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71.
Solans-Monfort X Chow C Gouré E Kaya Y Basset JM Taoufik M Quadrelli EA Eisenstein O 《Inorganic chemistry》2012,51(13):7237-7249
DFT(B3PW91) calculations have been carried out to propose a pathway for the N(2) cleavage by H(2) in the presence of silica-supported tantalum hydride complexes [(≡SiO)(2)TaH(x)] that forms [(≡SiO)(2)Ta(NH)(NH(2))] (Science 2007, 317, 1056). The calculations, performed on the cluster models {μ-O[(HO)(2)SiO](2)}TaH(1) and {μ-O[(HO)(2)SiO](2)}TaH(3), labelled as (≡SiO)(2)TaH(x) (x = 1, 3), show that the direct hydride transfers to coordinated N-based ligands in (≡SiO)(2)TaH(η(2)-N(2)) and (≡SiO)(2)TaH(η(2)-HNNH) have high energy barrier barriers. These high energy barriers are due in part to a lack of energetically accessible empty orbitals in the negatively charged N-based ligands. It is shown that a succession of proton transfers and reduction steps (hydride transfer or 2 electron reduction by way of dihydride reductive coupling) to the nitrogen-based ligands leads to more energetically accessible pathways. These proton transfers, which occur by way of heterolytic activation of H(2), increase the electrophilicity of the resulting ligand (diazenido, N(2)H(-), and hydrazido, NHNH(2)(-), respectively) that can thus accept a hydride with a moderate energy barrier. In the case of (≡SiO)(2)TaH(η(2)-HNNH), the H(2) molecule that is adding across the Ta-N bond is released after the hydride transfer step by heterolytic elimination from (≡SiO)(2)TaH(NH(2))(2), suggesting that dihydrogen has a key role in assisting the final steps of the reaction without itself being consumed in the process. This partly accounts for the experimental observation that the addition of H(2) is needed to convert an intermediate, identified as a diazenido complex [(≡SiO)(2)TaH(η(2)-HNNH)] from its ν(N-H) stretching frequency of 3400 cm(-1), to the final product. Throughout the proposed mechanism, the tantalum remains in its preferred high oxidation state and avoids redox-type reactions, which are more energetically demanding. 相似文献
72.
Mixed convection heat transfer about a semi-infinite inclined plate in the presence of magneto and thermal radiation effects
is studied. The fluid is assumed to be incompressible and dense. The nonlinear coupled parabolic partial differential equations
governing the flow are transformed into the non-similar boundary layer equations, which are then solved numerically using
the Keller box method. The effects of the mixed convection parameter R
i, the angle of inclination α, the magnetic parameter M and the radiation–conduction parameter R
d on the velocity and temperature profiles as well as on the local skin friction and local heat transfer parameters. For some
specific values of the governing parameters, the results are compared with those available in the literature and a fairly
good agreement is obtained. 相似文献
73.
Problem-based learning (PBL) and science, technology, engineering, and mathematics (STEM) are two acronyms widely visible in education literature today. However, few studies have explored these in connection with one another, specifically with regard to teacher preparation. This study investigated how 47 prospective elementary teachers developed PBL units and how they integrated STEM and other disciplines into those units. It also addressed the affordances and constraints of integrated STEM as perceived by the prospective elementary teachers. Data sources in this multimethod study included PBL units and interviews. Findings revealed that all of the units integrated at least two of the STEM disciplines, as well as literacy, in a variety of ways. The prospective teachers articulated perceived benefits of integrated STEM, such as: making connections across content areas, preparing students for the real world, teaching students that failure is not a bad thing, and providing future opportunities. They also addressed perceived barriers of integrated STEM, such as: having limited experience with the content, diminishing the effect of individual content areas, and needing better curriculum alignment. Overall, this study provides evidence that PBL can be a pedagogical approach to integrate STEM. Implications for teachers, teacher educators, and curriculum specialists are discussed. 相似文献
74.
Alkan A Kutlu R Hallac T Sigirci A Emul M Pala N Altinok T Aslan M Sarac K Ozcan C 《Magnetic resonance imaging》2004,22(5):707-713
Our purpose was to investigate, by magnetic resonance (MR) spectroscopy, the metabolite changes in the brains of subjects in the shoemaking industry who had been chronically exposed to organic solvents. A total of 49 male subjects and 30 age-matched healthy volunteers underwent detailed neurological and psychiatric examinations. All subjects had long-echo [repetition time (TR) 2000 ms, echo time (TE) 136 ms] single-voxel MR spectroscopy. Voxels (15 x 15 x 15 mm(3)) were placed in the parietal white matter, thalamus, and basal ganglia. N-acetylaspartate (NAA)/creatine (Cr) and choline (Cho)/Cr ratios were calculated. There was no significant difference between the study subjects and the control group in NAA/Cr ratios obtained from thalamus, basal ganglia, and parietal white matter. Cho/Cr ratios in thalamus, basal ganglia, and parietal white matter were found to be significantly increased compared to controls. There was a positive correlation between basal ganglia Cho/Cr ratio and duration of exposure (r = 0.63). MR spectroscopy should be performed to reveal metabolite changes and determine the degree of brain involvement in solvent-related industry workers. 相似文献
75.
