Regioselective Synthesis of Some New Pyrazolo[1,5‐a]pyrimidines,Pyrazolo[1,5‐a]quinazoline and Pyrimido[4′,5′:3,4]pyrazolo[1,5‐a] pyrimidines Containing Thiazole Moiety

A regioselective synthesis of novel pyrazolo[1,5‐a]pyrimidines, pyrazolo[1,5‐a]quinazoline and pyrimido[4′,5′:3,4]pyrazolo[1,5‐a]pyrimidines incorporating a thiazole moiety was described via the reactions of the versatile, readily accessible 5‐amino‐3‐(phenylamino)‐N‐(4‐phenylthiazol‐2‐yl)‐1H‐pyrazole‐4‐carboxamide 3 with appropriate 1,3‐biselectrophilic reagents namely, β‐diketones, enaminones, and α,β‐unsaturated cyclic ketone. The newly synthesized compounds were elucidated by elemental analysis, spectral data, and alternative synthetic route whenever possible.     

An explicit example of a noncrossed product division algebra

The paper presents an explicit example of a noncrossed product division algebra of index and exponent 8 over the field ?(s)(t). It is an iterated twisted function field in two variables D(x, σ)(y, τ ) over a quaternion division algebra D which is defined over the number field ?(√3,√?7). The automorphisms σ and τ are computed by solving relative norm equations in extensions of number fields. The example is explicit in the sense that its structure constants are known. Moreover, it is pointed out that the same arguments also yield another example, this time over the field ?((s))((t)), given by an iterated twisted Laurent series ring D((x, σ))((y, τ )) over the same quaternion division algebra D. (© 2004 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Bayesian unsupervised classification framework based on stochastic partitions of data and a parallel search strategy

Advantages of statistical model-based unsupervised classification over heuristic alternatives have been widely demonstrated in the scientific literature. However, the existing model-based approaches are often both conceptually and numerically instable for large and complex data sets. Here we consider a Bayesian model-based method for unsupervised classification of discrete valued vectors, that has certain advantages over standard solutions based on latent class models. Our theoretical formulation defines a posterior probability measure on the space of classification solutions corresponding to stochastic partitions of observed data. To efficiently explore the classification space we use a parallel search strategy based on non-reversible stochastic processes. A decision-theoretic approach is utilized to formalize the inferential process in the context of unsupervised classification. Both real and simulated data sets are used for the illustration of the discussed methods.     

Utilisation of customer feedback in a university hospital laboratory

The article describes the customer feedback system at a university hospital laboratory and the analysis of the feedback data from clinical customers in 2001–2006. The most common subject matters of the feedback were suspicion of the validity of laboratory results, delay in service and lacking test results, covering 82% of the 115 reports. The investigations of the cases revealed errors or defects in laboratory services in 81 cases. The most common errors or defects were erroneous test results (35 cases; 43%), delayed test results (24 cases; 30%) and lacking test results (15 cases; 18%). The most common underlying causes for a laboratory error or defect were unintended errors and non-compliance with operating instructions. Seventy-six percent of the feedback reports led to corrective actions. It is important to react to every instance of customer feedback and to find out possible errors or defects in the laboratory process. Uncovering the underlying causes makes adequate corrective and preventive actions possible.     

A comparison of time integration methods in an unsteady low‐Reynolds‐number flow

This paper describes three different time integration methods for unsteady incompressible Navier–Stokes equations. Explicit Euler and fractional‐step Adams–Bashford methods are compared with an implicit three‐level method based on a steady‐state SIMPLE method. The implicit solver employs a dual time stepping and an iteration within the time step. The spatial discretization is based on a co‐located finite‐volume technique. The influence of the convergence limits and the time‐step size on the accuracy of the predictions are studied. The efficiency of the different solvers is compared in a vortex‐shedding flow over a cylinder in the Reynolds number range of 100–1600. A high‐Reynolds‐number flow over a biconvex airfoil profile is also computed. The computations are performed in two dimensions. At the low‐Reynolds‐number range the explicit methods appear to be faster by a factor from 5 to 10. In the high‐Reynolds‐number case, the explicit Adams–Bashford method and the implicit method appear to be approximately equally fast while yielding similar results. Copyright © 2002 John Wiley & Sons, Ltd.     

Combined XPS and DFT investigation of the adsorption modes of methyl enol ether functionalized cyclooctyne on Si(001)

The reaction of methyl enol ether functionalized cyclooctyne on the silicon (001) surface was investigated by means of X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT). Three different groups of final states were identified; all of them bind on Si(001) via the strained triple bond of cyclooctyne but they differ in the configuration of the methyl enol ether group. The majority of molecules adsorbs without additional reaction of the enol ether group; the relative contribution of this configuration to the total coverage depends on substrate temperature and coverage. Further configurations include enol ether groups which reacted on the silicon surface either via ether cleavage or enol ether groups which transformed on the surface into a carbonyl group.     

A Neutral Silicon/Phosphorus Frustrated Lewis Pair

Frustrated Lewis pairs (FLPs) have a great potential for activation of small molecules. Most known FLP systems are based on boron or aluminum atoms as acid functions, few on zinc, and only two on boron‐isoelectronic silicenium cation systems. The first FLP system based on a neutral silane, (C₂F₅)₃SiCH₂P(tBu)₂ ( 1 ), was prepared from (C₂F₅)₃SiCl with C₂F₅ groups of very high electronegativity and LiCH₂P(tBu)₂. 1 is capable of cleaving hydrogen, and adds CO₂ and SO₂. Hydrogen splitting was confirmed by H/D scrambling reactions. The structures of 1 , its CO₂ and SO₂ adducts, and a decomposition product with CO₂ were elucidated by X‐ray diffraction.     

Surface Buckling and Subsurface Oxygen: Atomistic Insights into the Surface Oxidation of Pt(111)

Platinum is a catalyst of choice in scientific investigations and technological applications, which are both often carried out in the presence of oxygen. Thus, a fundamental understanding of platinum’s (electro)catalytic behavior requires a detailed knowledge of the structure and degree of oxidation of platinum surfaces in operando. ReaxFF reactive force field calculations of the surface energies for structures with up to one monolayer of oxygen on Pt(111) reveal four stable surface phases characterized by pure adsorbate, high‐ and low‐coverage buckled, and subsurface‐oxygen structures, respectively. These structures and temperature programmed desorption (TPD) spectra simulated from them compare favorably with and complement published scanning tunneling microscopy (STM) and TPD experiments. The surface buckling and subsurface oxygen observed here influence the surface oxidation process, and are expected to impact the (electro)catalytic properties of partially oxidized Pt(111) surfaces.