TiO2-ZrO2 (Ti-Zr) carrier was prepared by a co-precipitation method and 1 wt. % V2O5 and 0.2 CeO2 (the Mole ratio of Ce to Ti-Zr) was impregnated to obtain the V2O5-CeO2/TiO2-ZrO2 catalyst for the selective catalytic reduction of NOx by NH3. The transient activity tests and the in situ DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) analyses were employed to explore the NH3-SCR (selective catalytic reduction) mechanism systematically, and by designing various conditions of single or mixing feeding gas and pre-treatment ways, a possible pathway of NOx reduction was proposed. It was found that NH3 exhibited a competitive advantage over NO in its adsorption on the catalyst surface, and could form an active intermediate substance of -NH2. More acid sites and intermediate reaction species (-NH2), at lower temperatures, significantly promoted the SCR activity of the V2O5-0.2CeO2/TiO2-ZrO2 catalyst. The presence of O2 could promote the conversion of NO to NO2, while NO2 was easier to reduce. The co-existence of NH3 and O2 resulted in the NH3 adsorption strength being lower, as compared to tests without O2, since O2 could occupy a part of the active site. Due to CeO2’s excellent oxygen storage-release capacity, NH3 adsorption was weakened, in comparison to the 1 wt. % V2O5-0.2CeO2/TiO2-ZrO2 catalyst. If NOx were to be pre-adsorbed in the catalyst, the formation of nitrate and nitro species would be difficult to desorb, which would greatly hinder the SCR reaction. All the findings concluded that NH3-SCR worked mainly through the Eley-Rideal (E-R) mechanism.
Quantum confinement of a two-dimensional electron gas by supramolecular nanoporous networks is investigated using the boundary elements method based on Green's functions for finite geometries and electron plane wave expansion for periodic systems. The "particle in a box" picture was analyzed for cases with selected symmetries that model previously reported architectures constructed from organic and metal-organic scattering centers confining surface state electrons of Ag(111) and Cu(111). First, by analyzing a series of cases with systematically defined parameters (scattering geometry, potentials, and effective broadening), we demonstrate how the scattering processes affect the properties of the confined electrons. For the features of the local density of states reported by scanning tunneling spectroscopy (STS), we disentangle the contributions of lifetime broadening and splitting of quantum well states due to coupling of neighboring quantum dots. For each system, we analyze the local electron density distribution and relate it to the corresponding band structure as calculated within the plane-wave expansion framework. Then, we address two experimental investigations, where in one case only STS data and in the other case mainly angle-resolved photoemission spectroscopy (ARPES) data were reported. In both cases, the experimental findings can be successfully simulated. Furthermore, the missing information can be complemented because our approach allows to correlate the information obtained by STS with that of ARPES. The combined analysis of several observations suggests that the scattering potentials created by the network originate primarily from the adsorbate-induced changes of the local surface dipole barrier.
Analysis of metabolites is often performed using separations coupled to mass spectrometry which is challenging due to their vast structural heterogeneity and variable charge states. Metabolites are often separated based on their class/functional group which in large part determine their acidity or basicity. This charge state dictates the ionization mode and efficiency of the molecule. To improve the sensitivity and expand the coverage of the mammalian metabolome, multifunctional derivatization with sheathless CE-ESI-MS was undertaken. In this work, amines, hydroxyls and carboxylates were labeled with tertiary amines tags. This derivatization was performed in under 100 min and resulted in high positive charge states for all analytes investigated. Amino acids and organic acids showed average limits of detection of 76 nM with good linearity of 0.96 and 10% RSD for peak area. Applying this metabolomic profiling system to bovine aortic endothelial cells showed changes in 15 metabolites after treatment with high glucose. The sample injection volume on-capillary was <300 cells for quantitative analyses. Targeted metabolites were found in human tissue, which indicates possible application of the system complex metabolome quantitation.
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