Metal Single-Atom Cocatalyst on Carbon Nitride for the Photocatalytic Hydrogen Evolution Reaction: Effects of Metal Species

Single-atom (SA) catalysts exhibit high activity in various reactions because there are no inactive internal atoms. Accordingly, SA cocatalysts are also an active research fields regarding photocatalytic hydrogen (H₂) evolution which can be generated by abundant water and sunlight. Herein, it is investigated whether 10 transition metal elements can work as an SA on graphitic carbon nitride (g-C₃N₄; i.e., gCN), a promising visible-light-driven photocatalyst. A method is established to prepare SA-loaded gCN at high loadings (weight of ≈3 wt.% for Cu, Ni, Pd, Pt, Rh, and Ru) by modulating the photoreduction power. Regarding Au and Ag, SAs are formed with difficulty without aggregation because of the low binding energy between gCN and the SA. An evaluation of the photocatalytic H₂-evolution activity of the prepared metal SA-loaded gCN reveals that Pd, Pt, and Rh SA-loaded gCN exhibits relatively high H₂-evolution efficiency per SA. Transient absorption spectroscopy and electrochemical measurements reveal the following: i) Pd SA-loaded gCN exhibits a particularly suitable electronic structure for proton adsorption and ii) therefore they exhibit the highest H₂-evolution efficiency per SA than other metal SA-loaded gCN. Finally, the 8.6 times higher H₂-evolution rate per active site of Pd SA is achieved than that of Pd-nanoparticles cocatalyst.     

Multihormone-producing islet cell tumor of the pancreas associated with somatostatin-immunoreactive amyloid: immunohistochemical and immunoelectron microscopic studies

OBJECTIVE: To assess the association between high but nondiabetic blood glucose levels and the risk of death from all causes, coronary heart disease (CHD), cardiovascular disease, and neoplasms. RESEARCH DESIGN AND METHODS: We studied the 20-year mortality of non-diabetic, working men, age 44-55 years, in three European cohorts known as the Whitehall Study (n = 10,025), the Paris Prospective Study (n = 6,629), and the Helsinki Policeman Study (n = 631). These men were identified by their 2-h glucose levels following an oral glucose tolerance test and by the absence of a prior diagnosis of diabetes. As the protocol for the oral glucose tolerance test and methods for measuring glucose differed between studies, mortality was analyzed according to the percentiles of the 2-h and fasting glucose distributions, using the Cox's proportional hazards model. RESULTS: Men in the upper 20% of the 2-h glucose distributions and those in the upper 2.5% for fasting glucose had a significantly higher risk of all-cause mortality in comparison with men in the lower 80% of these distributions, with age-adjusted hazard ratios of 1.6 (95% CI 1.4-1.9) and 2.0 (1.6-2.6) for the upper 2.5%. For death from cardiovascular and CHD, men in the upper 2.5% of the 2-h and fasting glucose distributions were at higher risk, with age-adjusted hazard ratios for CHD of 1.8 (1.4-2.4) and 2.7 (1.7-4.4), respectively. CONCLUSIONS: If early intervention aimed at lowering blood glucose concentrations can be shown to reduce mortality, it may be justified to lower the levels of both 2-h and fasting glucose, which define diabetes.     

The ultrastructure of the lens capsule abnormalities in Alport''s syndrome

Chronic overexpression of the neurite growth-promoting factor S100beta has been implicated in the pathogenesis of neuritic plaques in Alzheimer's disease. Such plaques are virtually universal in middle-aged Down's syndrome, making Down's a natural model of Alzheimer's disease. We determined numbers of astrocytes overexpressing S100beta, and of neurons overexpressing beta-amyloid precursor protein (beta-APP), and assayed for neurofibrillary tangles in neocortex of 20 Down's syndrome patients (17 weeks gestation to 68 years). Compared to controls, there were twice as many S100beta-immunoreactive (S100beta+) astrocytes in Down's patients at all ages: fetal, young, and adult (p = 0.01, or better, in each age group). These were activated (i.e., enlarged), and intensely immunoreactive, even in the fetal group. There were no neurofibrillary changes in fetal or young Down's patients. The numbers of S100beta+ astrocytes in young and adult Down's patients correlated with the numbers of neurons overexpressing beta-APP (p < 0.05). Our findings are consistent with the idea that conditions--including Down's syndrome--that promote chronic overexpression of S100beta may confer increased risk for later development of Alzheimer's disease.     

