Controllable Activation of ß-Alkyl Nitroalkenes: Regioselective Synthesis of Allyl and Vinyl Sulfones.

The regiospecific radical reactions of ß-alkyl nitroalkenes with sulfonyl hydrazides depended to a great extent on the choice of a solvent and catalyst. In the presence of dimethylformamide (DMF), ß-alkyl nitroalkenes more likely converted into electron-rich allyl nitro compounds, which reacted with sulfonyl hydrazides to afford allyl sulfones with high regioselectivity. While in acetonitrile (CH3CN), vinyl sulfones were obtained directly via sulfonation of electron-deficient ß-alkyl nitroalkenes. The mechanism investigation revealed that the regioselectivity was controlled by the equilibrium of ß-alkyl nitroalkenes and allyl nitro compounds.

Multimorbidity of Allergic Conditions in Urban Citizens of Southern China: A Real-World Cross-Sectional Study.

BACKGROUND: Extensive knowledge of allergic multimorbidities is required to improve the management of allergic diseases with the industrialization of China. However, the demography and allergen distribution patterns of allergic multimorbidities in China remain unclear, despite the increasing prevalence of allergies. METHODS: This was a real-world, cross-sectional study of 1273 outpatients diagnosed with one or more allergic diseases in Guangzhou, the most populated city of southern China, with leading industrial and commercial centers, between April 2021 and March 2022. Seven allergic diseases (allergic rhinitis (AR), asthma (AS)/cough variant asthma (CVA), atopic dermatitis (AD)/eczema, food allergy (FA), allergic conjunctivitis (AC), drug allergy (DA), and anaphylaxis) were assessed. Positive rates of sensitization to different allergens were measured using an allergen detection system of the UniCAP (Pharmacia Diagnostics, Sweden) instrument platform to compare the groups of allergic multimorbidities against a single entity. RESULTS: There were 659 (51.8%) males and 614 (48.2%) females aged from 4 months to 74 years included in the analysis. The study participants who were diagnosed with allergic diseases had an average of 1.6 diagnoses. Overall, 46.5% (592 of 1273) of the patients had more than one allergic condition, and allergic rhinitis was the most common type of multimorbidity. Women were more likely to suffer from an allergic disease alone, whereas allergic multimorbidities were more likely to be diagnosed in men (p = 0.005). In addition, allergic multimorbidities were common in all age groups, with an incidence ranging from 37.1% to 57.4%, in which children and adolescents were more frequently diagnosed with allergic multimorbidities than adults (18-60 years old) (all p < 0.05). Allergic multimorbidity was observed throughout the year. A difference in the positive rate of allergens sensitization and total immunoglobulin E (tIgE) levels between different allergic multimorbidities was observed. CONCLUSIONS: Allergic multimorbidities were very commonly found in nearly half of all patients with allergies. The proportion of allergic multimorbidities varied with the type of disease, sex, age, and allergen distribution pattern. These findings may help clinicians to develop "One health" strategies for the clinical management of allergic diseases.

Underfocus Laser Induced Ni Nanoparticles Embedded Metallic MoN Microrods as Patterned Electrode for Efficient Overall Water Splitting.

Transition metal nitrides have shown large potential in industrial application for realization of the high active and large current density toward overall water splitting, a strategy to synthesize an inexpensive electrocatalyst consisting of Ni nanoparticles embedded metallic MoN microrods cultured on roughened nickel sheet (Ni/MoN/rNS) through underfocus laser heating on NiMoO4 ·xH2 O under NH3 atmosphere is posited. The proposed laser preparation mechanism of infocus and underfocus modes confirms that the laser induced stress and local high temperature controllably and rapidly prepared the patterned Ni/MoN/rNS electrodes in large size. The designed Ni/MoN/rNS presents outstanding catalytic performance for hydrogen evolution reaction (HER) with a low overpotential of 67 mV to deliver a current density of 10 mA cm-2 and for the oxygen evolution reaction (OER) with a small overpotential of 533 mV to deliver 200 mA cm-2 . Density functional theory (DFT) calculations and Kelvin probe force microscopy (KPFM) further verify that the constructed interface of Ni/MoN with small hydrogen absorption Gibbs free energy (ΔGH* ) (-0.19 eV) and similar electrical conductivity between Ni and metallic MoN, which can explain the high intrinsic catalytic activity of Ni/MoN. Further, the constructed two-electrode system (-) Ni/MoN/rNS||Ni/MoN/rNS (+) is employed in an industrial water-splitting electrolyzer (460 mA cm-2 for 120 h), being superior to the performance of commercial nickel electrode.

Non-thermal radiation heating synthesis of nanomaterials.

