Iridium/graphene nanostructured catalyst for the N-alkylation of amines to synthesize nitrogen-containing derivatives and heterocyclic compounds in a green process.

A facile iridium/graphene-catalyzed methodology providing an efficient synthetic route for C-N bond formation is reported. This catalyst can directly promote the formation of C-N bonds, without pre-activation steps, and without solvents, alkalis and other additives. This protocol provides a direct N-alkylation of amines using a variety of primary and secondary alcohols with good selectivity and excellent yields. Charmingly, the use of diols resulted in intermolecular cyclization of amines, and such products are privileged structures in biologically active compounds. Two examples illustrate the advantages of this catalyst in organic synthesis: the tandem catalysis to synthesize hydroxyzine, and the intermolecular cyclization to synthesize cyclizine. Water is the only by-product, which makes this catalytic process sustainable and environmentally friendly.

Graphite Felt Modified by Atomic Layer Deposition with TiO2 Nanocoating Exhibits Super-Hydrophilicity, Low Charge-Transform Resistance, and High Electrochemical Activity.

Graphite felt (GF) is a multi-functional material and is widely used as electrodes of electrochemical devices for energy and environmental applications. However, due to the inherent hydrophobicity of graphite felt, it must be hydrophilically pretreated to obtain good electrochemical activity. Metal oxides coating is one of the feasible methods to modify the surface of GF, and in order to ensure that the metal oxides have a better conductivity for obtaining higher electrochemical activity, a subsequent H2 heat-treatment process is usually adopted. In this study, atomic layer deposition (ALD) is used to deposit TiO2 nanocoating on graphite felt (GF) for surface modification without any H2 thermal post-treatment. The results show that the ALD-TiO2-modified GF (ALD-TiO2/GF) owns excellent hydrophilicity. Moreover, the ALD-TiO2/GF exhibits excellent electrochemical properties of low equivalent series resistance (Rs), low charge-transfer resistance (Rct), and high electrochemical activity. It demonstrates that ALD is an applicable technique for modifying the GF surface. In addition, it can be reasonably imagined that not only TiO2 film can effectively modify the GF surface, but also other metal oxides grown by ALD with nanoscale-thickness can also obtain the same benefits. We anticipate this work to be a starting point for modifying GF surface by using ALD with metal oxides nanocoating.

A reduced graphene oxide-supported iridium nanocatalyst for selective transformation of alcohols into carbonyl compounds via a green process.

A nanocatalyst constructed from reduced graphene oxide and iridium atoms (RGOIrNc) showed high selectivity (99%-100%) and reliability for the transformation of aromatic alcohols into carbonyl compounds via ultrasonication without using harmful chemicals and solvents. Experimental data including Fourier transform infrared spectroscopy, x-ray diffraction, spherical-aberration-corrected field emission transmission electron microscopy and Raman spectra confirmed the nanostructure of the RGOIrNc. Noticeably, the structural characteristics of this catalyst remained unchanged within 25 catalytic cycles and the activity and selectivity for the transformation of benzylic alcohols showed good stability. The average turnover frequency is greater than 9000 h-1, the total turnover number is more than 150 000 after 25 catalytic cycles and the productivity of carbonyl compounds reaches 376 048 [Formula: see text], indicating that RGOIrNc catalyst has good durability and stability and high 'greenness'.

Graphene oxide-iridium nanocatalyst for the transformation of benzylic alcohols into carbonyl compounds.

A catalyst constructed from graphene oxide and iridium chloride exhibited high activity and reliability for the selective transformation of benzylic alcohols into aromatic aldehydes or ketones. Instead of thermal reaction, the transformation was performed under ultrasonication, a green process with low byproduct, high atomic yield and high selectivity. Experimental data obtained from spherical-aberration corrected field emission TEM (ULTRA-HRTEM), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy and Raman spectra confirm the nanostructure of the title complex. Noticeably, the activity and selectivity for the transformation of benzylic alcohols remained unchanged within 25 catalytic cycles. The average turn over frequency is higher than 5000 h-1, while the total turnover number (TON) is more than one hundred thousand, making it a high greenness and eco-friendly process for alcohol oxidation.

Structural, Magnetic, and Electronic Properties of Mixed Spinel NiFe2-xCrxO4 Nanoparticles Synthesized by Chemical Combustion.