We investigate the resonant production of color octet muons in order to explore the discovery potential of Future Circular Collider(FCC)-based μp colliders.It is shown that the search potentials of μp colliders essentially surpass the potential of the LHC and would exceed that of the FCC pp collider. 相似文献
76.
Polycaprolactone (PCL) based α,ω-methacrylated macromonomer (DMPCL) was synthesized via enzymatic ring-opening polymerization (eROP) by using Novozyme 435 as the enzyme immobilized catalyst. DMPCL was further photopolymerized with monofunctional poly(ethylene glycol) methyl ether methacrylate (PEGMA-950) macromonomer and trimethylolpropane triacrylate (TMPTA) as tri-functionalized crosslinking agent in glass vials when CHCl3 was the solvent and Irgacure 819 was the photoinitiator. Ultraviolet (UV) Light Emitting Diode (LED) bulbs enabled photoinduced reactions at room temperature with low heat generation and high reaction efficiency. The obtained gels were characterized with Fourier Transform Infrared Spectroscopy (FT-IR) and Differential Scanning Calorimetry (DSC). DMPCL participated as an effective crosslinking agent in the photopolymerization of PEGMA-950. Combined usage of DMPCL and PEGMA-950 resulted in significantly more effective polymerization than the separate photopolymerizations of these macromonomers. 相似文献
77.
Regina S. Burachik Rafail N. Gasimov Nergiz A. Ismayilova C. Yalçin. Kaya 《Journal of Global Optimization》2006,34(1):55-78
We study convergence properties of a modified subgradient algorithm, applied to the dual problem defined by the sharp augmented
Lagrangian. The primal problem we consider is nonconvex and nondifferentiable, with equality constraints. We obtain primal
and dual convergence results, as well as a condition for existence of a dual solution. Using a practical selection of the
step-size parameters, we demonstrate the algorithm and its advantages on test problems, including an integer programming and
an optimal control problem.
*Partially Supported by 2003 UniSA ITEE Small Research Grant Ero2.
Supported by CAPES, Brazil, Grant No. 0664-02/2, during her visit to the School of Mathematics and Statistics, UniSA. 相似文献
78.
We consider a biodiesel production company that collects waste vegetable oil from source points that generate waste in large amounts. The company uses the collected waste as raw material for biodiesel production. The manager of this company needs to decide which of the present source points to include in the collection program, which of them to visit on each day, which periodic routing schedule to repeat over an infinite horizon and how many vehicles to operate such that the total collection, inventory and purchasing costs are minimized while the production requirements and operational constraints are met. For this selective and periodic inventory routing problem, we propose two different formulations, compare them and apply the better performing one on a real-world problem with 36 scenarios. We generate lower bounds using a partial linear relaxation model, and observe that the solutions obtained through our model are within 3.28% of optimality on the average. Several insights regarding the customer selection, routing and purchasing decisions are acquired with sensitivity analysis. 相似文献
79.
Using explicit constructions of the Weierstrass mock modular form and Eisenstein series coefficients, we obtain closed formulas for the generating functions of values of shifted convolution L-functions associated to certain elliptic curves. These identities provide a surprising relation between weight 2 newforms and shifted convolution L-values when the underlying elliptic curve has modular degree 1 with conductor N such that \(\text {genus}(X_0(N)) = 1\). 相似文献
80.
Murat Kaya Mehmet Gökhan Halıcı Fatih Duman Sevil Erdoğan Talat Baran 《Natural product research》2015,29(13):1280-1284
Lichens are symbiotic associations formed mainly by ascomycete fungi and green algae or cyanobacteria. The presence of chitin in the fungal cell wall has been revealed by previous studies. Considering the presence of fungi in the lichens, this work determines the presence of chitin in a cosmopolitan lichen species Xanthoria parietina. In this study, chitin was derived from a lichen species for the first time and its physicochemical properties were determined by Fourier transform infrared spectroscopy, thermogravimetric analysis, X-ray diffraction, scanning electron microscopy and elemental analysis. The dry weight chitin content of X. parietina was 4.23%, and this chitin was in the α-form. The crystalline index value of the lichen chitin was calculated as 70.1%. The chitin from X. parietina had a smooth surface. 相似文献