The nanoscale effect enables the unique magnetic, optical, thermal and electrical properties of nanostructured materials and has attracted extensive investigation for applications in catalysis, biomedicine, sensors, and energy storage and conversion. The widely used synthesis methods, such as traditional hydrothermal reaction and calcination, are bulk heating processes based on thermal radiation. Differing from traditional heating methods, non-thermal radiation heating technique is a local heating mode. In this regard, this review summarizes various non-thermal radiation heating methods for synthesis of nanomaterials, including microwave heating, induction heating, Joule heating, laser heating and electron beam heating. The advantages and disadvantages of these non-thermal radiation heating methods for the synthesis of nanomaterials are compared and discussed. Finally, the future development and challenges of non-thermal radiation heating method for potential synthesis of nanomaterials are discussed.

A Universal Process: Self-Templated and Orientated Fabrication of XMoO4 (X: Ni, Co, or Fe) Nanosheets on MoO2 Nanoplates as Electrocatalysts for Efficient Water Splitting.

Fabrication of superior nonprecious electrocatalysts is essential for water electrolysis. Herein, the epitaxial growth of the XMoO4 (X = Ni, Co, Fe) nanosheets on the hexagonal MoO2 nanoplates are carried out. The preoxidation of MoO2 nanoplate is fatal to the epitaxial growth of a nanosheets array on MoO2 nanoplates. The hierarchical heterostructure of the vertically aligned NiMo nanosheets on MoO2 nanoplate (NiMo/MoO2) is well-maintained in the process of in situ topotactic reduction transformation from NiMoO4·xH2O/MoO2. Attributing it to the rich electroactive sites from nanosheets array, together with the intrinsic electrocatalytic performance of NiMo alloy, the as-engineered NiMo/MoO2 as electrocatalyst exhibits admirable hydrogen evolution reaction (HER) activity with a small onset potential of -12 mV vs RHE (1 mA cm-2) and a tafel value of 43.6 mV dec-1 at alkaline media. Furthermore, the obtained CoMoO4/MoO2 possesses excellent oxygen evolution performance, which is verified by an ultralow overpotential of 230 mV@10 mA cm-2, small Tafel slope (51 mV dec-1), and robust durability. The developed NiMo/MoO2 and CoMoO4/MoO2 electrocatalysts are assembled into an alkaline electrolyzer, which affords a cell potential of 1.51 V at 10 mA cm-2, as well as outstanding operational durability, which is superior to the typically constructed 20 wt % Pt/C-RuO2 system (1.59 V at 10 mA cm-2). Hence, the universal strategy using MoO2 nanoplates as Mo source and epitaxial substrate may be extended to explore and construct economical and superior Mo-based electrocatalysts for water electrolysis.

Charge Redistribution Caused by S,P Synergistically Active Ru Endows an Ultrahigh Hydrogen Evolution Activity of S-Doped RuP Embedded in N,P,S-Doped Carbon.

Water splitting for production of hydrogen as a clean energy alternative to fossil fuel has received much attention, but it is still a tough challenge to synthesize electrocatalysts with controllable bonding and charge distribution. In this work, ultrafine S-doped RuP nanoparticles homogeneously embedded in a N, P, and S-codoped carbon sheet (S-RuP@NPSC) is synthesized by pyrolysis of poly(cyclotriphosphazene-co-4,4'-sulfonyldiphenol) (PZS) as the source of C/N/S/P. The bondings between Ru and N, P, S in PZS are regulated to synthesize RuS2 (800 °C) and S-RuP (900 °C) by different calcination temperatures. The S-RuP@NPSC with low Ru loading of 0.8 wt% with abundant active catalytic sites possesses high utilization of Ru, the mass catalytic activity is 22.88 times than 20 wt% Pt/C with the overpotential of 250 mV. Density functional theory calculation confirms that the surface Ru (-0.18 eV) and P (0.05 eV) are catalytic active sites for the hydrogen evolution reaction (HER), and the according charge redistribution of Ru is regulated by S and P with reverse electronegativity and electron-donor property to induce a synergistically enhanced reactivity toward the HER. This work provides a rational method to regulate the bonding and charge distribution of Ru-based electrocatalysts by reacting macromolecules with multielement of C/N/S/P with Ru.

One-Step Sublimation and Epitaxial Growth of CdS-Cd Heterogeneous Nanoparticles on S-Doped MoO2 Nanosheets for Efficient Visible Light-Driven Photocatalytic H2 Generation.

As a green, pollution-free, and renewable clean energy source, photocatalytic H2 production has attracted great attention. Here, epitaxial growth of pyramidal CdS-Cd nanoparticles on S-doped MoO2 nanosheets (CdS-Cd/S-MoO2) was prepared by one-step co-sublimation of CdS and MoO3. The photogenerated electrons of CdS as a photocatalyst are transferred to Cd and S-MoO2 as co-catalysts for H2 production, which is observed by surface photovoltage (SPV) under visible light irradiation. At last, the obtained CdS-Cd/S-MoO2 presented an efficient photocatalytic performance under the visible light (>420 nm) with a prominent H2 generation rate of as high as 24.98 µmol h-1 mg-1, which is 11 times higher than that of the CdS-Cd nanoparticles (2.26 µmol h-1 mg-1), and it is superior than that of the CdS (1.51 µmol h-1 mg-1).