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1.
Franklin D. Hardcastle Israel E. Wachs Hellmut Eckert David A. Jefferson 《Journal of solid state chemistry》1991,90(2)
The Bi2O3---V2O5 system was examined using Raman spectroscopy and solid state 51V wideline, magic-angle spinning (MAS), and nutation NMR spectroscopy. The methods are shown to be complementary in the identification of the various phases and in the characterization of their vanadium site symmetries. Most of the compositions examined (1:1 ≤ Bi:V ≤ 60:1) are multiphasic. Depending on the Bi:V ratio, the following phases have been identified: BiVO4, Bi4V2O11, a triclinic type-II phase, a cubic type-I phase, γ-Bi2O3 doped with V(V) (sillenite), and β-Bi2O3. Detailed spectroscopic characterization reveals that vanadium is tetrahedrally coordinated in all these compounds, and that the degree of symmetry increases with increasing Bi:V ratio. At the highest Bi:V ratios, the combined interpretation of the Raman and NMR data provides strong evidence for the presence of Bi5+O4 tetrahedra. 相似文献
2.
CH3OH temperature programmed surface reaction (TPSR) spectroscopy was employed to determine the chemical nature of active surface sites for bulk mixed metal oxide catalysts. The CH3OH-TPSR spectra peak temperature, Tp, for model supported metal oxides and bulk, pure metal oxides was found to be sensitive to the specific surface metal oxide as well as its oxidation state. The catalytic activity of the surface metal oxide sites was found to decrease upon reduction of these sites and the most active surface sites were the fully oxidized surface cations. The surface V5+ sites were found to be more active than the surface Mo6+ sites, which in turn were significantly more active than the surface Nb5+ and Te4+ sites. Furthermore, the reaction products formed also reflected the chemical nature of surface active sites. Surface redox sites are able to liberate oxygen and yield H2CO, while surface acidic sites are not able to liberate oxygen, contain either H+ or oxygen vacancies, and produce CH3OCH3. Surface V5+, Mo6+, and Te4+ sites behave as redox sites, and surface Nb5+ sites are Lewis acid sites. This experimental information was used to determine the chemical nature of the different surface cations in bulk Mo-V-Te-Nb-Ox mixed oxide catalysts (Mo(0.6)V(1.5)Ox, Mo(1.0)V(0.5)Te(0.16)Ox, Mo(1.0)V(0.3)Te(0.16)Nb(0.12)Ox). The bulk Mo(0.6)V(1.5)Ox and Mo(1.0)V(0.5)Te(0.16)Ox mixed oxide catalytic characteristics were dominated by the catalytic properties of the surface V5+ redox sites. The surface enrichment of these bulk mixed oxide by surface V5+ is related to its high mobility, V5+ possesses the lowest Tammann temperature among the different oxide cations, and the lower surface free energy associated with the surface termination of V=O bonds. The quaternary bulk Mo(1.0)V(0.3)Te(0.16)Nb(0.12)Ox mixed oxide possessed both surface redox and acidic sites. The surface redox sites reflect the characteristics of surface V5+ and the surface acidic sites reflect the properties normally associated with supported Mo6+. The major roles of Nb5+ and Te4+ appear to be that of ligand promoters for the more active surface V and Mo sites. These reactivity trends for CH3OH ODH parallel the reactivity trends of propane ODH because of their similar rate-determining step involving cleavage of a C-H bond. This novel CH3OH-TPSR spectroscopic method is a universal method that has also been successfully applied to other bulk mixed metal oxide systems to determine the chemical nature of the active surface sites. 相似文献
3.
