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31.
Quantum chemical calculations were performed to study the mechanism of ethene epoxidation with hydrogen peroxide. The calculations were carried out at the B3LYP/6-311+G(d,p) level of theory. The applicability of this functional to the problem at hand, including basis set effects, was validated by CCSD(T) and CASSCF based multireference MP2 calculations. A mechanism was determined where hydrogen peroxide becomes polarized in the transition state upon binding to the ethene molecule. The distant hydroxide fragment of the attached hydrogen peroxide molecule becomes partly negatively charged, while the other part of the molecule involves a proton and becomes partly positively charged. In the absence of water an activation energy of 139.7 kJ mol(-1) was determined for the isolated H(2)O(2) + C(2)H(4) system. By microsolvating with water, the impact of a hydrogen-bonded network on the activation energy was addressed. A 43.7 kJ mol(-1) lowering of the activation energy, DeltaE(a), was observed when including up to 4 water molecules in the model. This effect results from the stabilization of the proton and hydroxide fragments in the transition state. The findings are discussed in the context of previous theoretical studies on similar systems. Effects of adding or removing a proton to mimic acidic and alkaline conditions are addressed and the limitations of the model in solvating the excess charge are discussed. 相似文献
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33.
Influence of adding carbon nanotubes on photoelectric conversion properties of dye-doped titania gel
Hiromasa Nishikiori Takuma Ohta Yohei Uesugi Hiroyuki Itai Morinobu Endo Tsuneo Fujii 《Research on Chemical Intermediates》2012,38(8):1857-1869
Multiwalled carbon nanotubes (MWCNTs) were incorporated into amorphous dye-doped titania gel by the sol?Cgel method at room temperature. The working electrodes were prepared by coating the ITO glass with the sol?Cgel titania precursor containing the dye and MWCNTs. The photoelectric conversion properties of the electrodes were examined by simple spectroscopic and electric measurements. The photocurrent spectrum originated from the absorption of the dye. The short circuit photocurrent was enhanced by adding a small amount of MWCNTs evenly to the amorphous dye-doped titania gel. The open circuit voltage was due to the semiconducting characteristics property of the titania gel. The experimental results indicated the electron transport from the dye excited states to the MWCNTs through the titania gel. The MWCNTs functioned as bridges between the titania and ITO. Steam treatment of the titania gel electrodes significantly increased the photoelectric performance due to crystallization of the titania and enhancement of the dye?Ctitania interaction forming the chelate complex on the titania particle surface. 相似文献
34.
Antenatal diagnosis of placenta accreta with MR is not easy even now because T2-weighted images (T2WI) cannot differentiate chorionic villi from decidua basalis. We performed dynamic contrast MRI to study whether trophoblastic villi could be separately demonstrated from the decidua basalis, and whether the contrast resolution between the placenta and myometrium could improve compared to T2WI. Six pregnant women with prior cesarean section were examined at 34-38 gestational weeks. Sagittal T2-weighted images with fast spin echo sequences and dynamic contrast studies with fast field echo sequence every 10-14 s after contrast injection were performed. We analyzed the enhancing pattern of the placenta and compared the contrast between placenta and myometrium. We reviewed medical records to identify complications during the placental delivery and the complications of their newborns. In the early phase after contrast enhancement, multiple foci of the strong lobular enhancement were observed in all cases. Other parts of placenta were slowly but strongly enhanced following them. We speculated that the former corresponded to intervillous space and the latter decidua basalis. The contrast between placenta and myometrium tended to be distinct near the inner cervical os on both T2WI and dynamic contrast study. On the other hand, it was indistinct in the upper part of the uterine body on T2WI despite it was clearly demonstrated on dynamic contrast study. The placentae were delivered without any complication in all cases. Although two neonates showed fetal distress, none of the infant remained any sequelae at the time of the discharge. The other four were well although one of them complicated with meconium staining. As dynamic contrast MRI can differentiate chorionic villi and decidua basalis, and can provide excellent contrast between placenta and myometrium at anywhere within the uterus, it may be a promising technique for antepartum diagnosis of the placenta accreta. 相似文献
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36.
It is well known that there are planar sets of Hausdorff dimension greater than 1 which are graphs of functions, i.e., all
their vertical fibres consist of 1 point. We show this phenomenon does not occur for sets constructed in a certain “regular”
fashion. Specifically, we consider sets obtained by partitioning a square into 4 subsquares, discarding 1 of them and repeating
this on each of the 3 remaining squares, etc.; then almost all vertical fibres of a set so obtained have Hausdorff dimension
at least 1/2. Sharp bounds on the dimensions of sets of exceptional fibres are presented.
Partially supported by a grant from the Landau Centre for Mathematical Analysis. 相似文献
37.
Itai Benjamini 《Journal of Theoretical Probability》1991,4(3):631-637
In this note we construct two quasi-isometric graphs. One admits an infinite dimensional space of nonconstant bounded harmonic functions, while the other admits only constant bounded harmonic functions. Translation of the construction to manifolds answers a problem due to T. Lyons. 相似文献
38.
39.
Alon Itai Michael Rodeh 《Journal of Algorithms in Cognition, Informatics and Logic》1985,6(3):409-429
Consider k stations wishing to transmit messages over a network of channels to a common receiver. The capacity of a channel is the maximum amount of data which can be transmitted in a time unit. In addition to the transmission stations, the network contains switching nodes. Given that the jth station has σj messages (j = 1,…, k) to transmit, it is desired to find a schedule with minimum completion time T. The amount of data sent over a channel may vary in time. A schedule is stationary if the amount of data sent in a time unit is constant throughout the schedule. It is first shown that for every schedule there exists a stationary schedule with the same completion time. Thus, the search for an optimum schedule is confined to stationary schedules. The problem of finding an optimum stationary schedule is formulated as a multisource single-sink network flow problem, in which the net amount of outgoing flow from each source (transmission station) within one time unit is . An O(k|E||V|2) time algorithm to find the minimum T similar to Dinic's flow algorithm is suggested. Using Sleator and Tarjan's techniques an O(k2|E||V|log|V|) algorithm is derived. The running time of both algorithms is independent of the σj's and the capacities. 相似文献
40.
For the purpose of utilizing ESDIAD as a real-time probe for surface processes, we have developed an instrument which can measure ESDIAD images and time of flight (TOF) spectra of desorbing ions in temperature-programmed surface processes. TOF measurements are carried out to identify the mass and to determine the kinetic energy distribution of the desorbed ions. This temperature-programmed (TP-) ESDIAD/TOF system was used to observe coadsorption layers of methylamine and CO on Ru(001) which have been previously studied by our group using LEED, TPD and HREELS, also drawing upon a comparison of findings with the coadsorption system of CO and ammonia. ESDIAD images acquired for temperature-programmed surface processes in real time were found to provide new insight into the dynamic behaviour of the coadsorption layers. As to the pure adsorption of ammonia and methylamine, the second and the first (chemisorbed) layers can be easily discriminated in their different ESD detection efficiency due to the difference in neutralization rate. The intensity change of H+ ions with temperature shows the process of the decomposition of methylamine to be dependent on CO coverage. The intensity of O+ originating from CO changes due to the change of CO adsorption site in the reaction process. The angular distribution of H+ ions which correspond to CH2=NH…Ru species appears at 250–300 K in the presence of high CO pre-coverage. 相似文献