A series of nickel-chromium-ferrite NiFe2-xCrxO4 (with x = 1.25) nanoparticles (NPs) with a cubic spinel structure and with size d ranging from 1.6 to 47.7 nm was synthesized by the solution combustion method. A dual structure of all phonon modes revealed in Raman spectra is associated with metal cations of different types present in the spinel lattice sites. Mössbauer spectra of small NPs exhibit superparamagnetic behavior. However, the transition into the paramagnetic state occurs at a temperature that is unusually high for small particles (TN is about 240 K in the d = 4.5 nm NPs). The larger NPs with d > 20 nm do not exhibit superparamagnetic properties up to the Neel temperature. From the magnetic and Mössbauer data, the cation occupation of the tetrahedral (A) and octahedral [B] sites was determined (Fe0.75Ni0.25)[Ni0.75Cr1.25]O4. The saturation magnetization MS in the largest NPs is about (0.98-0.95) µB, which is more than twice higher the value in bulk ferrite (Fe)[CrNi]O4. At low temperatures the total magnetic moment of the ferrite coincides with the direction of the B-sublattice moment. In the NPs with d > 20 nm, the compensation of the magnetic moments of A- and B-sublattices was revealed at about Tcom = 360-365 K. This value significantly exceeds the point Tcom in bulk ferrites NiFexCr2-xO4 (about 315 K) with the similar Cr concentration. However, in the smaller NPs NiFe0.75Cr1.25O4 with d ≤ 11.7 nm, the compensation effect does not occur. The magnetic anomalies are explained in terms of highly frustrated magnetic ordering in the B sublattice, which appears due to the competition of AFM and FM exchange interactions and results in a canted magnetic structure.

Community-associated methicillin-resistant Staphylococcus aureus necrotizing pneumonia in a healthy neonate.

The number of cases of community-associated methicillin-resistant Staphylococcus aureus (CA-MRSA) pneumonia has increased since the late 1990s, with skin and soft tissue infections predominant among neonates. Herein, we present a rare case of CA-MRSA necrotizing pneumonia with empyema following respiratory syncytial virus (RSV) infection in a healthy neonate. Despite prompt vancomycin treatment, the disease worsened and finally we had to perform pneumonectomy. This case highlights the possibility of emerging CA-MRSA-related invasive disease among neonates.

The influence of reconstruction algorithm and heart rate on coronary artery image quality and stenosis detection at 64-detector cardiac CT.

OBJECTIVE: We wanted to evaluate the impact of two reconstruction algorithms (halfscan and multisector) on the image quality and the accuracy of measuring the severity of coronary stenoses by using a pulsating cardiac phantom with different heart rates (HRs). MATERIALS AND METHODS: Simulated coronary arteries with different stenotic severities (25, 50, 75%) and different luminal diameters (3, 4, 5 mm) were scanned with a fixed pitch of 0.16 and a 0.35 second gantry rotation time on a 64-slice multidetector CT. Both reconstruction algorithms (halfscan and multisector) were applied to HRs of 40-120 beats per minute (bpm) at 10 bpm intervals. Three experienced radiologists visually assessed the image quality and they manually measured the stenotic severity. RESULTS: Fewer measurement errors occurred with multisector reconstruction (p = 0.05), a slower HR (p < 0.001) and a larger luminal diameter (p = 0.014); measurement errors were not related with the observers or the stenotic severity. There was no significant difference in measurements as for the reconstruction algorithms below an HR of 70 bpm. More nonassessable segments were visualized with halfscan reconstruction (p = 0.004) and higher HRs (p < 0.001). Halfscan reconstruction had better quality scores when the HR was below 60 bpm, while multisector reconstruction had better quality scores when the HR was above 90 bpm. For the HRs between 60 and 90 bpm, both reconstruction modes had similar quality scores. With excluding the nonassessable segments, both reconstruction algorithms achieved a similar mean measured stenotic severity and similar standard deviations. CONCLUSION: At a higher HR (above 90 bpm), multisector reconstruction had better temporal resolution, fewer nonassessable segments, better quality scores and better accuracy of measuring the stenotic severity in this phantom study.

The short-/intermediate-term changes in novel vascular inflammatory markers after angioplasty plus stenting in patients with symptomatic advanced systemic arterial diseases.

Studies on cell adhesion molecules and high-sensitivity C-reactive protein (hs-CRP) in systemic arterial diseases are limited in numbers and some results not consistent. It also remains undefined whether, for how long and to what extent these markers are perturbed after angioplasty. Patients with systemic arterial diseases admitted for percutaneous transluminal angioplasty (PTA) by standard procedures and techniques were prospectively studied. Fasting morning blood samples were collected to determine general biochemistry and relevant molecules by commercially available methods at baseline, 2 weeks and 3 months post-PTA/stenting. A group of equally numbered sex- and age-matched asymptomatic subjects without illness were selected as control. A total of 33 patients (28 M/5 F, aged 72 +/- 2 years) were recruited. Patients with systemic arterial disease had significantly higher baseline serum creatinine, circulating VCAM-1, ICAM-1, and hs-CRP, but lower p-selectin and HDL-C than control subjects. Except ICAM-1, cell adhesion molecules and hs-CRP levels were aroused significantly for at least 2 weeks after PTA/stenting, returned to baseline by 3 months, but p-selectin remained elevated beyond 3 months. ICAM-1 only showed a modest rise after PTA but the overall change was insignificant. In conclusion, cell adhesion molecules and hs-CRP did play a significant role in patients with advanced systemic arterial diseases who underwent PTA/stenting.