechanism. 相似文献
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Olson JP Gichinga MG Butala E Navarro HA Gilmour BP Carroll FI 《Organic & biomolecular chemistry》2011,9(11):4276-4286
In previous studies we showed that 3-(substituted phenylethynyl)-5-methyl[1,2,4]triazine analogues of MPEP were potent antagonists of glutamate-mediated mobilization of internal calcium in an mGluR5 in vitro efficacy assay. In the present study we report the synthesis and evaluation of six 3-(substituted biphenylethynyl)-5-methyl[1,2,4]triazines (5a-f), and five 3-(substituted phenoxyphenylethynyl)-5-methyltriazines (6a-e). Compound 2-(4-fluorophenyl-5-[2-(5-methyl[1,2,4]triazine-3-yl)ethynyl]benzonitrile (5f) with an IC(50) of 28.2 nM was the most potent analogue. 相似文献
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Vânia B. Bueno Iolanda M. Cuccovia Hernan Chaimovich Luiz H. Catalani 《Colloid and polymer science》2009,287(6):705-713
Monomer free hydrogel nanoparticles (nanogels) were prepared by crosslinking preformed poly(N-vinyl-2-pyrrolidone) (PVP) entrapped in the aqueous pool of hexadecyltrimethylammonium bromide reverse micelles using the
Fenton reaction. The PVP nanoparticles were spherical with a dry diameter of 27 nm. The diameter of the swollen particles
was ten times higher, i.e., a swelling ratio, Q, above 900, characterizing this preparation as superabsorbent. PVP nanogel swelling was dependent on bound Fe3+ and varied with pH and ionic strength. Nanogel deswelling by salt followed the anions lyotropic series, i.e., . The value of Q reached 6,000 in iron-free PVP nanoparticles at low pH, making this nanogel one of the most efficient swelling systems so
far described. 相似文献
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This paper addresses a multi-period production/inventory problem with two suppliers, where demand sizes and supplier lead time are stochastic and correlated. A discrete time, single item inventory system is considered, where inventory levels are reviewed periodically and managed using a base-stock policy. At the end of each period, a replenishment order is placed, which enters a queue at the buffer stage and is consequently forwarded to the first available supplier. We present a mathematical model of this inventory system and determine optimal safety stock levels for it, in closed form, using matrix analytic techniques and the properties of phase type distributions. To account for the effect of order crossovers, which occur whenever replenishment orders do not arrive in the sequence in which they were placed, the inventory shortfall distribution is analyzed. Finally, a set of numerical experiments with a system with two suppliers is presented, where the proposed model is compared to other existing models. 相似文献
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A spray flamelet/progress variable approach is developed for use in spray combustion with partly pre-vaporised liquid fuel, where a laminar spray flamelet library accounts for evaporation within the laminar flame structures. For this purpose, the standard spray flamelet formulation for pure evaporating liquid fuel and oxidiser is extended by a chemical reaction progress variable in both the turbulent spray flame model and the laminar spray flame structures, in order to account for the effect of pre-vaporised liquid fuel for instance through use of a pilot flame. This new approach is combined with a transported joint probability density function (PDF) method for the simulation of a turbulent piloted ethanol/air spray flame, and the extension requires the formulation of a joint three-variate PDF depending on the gas phase mixture fraction, the chemical reaction progress variable, and gas enthalpy. The molecular mixing is modelled with the extended interaction-by-exchange-with-the-mean (IEM) model, where source terms account for spray evaporation and heat exchange due to evaporation as well as the chemical reaction rate for the chemical reaction progress variable. This is the first formulation using a spray flamelet model considering both evaporation and partly pre-vaporised liquid fuel within the laminar spray flamelets. Results with this new formulation show good agreement with the experimental data provided by A.R. Masri, Sydney, Australia. The analysis of the Lagrangian statistics of the gas temperature and the OH mass fraction indicates that partially premixed combustion prevails near the nozzle exit of the spray, whereas further downstream, the non-premixed flame is promoted towards the inner rich-side of the spray jet since the pilot flame heats up the premixed inner spray zone. In summary, the simulation with the new formulation considering the reaction progress variable shows good performance, greatly improving the standard formulation, and it provides new insight into the local structure of this complex spray flame. 相似文献
