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51.
The present review reports on the preparation and atomic-scale characterization of the thinnest possible films of the glass-forming materials silica and germania. To this end state-of-the-art surface science techniques, in particular scanning probe microscopy, and density functional theory calculations have been employed. The investigated films range from monolayer to bilayer coverage where both, the crystalline and the amorphous films, contain characteristic XO4 (X=Si,Ge) building blocks. A side-by-side comparison of silica and germania monolayer, zigzag phase and bilayer films supported on Mo(112), Ru(0001), Pt(111), and Au(111) leads to a more general comprehension of the network structure of glass former materials. This allows us to understand the crucial role of the metal support for the pathway from crystalline to amorphous ultrathin film growth.  相似文献   
52.
The study reports the first attempt to address the interplay between surface and bulk in hydride formation in ceria (CeO2) by combining experiment, using surface sensitive and bulk sensitive spectroscopic techniques on the two sample systems, i.e., CeO2(111) thin films and CeO2 powders, and theoretical calculations of CeO2(111) surfaces with oxygen vacancies (Ov) at the surface and in the bulk. We show that, on a stoichiometric CeO2(111) surface, H2 dissociates and forms surface hydroxyls (OH). On the pre-reduced CeO2−x samples, both films and powders, hydroxyls and hydrides (Ce−H) are formed on the surface as well as in the bulk, accompanied by the Ce3+ ↔ Ce4+ redox reaction. As the Ov concentration increases, hydroxyl is destabilized and hydride becomes more stable. Surface hydroxyl is more stable than bulk hydroxyl, whereas bulk hydride is more stable than surface hydride. The surface hydride formation is the kinetically favorable process at relatively low temperatures, and the resulting surface hydride may diffuse into the bulk region and be stabilized therein. At higher temperatures, surface hydroxyls can react to produce water and create additional oxygen vacancies, increasing its concentration, which controls the H2/CeO2 interaction. The results demonstrate a large diversity of reaction pathways, which have to be taken into account for better understanding of reactivity of ceria-based catalysts in a hydrogen-rich atmosphere.  相似文献   
53.
The three-component reaction comprising the interaction of 2-amino-4-antipyrinyl-5-ethylthiazole (1) with s-triazine (2) and pyrrolidine leads to 4-anitpyrinyl-5-ethyl-2-[(4-pyrrolidinyl)methyleneamino]thiazole (5). Structure 5 is supported by 1H- and 13C-NMR spectroscopy.  相似文献   
54.
We introduce the notion of n-fold track extensions of a category C by a natural system D and prove that such extensions represent classes in the cohomology of C with coefficients in D introduced by Baues–Wirsching. This generalizes a result of Huebschmann on the cohomology of groups.  相似文献   
55.
To characterize E. D. Sontag’s system of axioms for control-systems in a more operative manner we consider an equivalent algebraic structure, which we name Regel- Relative.  相似文献   
56.
    
The cyanine dyes Cy5 and Cy5.5 are presented as a new long wavelength-excitable donor-acceptor dye pair for homogeneous fluoroimmunoassays. The deactivation pathways responsible for the quenching of the fluorescence of the antibody-bound donor are elucidated. Upon binding of the donor dye to the antibodies at low dye/protein ratios, its fluorescence quantum yield rises to unity. Higher dye/protein ratios lead to progressive aggregation of the dyes, which results in quenching of monomer fluorescence due to resonance energy transfer (RET) from the monomers to the nonfluorescent dimers. The dependence of the quenching efficiency on the labeling ratio is described quantitatively by assuming a Poisson distribution of the dyes over the antibodies. The maximum fluorescence intensity per antibody is obtained at a labeling ratio of 4. Upon formation of the antibody-antigen complex, electron transfer and RET to the antigen-bound acceptor dye occur. Steady-state and time-resolved fluorescence measurements reveal that approximately 50% of the donor quenching is due to RET, while the residual quenching effect is caused by the static quenching process.  相似文献   
57.
路军岭  高鸿钧  时东霞 《物理》2007,36(5):370-376
现实中的催化剂是个相当复杂的系统体系,且为粉末状,限制了多种表面科学表征手段的应用,科学家通过建立简化的催化剂模型,充分利用目前多种有力的科技分析手段,如扫描隧道显微镜(STM)、透射电镜(TEM)、光电子能谱(XPS)、傅里叶变换红外吸收谱(FTIR)、电子能量损失谱(EELS)等,直观地在原子尺度上研究催化反应的机理,从而使得人们能够设计出选择性能更高、催化性能更好的催化剂.  相似文献   
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