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排序方式: 共有266条查询结果,搜索用时 15 毫秒
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Benz L Park A Corey JR Mezher MP Park VC 《Langmuir : the ACS journal of surfaces and colloids》2012,28(27):10209-10216
The interaction of two sets of structurally related molecules, thiophenol/thioanisole, and thiophene/tetrahydrothiophene, with vacuum-annealed and ion-bombarded TiO(2)(110) surfaces has been studied using a combination of temperature-programmed reaction spectroscopy (TPRS) and X-ray photoelectron spectroscopy (XPS). All thioethers studied were observed to adsorb and desorb from both surfaces without producing reaction products, while thiophenol, the only species studied containing a S-H bond, reacted with both surfaces. Approximately 25% of surface bound thiophenol decomposed over the vacuum-annealed surface. On the bombarded surface, thiophenol both decomposed into surface-bound C(x)H(y)/S fragments, and reacted to form benzene, which desorbed from the surface at 400 K. We propose that phenylthiolate formation on the bombarded surface leads to the observed production of benzene. These results highlight the importance of defects in the reactivity of titania, and lay the foundation for the study of larger, refractory sulfur compounds present in fuel. 相似文献
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The luminescence intensity of Tb3+ embedded in sputter deposited and subsequently annealed AlN shows strong concentration dependence. The intensity of the characteristic green luminescence of Tb3+ rises at low concentrations with rising concentration. At higher concentrations, strong concentration quenching occurs. The optimum concentration range of Tb3+ in AlN was observed to range between 2.5 at% Tb and 3.6 at% Tb. The experimentally evaluated concentration dependence results can be described by a rate equation approach based on available models of luminescence quenching. 相似文献
96.
Reactions of acrolein, water, and oxygen with the vacuum-reduced surface of TiO2(1 1 0) are reported in a temperature programmed reaction study of the interaction of an aldehydic pollutant with a reducible metal oxide. A total of 25% of the acrolein that binds to the surface is converted to products. Notably, carbon-carbon coupling occurs with 86% selectivity for formation of C6 products: C6H8, identified as 1,3-cyclohexadiene, in a peak at 500 K and benzene immediately thereafter at 530 K. Acrolein is evolved from the surface in three peaks: a peak independent of coverage at 495 K, attributed to decomposition of an intermediate that is partly converted to C6H8; a coverage-dependent peak that shifts from 370 K (low coverage) to 260 K (high coverage), which is attributed to adsorption at 5-fold coordinated Ti sites; and a multilayer state at 160 K. Water and acrolein compete for 5-fold coordinated titanium sites when dosed sequentially. The addition of water also opens a new reaction pathway, leading to the hydrogenation of acrolein to form propanal. Water has no effect on the yield of 1,3-cyclohexadiene. Exposure of the surface to oxygen prior to acrolein dosing quenches the evolution of acrolein at 495 K and concurrently eliminates the coupling. From these results, we propose that reduced subsurface defects such as titanium ion interstitials play a role in the reactions observed here. The notion that subsurface defects may contribute to the reactivity of organic molecules over reducible oxide substrates may prove to be general. 相似文献
97.
Castro-Román F Benz RW White SH Tobias DJ 《The journal of physical chemistry. B》2006,110(47):24157-24164
In the absence of external stress, the surface tension of a lipid membrane vanishes at equilibrium, and the membrane exhibits long wavelength undulations that can be described as elastic (as opposed to tension-dominated) deformations. These long wavelength fluctuations are generally suppressed in molecular dynamics simulations of membranes, which have typically been carried out on membrane patches with areas <100 nm2 that are replicated by periodic boundary conditions. As a result, finite system-size effects in molecular dynamics simulations of lipid bilayers have been subject to much discussion in the membrane simulation community for several years, and it has been argued that it is necessary to simulate small membrane patches under tension to properly model the tension-free state of macroscopic membranes. Recent hardware and software advances have made it possible to simulate larger, all-atom systems allowing us to directly address the question of whether the relatively small size of current membrane simulations affects their physical characteristics compared to real macroscopic bilayer systems. In this work, system-size effects on the structure of a DOPC bilayer at 5.4 H2O/lipid are investigated by performing molecular dynamics simulations at constant temperature and isotropic pressure (i.e., vanishing surface tension) of small and large single bilayer patches (72 and 288 lipids, respectively), as well as an explicitly multilamellar system consisting of a stack of five 72-lipid bilayers, all replicated in three dimensions by using periodic boundary conditions. The simulation results are compared to X-ray and neutron diffraction data by using a model-free, reciprocal space approach developed recently in our laboratories. Our analysis demonstrates that finite-size effects are negligible in simulations of DOPC bilayers at low hydration, and suggests that refinements are needed in the simulation force fields. 相似文献
98.
Dr. Samuel E. Griffin Grant P. Domecus Clarissa E. Flores Dr. R. Eric Sikma Prof. Lauren Benz Prof. Seth M. Cohen 《Angewandte Chemie (International ed. in English)》2023,62(23):e202301611
Low-valent metal–organic frameworks (LVMOFs) and related materials have gained interest due to their potential applications in heterogeneous catalysis. However, of the few LVMOFs that have been reported, none have shown catalytic activity. Herein, a low-valent metal-organic material constructed from phosphine linkers and IrI nodes is reported. This material is effectively a crystalline, insoluble analogue of Vaska's complex. As such, the material reversibly binds O2 and catalyzes the reductive formation of enamines from amides. 相似文献
99.
Walter Benz 《Geometriae Dedicata》2000,81(1-3):219-230
For arbitrary pre-Hilbert spaces X of dimension at least 2, we define the notion of Lorentz–Minkowski distance. We determine all Lorentz transformations, i.e. all distance preserving mappings of X into itself, introduce relativistic addition, and characterize the 2-point-invariants of the group of bijective Lorentz tranformations and, especially, the distance in question. 相似文献
100.
In this study, we present the synthesis of 5-(3,5-dinitro-1H-pyrazol-4-yl)-1H-tetrazole and its energetic derivatives starting from 4-amino-3,5-dinitropyrazole, which was diazotized and cyanide substituted. A subsequent cycloaddition reaction with sodium azide led to 5-(3,5-dinitro-1H-pyrazol-4-yl)-1H-tetrazole ( 3 ). Several alkaline metal and nitrogen-rich salts were prepared and characterized by low-temperature X-ray diffraction. Additionally, all compounds were analyzed by vibrational spectroscopy (IR), 1H, 13C and 14N NMR spectroscopy, elemental analysis and differential thermal analysis (DTA). Additionally, the heats of formation for selected compounds were calculated using the atomization method based on CBS-4M enthalpies as well as important detonation parameters by using the EXPLO5 code (V6.05). Furthermore, the sensitivities of 3 and all synthesized salts toward friction, impact and electrostatic discharge according to BAM (Bundesamt für Materialforschung) were determined and compared to RDX. 相似文献