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51.
Sanja Stevanović Vladimir Panić Dušan Tripković Vladislava M. Jovanović 《Electrochemistry communications》2009,11(1):18-21
The contribution of carbon functional groups (CFG) to methanol oxidation at carbon-supported Pt catalysts is studied in this work. Platinum black, attached in a form of a thin layer to electrochemically treated glassy carbon (GC), is investigated as a model system. Impedance measurements reveal significant changes in capacitive response of GC anodically polarized in H2SO4 solution in comparison to unoxidized state. XPS analyses show the increased fraction of oxygen-containing CFGs upon electrochemical treatment of GC. The activity of Pt black attached to oxidized GC for methanol oxidation is more than two times larger in comparison to the catalyst attached to unoxidized GC. Increased activity is most likely due to the promotion of COads removal by increased content of CFGs. 相似文献
52.
Stevanović SI Panić VV Dekanski AB Tripković AV Jovanović VM 《Physical chemistry chemical physics : PCCP》2012,14(26):9475-9485
We report on new insights into the relationships between structure and activity of glassy carbon (GC), as a model material for electrocatalyst support, during its anodization in acid solution. Our investigation strongly confirms the role of CFGs in promotion of Pt activity by the "spill-over" effect related to CO(ads) for methanol electrooxidation (MEO) on a carbon-supported Pt catalyst. Combined analysis of voltammetric and impedance behaviour as well as changes in GC surface morphology induced by intensification of anodizing conditions reveal an intrinsic influence of the carbon functionalization and the structure of a graphene oxide (GO) layer on the electrical and electrocatalytic properties of activated GC. Although GO continuously grows during anodization, it structurally changes from being a graphite inter-layer within graphite ribbons toward a continuous GO surface layer that deteriorates the native structure of GC. As a consequence of the increased distance between GO-spaced graphite layers, the GC conductivity decreases until the case of profound GO exfoliation under drastic anodizing conditions. This exposes the native, yet abundantly functionalized, GC texture. While GC capacitance continuously increases with intensification of anodizing conditions, the surface nano-roughness and GO resistance reach the highest values at modest anodizing conditions, and then decrease upon drastic anodization due to the onset of GO exfoliation. We found for the first time that the activity of a GC-supported Pt catalyst in MEO, as one of the promising half-reactions in polymer electrolyte fuel cells, strictly follows the changes in GC nano-roughness and GO-induced GC resistance. The highest GC/Pt MEO activity is reached when optimal distance between graphite layers and optimal degree of GC functionalization bring the highest amount of CFGs into intimate contact with the Pt surface. This confirms the promoting role of CFGs in MEO catalysis. 相似文献
53.
In this paper a qualocation method is analysed for parabolicpartial differential equations in one space dimension. Thismethod may be described as a discrete H1-Galerkin method inwhich the discretization is achieved by approximating the integralsby a composite Gauss quadrature rule. An O (h4-i) rate of convergencein the Wi.p norm for i = 0, 1 and 1 p is derived for a semidiscretescheme without any quasi-uniformity assumption on the finiteelement mesh. Further, an optimal error estimate in the H2 normis also proved. Finally, the linearized backward Euler methodand extrapolated Crank-Nicolson scheme are examined and analysed. 相似文献
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In this article, we propose and analyze an alternate proof of a priori error estimates for semidiscrete Galerkin approximations to a general second order linear parabolic initial and boundary value problem with rough initial data. Our analysis is based on energy arguments without using parabolic duality. Further, it follows the spirit of the proof technique used for deriving optimal error estimates for finite element approximations to parabolic problems with smooth initial data and hence, it unifies both theories, that is, one for smooth initial data and other for nonsmooth data. Moreover, the proposed technique is also extended to a semidiscrete mixed method for linear parabolic problems. In both cases, optimal L 2-error estimates are derived, when the initial data is in L 2. A superconvergence phenomenon is also observed, which is then used to prove L ∞-estimates for linear parabolic problems defined on two-dimensional spatial domain again with rough initial data. 相似文献
56.
Saumya Bajpai Neela Nataraj Amiya K. Pani Pedro Damazio Jin Yun Yuan 《Numerical Methods for Partial Differential Equations》2013,29(3):857-883
Finite element Galerkin method is applied to equations of motion arising in the Kelvin–Voigt model of viscoelastic fluids for spatial discretization. Some new a priori bounds which reflect the exponential decay property are obtained for the exact solution. For optimal L∞( L 2) estimate in the velocity, a new auxiliary operator which is based on a modification of the Stokes operator is introduced and analyzed. Finally, optimal error bounds for the velocity in L∞( L 2) as well as in L∞( H )‐norms and the pressure in L∞(L2)‐norm are derived which again preserves the exponential decay property. © 2012 Wiley Periodicals, Inc. Numer Methods Partial Differential Eq, 2013 相似文献
57.
An efficient synthesis of 3,4-dihydropyrimidine 2(1H)-ones and thiones(3,4-DHPMs) core was prepared by one-pot threecomponent Biginelli condensation and which was catalyzed by trifluoromethane sulfonic acid.The classical Bignelli reaction has been extended by the use of N-substituted benzoxazolyl semicarbazides and thiosemicarbazides and this method has the advantage of excellent yields and short reaction times. 相似文献
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Synthesis,crystal structure and magnetic properties of Yb8Ag18.5Al47.5, Yb2Pd2Cd and Yb1.35Pd2Cd0.65
S.K. Dhar R. Settai Y. Ōnuki A. Galatanu Y. Haga P. Manfrinetti M. Pani 《Journal of magnetism and magnetic materials》2007
We report the synthesis of three new Yb-based compounds, Yb8Ag18.5Al47.5 (Yb8Cu17Al49-type, tetragonal tI74–I4/mmm), Yb2Pd2Cd (Mo2B2Fe-type, tetragonal tP10-P4/mbm) and Yb1.35Pd2Cd0.65 (MnCu2Al-type, cubic cF16–Fm3¯m). The crystal symmetry of these compounds has been determined and the complete structural characterisation carried out by single crystal and powder diffraction techniques. Two symmetry in-equivalent sites are available for the Yb ions in Yb8Ag18.5Al47.5 and Yb1.35Pd2Cd0.65. The 4f levels of the Yb ions are appreciably hybridised in Yb8Ag18.5Al47.5 and to a lesser extent in Yb2Pd2Cd as inferred from the magnetisation and heat capacity data. Signatures of heavy fermion behaviour are observed in the heat capacity data of Yb2Pd2Cd in which the heat capacity, C/T, increases at low temperatures attaining a value of ≈600 mJ/mol K2 at 1.8 K. The electrical resistivity of Yb2Pd2Cd follows a linear variation with temperature, T, between 1.4 and 5 K, thus indicating a possible non-Fermi liquid behaviour. In contrast, Yb ions are trivalent in Yb1.35Pd2Cd0.65 and order magnetically near 1.4 K. 相似文献