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1.
Wacker oxidation is an industry-adopted process to transform olefins into value-added epoxides and carbonyls. However, traditional Wacker oxidation involves the use of homogeneous palladium and copper catalysts for the olefin addition and reductive elimination. Here, we demonstrated an ultrahigh loading Cu single atom catalyst(14% Cu, mass fraction) for the palladium-free Wacker oxidation of 4-vinylanisole into the corresponding ketone with N-methylhydroxylamine hydrochloride as an additive under mild conditions. Mechanistic studies by 18O and deuterium isotope labelling revealed a hydrogen shift mechanism in this palladium-free process using N-methylhydroxylamine hydrochloride as the oxygen source. The reaction scope can be further extended to Kucherov oxidation. Our study paves the way to replace noble metal catalysts in the traditional homogeneous processes with single atom catalysts. 相似文献
2.
Kai Xu Zhenchang Tang Yan Zhang Wanshu Li Haiou Li Lihui Wang Liming Liu Honghang Wang Feng Chi Xiaowen Zhang 《Current Applied Physics》2019,19(10):1076-1081
Germanium dioxide (GeO2) aqueous solutions are facilely prepared and the corresponding anode buffer layers (ABLs) with solution process are demonstrated. Atomic force microscopy, X-ray photoelectron spectroscopy and ultraviolet photoelectron spectroscopy measurements show that solution-processed GeO2 behaves superior film morphology and enhanced work function. Using GeO2 as ABL of organic light-emitting diodes (OLEDs), the visible device with tris(8-hydroxy-quinolinato)aluminium as emitter gives maximum luminous efficiency of 6.5 cd/A and power efficiency of 3.5 lm/W, the ultraviolet device with 3-(4-biphenyl)-4-phenyl-5-tert-butylphenyl-1,2,4-triazole as emitter exhibits short-wavelength emission with peak of 376 nm, full-width at half-maximum of 42 nm, maximum radiance of 3.36 mW/cm2 and external quantum efficiency of 1.5%. The performances are almost comparable to the counterparts with poly (3,4-ethylenedioxythiophene):poly (styrenesulfonate) as ABL. The current, impedance, phase and capacitance as a function of voltage characteristics elucidate that the GeO2 ABL formed from appropriate concentration of GeO2 aqueous solution favors hole injection enhancement and accordingly promoting device performance. 相似文献
3.
4.
A rigorous and systematic intercomparison of codes used for the retrieval of trace gas profiles from high-resolution ground-based solar absorption FTIR measurements is presented for the first time. Spectra were analyzed with the two widely used independent, retrieval codes: SFIT2 and PROFFIT9. Vertical profiles of O3, HNO3, HDO, and N2O were derived from the same set of typical observed spectra. Analysis of O3 was improved by using updated line parameters. It is shown that profiles and total column amounts are in excellent agreement, when similar constraints are applied, and that the resolution kernel matrices are also consistent. Owing to the limited altitude resolution of ground-based observations, the impact of the constraints on the solution is not negligible. It is shown that the results are also compatible for independently chosen constraints. Perspectives for refined constraints are discussed. It can be concluded that the error budget introduced by the radiative transfer code and the retrieval algorithm on total columns deduced from high-resolution ground-based solar FTIR spectra is below 1%. 相似文献
5.
A formulation of an implicit characteristic-flux-averaging method for the unsteady Euler equations with real gas effects is presented. Incorporation of a real gas into a general equation of state is achieved by considering the pressure as a function of density and specific internal energy. The Ricmann solver as well as the flux-split algorithm are modified by introducing the pressure derivatives with respect to density and internal energy. Expressions for calculating the values of the flow variables for a real gas at the cell faces are derived. The Jacobian matrices and the eigenvectors are defined for a general equation of state. The solution of the system of equations is obtained by using a mesh-sequencing method for acceleration of the convergence. Finally, a test case for a simple form of equation of state displays the differences from the corresponding solution for an ideal gas. 相似文献
6.
In this work, a comparison of the interfacial electronic properties between a semiconducting oligomer and a variety of substrates with different properties—metal, semiconductor and oxide layers—is reported. The interface formation was studied by X-ray and Ultraviolet photoelectron spectroscopies (XPS, UPS). High purity oligomer films with thickness up to 10 nm were prepared by stepwise evaporation on the clean substrates under ultrahigh vacuum (UHV) conditions. Analysis of the oligomer and substrate related XPS spectra clarified the interfacial chemistry and band bending in the semiconducting materials. The valence band structure and the interfacial dipoles were determined by UPS. The barriers for hole injection were measured at the interfaces of the organic film with all substrates. The interfacial energy band diagrams were deduced in all cases from the combination of XPS and UPS results. Emphasis was given on the influence of the substrate work function (eΦ) on the electronic properties of these interfaces. 相似文献
7.
R. Resel M. Oehzelt O. Lengyel T.U. Schülli G. Hlawacek C. Teichert G. Koller 《Surface science》2006,600(19):4645-4649
A para-sexiphenyl monolayer of near up-right standing molecules (nominal thickness of 30 Å) is investigated in-situ by X-ray diffraction using synchrotron radiation and ex-situ by atomic force microscopy. A terrace like morphology is observed, the step height between the terraces is approximately one molecular length. The monolayer terraces, larger than 20 μm in size, are extended along the [0 0 1] direction of the TiO2(1 1 0) substrate i.e. along the Ti-O rows of the reconstructed substrate surface. The structure of the monolayer and its epitaxial relationship to the substrate is determined by grazing incidence X-ray diffraction. Extremely sharp diffraction peaks reveal high crystalline order within the monolayer, which was found to have the bulk structure of sexiphenyl. The monolayer terraces are epitaxially oriented with the (0 0 1) plane parallel to the substrate surface (out-of-plane order). Four epitaxial relationships are observed. This in-plane alignment is determined by the arrangement of the terminal phenyl rings of the sexiphenyl molecules parallel to the oxygen rows of the substrate. 相似文献
8.
We present a study of the growth kinetics of pentacene monolayer islands on SiO2 in the submonolayer regime by using Atomic Force Microscopy (AFM). Two distinct growth modes, namely correlated growth (CG) and non-correlated growth (NCG), have been identified by Voronoi tesselation. These two modes are characterized by different island growth kinetics. In the case of correlated growth, the average island size 〈A〉 scales with deposition time t i.e. 〈A〉 ∝ t whereas for non-correlated growth, 〈A〉 ∝ t2. The CG and NCG regimes are defined by the level of re-evaporation which determines the capture zones around the islands: Wigner-Seitz cells for CG and coronas of width λD (λD is the mean diffusion distance on SiO2 before re-evaporation) for NCG. A simple model is proposed to reproduce the experimental growth kinetics in both modes. 相似文献
9.
G. A. Kohring 《Journal of statistical physics》1992,66(3-4):1177-1184
A hydrodynamic cellular automata (HDCA) for simulating two-dimensional fluids with large viscosities is proposed. The model is characterized by a mean free path which is of the same size as in the FHP-II model, but with a viscosity more than 10 times larger. This new model should make simulations of flows at low Reynolds number more efficient. 相似文献
10.
V. E. Neuvazhaev I.É. Parshukov N. V. Pervinenko A. V. Ponomarev 《Journal of Applied Mechanics and Technical Physics》2004,45(5):656-664
Based on numerical calculations, the experiments on mixing at the interface of gases are analyzed. Single-mode and random disturbances of the interface and superposition of random disturbances onto long-wave perturbations are considered. Possible reasons for the higher value of the mixing constant obtained in the experiments are discussed. 相似文献