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Hernan R. Costabal Gary D. Withnell James C. Glass George Graf 《Physics letters. A》1982,88(8):432-434
The gamma-gamma perturbed angular correlation technique has been used to measure the relative motion of lipid molecules in synthetic phospholipid bilayers perfused with the anesthetic gas nitrous oxide. Time-integrated anisotropies for 111In, attached to the lipid headgroups, were determined above and below the order-fluid transition temperature. Compared to results with the pure bilayer, the data showed a three-fold decrease above and a four-fold decrease below the phase transition, suggesting a more ordered state of the membrane in the presence of the anesthetic. 相似文献
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Duarte P Ferreira DP Ferreira Machado I Vieira Ferreira LF Rodríguez HB San Román E 《Molecules (Basel, Switzerland)》2012,17(2):1602-1616
The photophysical behaviour of phloxine B adsorbed onto microcrystalline cellulose was evaluated by reflectance spectroscopy and laser induced time-resolved luminescence in the picosecond-nanosecond and microsecond-millisecond ranges. Analysis of the absorption spectral changes with concentration points to a small tendency of the dye to aggregate in the range of concentrations under study. Prompt fluorescence, phosphorescence and delayed fluorescence spectral decays were measured at room temperature and 77 K, without the need of sample degassing because cellulose protects triplet states from oxygen quenching. In all cases, spectral changes with time and lifetime distribution analysis were consistent with the dye coexisting in two different environments: dyes tightly entrapped between polymer chains in crystalline regions of cellulose showed longer fluorescence and phosphorescence lifetimes and more energetic triplet states, while dyes adsorbed in more amorphous regions of the support showed shorter lifetimes and less energetic triplet states. This behaviour is discussed in terms of the different dye-support interactions in both kinds of adsorption sites. 相似文献
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Maximiano FA Chaimovich H Cuccovia IM 《Langmuir : the ACS journal of surfaces and colloids》2006,22(19):8050-8055
The rate of decarboxylation of 6-nitrobenzisoxazole-3-carboxylate, NBOC, was determined in micelles of N-hexadecyl-N,N,N-trimethylammonium bromide or chloride (CTAB or CTAC), N-hexadecyl-N,N-dimethyl-3-ammonium-1-propanesulfonate (HPS), N-dodecyl-N,N-dimethyl-3-ammonium-1-propanesulfonate (DPS), N-dodecyl-N,N,N-trimethylammonium bromide (DTAB), hexadecylphosphocholine (HPC), and their mixtures. Quantitative analysis of the effect on micelles on the velocity of NBOC decarboxylation allowed the estimation of the rate constants in the micellar pseudophase, k(m), for the pure surfactants and their mixtures. The extent of micellar catalysis for NBOC decarboxylation, expressed as the ratio k(m)/k(w), where k(w) is the rate constant in water, varied from 240 for HPS to 62 for HPC. With HPS or DPS, k(m) decreased linearly with CTAB(C) mole fraction, suggesting ideal mixing. With HPC, k(m) increased to a maximum at a CTAB(C) mole fraction of ca. 0.5 and then decreased at higher CTAB(C). Addition of CTAB(C) to HPC, where the negative charge of the surfactant is close to the hydrophobic core, produces tight ion pairs at the interface and, consequently, decreases interfacial water contents. Interfacial dehydration at the surface in equimolar HPC/CTAB(C) mixtures, and interfacial solubilization site of the substrate, can explain the observed catalytic synergy, since the rate of NBOC decarboxylation increases markedly with the decrease in hydrogen bonding to the carboxylate group. 相似文献