Dr. Kazuhiko Amakawa Dr. Lili Sun Dr. Chunsheng Guo Dr. Michael Hävecker Pierre Kube Prof. Dr. Israel E. Wachs Soe Lwin Prof. Dr. Anatoly I. Frenkel Dr. Anitha Patlolla Prof. Dr. Klaus Hermann Prof. Dr. Robert Schlögl Dr. Annette Trunschke 《Angewandte Chemie (International ed. in English)》2013,52(51):13553-13557
Highly dispersed molybdenum oxide supported on mesoporous silica SBA‐15 has been prepared by anion exchange resulting in a series of catalysts with changing Mo densities (0.2–2.5 Mo atoms nm?2). X‐ray absorption, UV/Vis, Raman, and IR spectroscopy indicate that doubly anchored tetrahedral dioxo MoO4 units are the major surface species at all loadings. Higher reducibility at loadings close to the monolayer measured by temperature‐programmed reduction and a steep increase in the catalytic activity observed in metathesis of propene and oxidative dehydrogenation of propane at 8 % of Mo loading are attributed to frustration of Mo oxide surface species and lateral interactions. Based on DFT calculations, NEXAFS spectra at the O‐K‐edge at high Mo loadings are explained by distorted MoO4 complexes. Limited availability of anchor silanol groups at high loadings forces the MoO4 groups to form more strained configurations. The occurrence of strain is linked to the increase in reactivity. 相似文献
4.
V. Topin F. Dubois Y. Monerie F. Perales A. Wachs 《ournal of non Newtonian Fluid Mechanics》2011,166(1-2):63-72
We rely here on a non-smooth contact dynamics (NSCD) approach to treat particle collisions in a direct numerical simulation of a dense particulate flow. Interactions between particles are considered by a non-smooth formulation of particle dynamics at the microscopic scale, which enables one to straightforwardly implement complex contact laws. The hydrodynamic coupling is achieved by a distributed Lagrange multiplier/fictitious domain (DLM/FD) method. As a preliminary step, the relevance of our NSCD-DLM/FD method is assessed by comparing results of 2D sedimentation simulations with those obtained with a usual molecular dynamics collision model. Then, we use it to investigate how a fully immersed granular packing collapses depending on its initial particle volume fraction, providing clues on the micro-rheology of dense particulate flows. 相似文献
5.
6.
Moiré experimental techniques are used to measure displacement fields in viscoelastic plates undergoing large deformations at elevated temperatures. These experimental procedures are applicable to determining displacement fields in nonlinear materials. As preliminary information, the material properties are determined from creep studies. The moiré method is used to determine the strains under constant load and isothermal conditions. Tests are conducted for several combinations of load and temperature for 2.5 decades of time. Assuming thermorheologically simple behavior, the data are shifted to establish the creep extensional compliance over ten decades in time. The constitutive equations are formulated as integral equations, the kernels of which are the functions that were measured in this work. These equations are solved exactly for the infinitesimal case. The finite case is then approximated by an incremental superposition of a series of successiye infinitesimal solutions. The results are applied to a plate initially containing a circular hole, and are shown to agree closely with the experimental measurements. 相似文献
7.
Anders Bjö rner Michelle L. Wachs 《Transactions of the American Mathematical Society》1997,349(10):3945-3975
This is a direct continuation of Shellable Nonpure Complexes and Posets. I, which appeared in Transactions of the American Mathematical Society 348 (1996), 1299-1327.
8.
Numerical results are presented for a one-dimensional diffusion model for freely diffusing positrons in thin films with an initial exponential positron profile. The results are for two boundary conditions which are experimentally realizable. Since thermalized positrons generally obey this diffusion model, it should be possible to extract the bulk diffusion constant by fitting experimental measurements to the model's predictions. Recently, a scheme has been proposed for the brightness enhancement of slow positron beams. We discuss experimental methods for implementing this scheme and the various problems that may arise.Summer student at Brookhaven National Laboratory, 1980 相似文献
9.
The oxidation of CH3CN over silver particles was examined between 200 and 300°C. The kinetic data exhibit an unusually abrupt change in activity between 270 and 300°C which is attributed to the oxidation/decomposition of surface AgCN and possibly AgOCN. 相似文献
10.