Aerobic oxidation of alcohols over hydrotalcite-supported gold nanoparticles: the promotional effect of transition metal cations

Chromium (III)-containing hydrotalcites show strong synergy with gold nanoparticles in achieving high activity in the aerobic oxidation of alcohols.     

Improving background suppression in diffusion-weighted imaging of the abdomen and pelvis using STIR with single-axis diffusion encoding

Bowel contents and peripheral nerves often show high signal intensity at diffusion-weighted imaging (DWI) of the abdomen and pelvis, obscuring or mimicking pathology. This study introduced and compared short tau inversion recovery (STIR) with single-axis DWI to the usual combination of spectral fat suppression (SFS) with trace DWI in the suppression of bowel contents and peripheral nerves. Five volunteers underwent both STIR with single-axis DWI and SFS with trace DWI of the abdomen and pelvis. Images were evaluated by two observers with respect to the suppression of signal of bowel contents and peripheral nerves using four-point grading scales (4=poor suppression; 3=moderate suppression; 2=good suppression; 1=excellent suppression). Mean scores (±S.D.) regarding the suppression of bowel contents were 1.60±0.55 and 1.40±0.89 for STIR with single-axis DWI and 3.40±0.55 and 3.00±1.00 for SFS with trace DWI for observers 1 and 2, respectively. Mean scores regarding the suppression of peripheral nerves were 1.20±0.45 and 1.20±0.45 for STIR with single-axis DWI and 2.40±0.89 and 2.80±0.84 for SFS with trace DWI for observers 1 and 2, respectively. In conclusion, STIR with single-axis DWI is superior to SFS with trace DWI in the suppression of bowel signal and peripheral nerves.     

Computational aspects of satisfiability in probability logic

We consider the complexity of satisfiability in ε‐logic, a probability logic. We show that for the relational fragment this problem is ‐complete for rational , answering a question by Terwijn. In contrast, we show that satisfiability in 0‐logic is decidable. The methods we employ to prove this fact also allow us to show that 0‐logic is compact, while it was previously shown that ε‐logic is not compact for .     

Understanding the reactivity and basicity of zeolites: a periodic DFT study of the disproportionation of N(2)O(4) on alkali-cation-exchanged zeolite Y

The disproportionation of N(2)O(4) into NO(3)(-) and NO(+) on Y zeolites has been studied through periodic DFT calculations to unravel 1) the role of metal cations and the framework oxygen atoms and 2) the relationship between the NO(+) stretching frequency and the basicity of zeolites. We have considered three situations: adsorption on site II cations with and without a cation at site III and adsorption on a site III cation. We observed that cations at sites II and III cooperate to stabilize N(2)O(4) and that the presence of a cation at site III is necessary to allow the disproportionation reaction. The strength of the stabilization is due to the number of stabilizing interactions increasing with the size of the cation and to the Lewis acidity of the alkali cations, which increases as the size of the cations decreases. In the product, NO(3)(-) interacts mainly with the cations and NO(+) with the basic oxygen atoms of the tetrahedral aluminium through its nitrogen atom. As the cation size increases, the NO(3)(-)...cation interaction increases. As a result, the negative charge of the framework is less well screened by the larger cations and the interaction between NO(+) and the basic oxygen atoms becomes stronger. NO(+) appears to be a good probe of zeolite basicity, in agreement with experimental observations.     

N,N-acetals as N-acyliminium ion precursors: synthesis and absolute stereochemistry of epiquinamide

A stereoselective synthesis of (+)-epiquinamide is presented in combination with determination of the absolute configuration of the natural product. Key steps in the sequence involved chemoenzymatic formation of an enantiomerically pure cyanohydrin, reductive cyclization to the corresponding cyclic N,N-acetal, and subsequent conversion into a suitable N-acyliminium ion precursor to enable construction of the second ring.     

Kinetics of the Fischer-tropsch reaction

Long carbon chains: Self-assembly of monomeric carbon intermediates into long-chain hydrocarbons on catalytically reactive surface was studied when full reversibility of the chain growth is included in the kinetic model. Using Br?nsted-Evans-Polanyi relations, the maximum chain growth as a function of the surface reactivity is predicted.     

Real-time sizing of nanoparticles in microfluidic channels using confocal correlation spectroscopy

This Communication reports real-time sizing of nanoparticles in microfluidic systems using confocal correlation spectroscopy (CCS). CCS can be used to measure the size of both fluorescent and nonfluorescent particles at low concentrations (相似文献   

Hollow silica spheres with an ordered pore structure and their application in controlled release studies

Herein we report the synthesis and characterization of hollow silica spheres with a narrow size distribution, uniform wall thickness, and a worm-like pore structure. The formation of these spheres was monitored by confocal laser scanning microscopy and dynamic light scattering. A model for the molecular build-up of these silica hollow spheres is derived from these data in combination with studies of the as-made particles by transmission electron microscopy, scanning electron microscopy, pore size analysis, thermogravimetric analysis, and solid-state nuclear magnetic resonance. We further demonstrate that these spheres can be used for the encapsulation and subsequent release of different dye molecules.