Pinning of Dislocation Motion in bcc Solid 3He

We have measured the dissipation of dislocation motion in bcc solid ³ He using the high-Q torsional oscillator technique at 1079 Hz. We observed a broad maximum in the temperature dependence of the dissipation. The maximum of the dissipation can be explained by the theory of Granato and Lucke in which the dislocation mobility depends upon the interactions of dislocations with point defects. ⁴ He impurities tend to bind to the dislocation lines at low temperatures and pin this dislocation motion. The maximum of the dissipation corresponds to the depinning of the dislocation motion. From the amplitude dependence of the depinning temperature we first obtained the activation energy of 1.03 K of the impurity ⁴ He atom trapped on the dislocations in bcc solid ³ He at a molar volume of 24.30 cm ³ /mol. The activation energy of the impurity atom in bcc ³ He was found to be larger than the value of 0.7 Kin hcp ⁴ He.     

Site-specific lead distribution in scales of lead-administered carp (Cyprinus carpio) by non-destructive SR-XRF analysis

By utilizing non-destructive synchrotron radiation-excited X-ray fluorescence (SR-XRF), we observed the distribution of lead (Pb) in both ontogenic and regenerating scales of lead-administrated carp, Cyprinus carpio. The fish in the Pb-administered group were fed pellets containing 1 mg/g of Pb at a rate of 1.5% body weight per day for 30 days. In the ontogenic scales, Pb was highly accumulated near the basal edge of the scale and the accumulated amount decreased toward the focus of the scale. On the other hand, in the regenerating scales, high accumulation was observed near the basal edge and the accumulated amount remained high toward the focus. The present results of Pb accumulation correspond well with the region which is calcifying in the ontogenic and regenerating scales, and indicate that the distributions of Pb show when and how long Pb was administered.     

Dislocation Motion in bcc Solid 3He

We have measured the shear modulus of bcc solid ³ He at 827 Hz using the high- Q torsional oscillator technique. We observed a decrease in the shear modulus from the low-temperature value G₀ to about 0.4G₀ at a molar volume of 24.80 cm ³/mole and to 0.6G₀ at 24.32 cm ³/mole near the melting point. The reduction of an effective shear modulus is explained by the dislocation theory of Granato and Lücke.     

Accurate probe-response calculation in eddy current NDE by finite element method

A method is presented to evaluate flaw signals in eddy current NDE using the finite element technique. The analysis of the electromagnetic field is based on a three-dimensional finite element scheme that computes directly the electromagnetic field distortions due to defects. This direct field-distortion calculation together with an accurate unflawed field calculation provides accurate total field values in general three-dimensional geometries. The paper shows that the application of the reaction concept and the reciprocity theory allows computations of the probe responses by performing integrals over the flaw region only, even if the analysis is performed by a finite element scheme. Two benchmark problems—a plate with rectangular slot scanned by a differential probe and a tube with axial and circumferential slots scanned by an absolute probe—have been solved to demonstrate the validity and the efficiency of the method. The calculated probe responses show good agreement with the measured trajectories. In order to reach better quantitative agreement, a calibration algorithm that adjusts the parameters of the cylindrical coil model and the lift-off within the range of the geometrical tolerances has been developed.     

Calculation of Grain-Boundary Bonding in Rare-Earth-Doped β-Si3N4

First-principles molecular orbital calculations are performed by the discrete variational Xalpha method using model clusters of rare-earth-doped β-Si₃N₄ and the interface between prismatic planes of β-Si₃N₄ and intergranular glassy films. On the basis of the total overlap population of each cluster, the rare-earth ions are implied to be stable in the grain-boundary model, while they are not stable in the bulk model. These results are consistent with experimental observations showing significant segregation of Ln³⁺ ions at the grain boundary and no solubility of Ln³⁺ into bulk β-Si₃N₄. Grain-boundary bonding is weakened with an increase of the ionic radius of the rare-earth ions, which provides a reasonable explanation for the ionic size dependence of the crack propagation behaviors as well as the growth rate of the prismatic plane in the rare-earth-doped β-Si₃N₄ during liquid-phase sintering.