The Mars-Van Krevelen cycle and non-noble metal Ni jointly promoting Z-scheme charge transfer: a study on the photothermal synergy effect applied in selectively oxidizing aromatic alcohols.

Photothermal catalysis is a promising method for selectively oxidizing organic compounds, effectively addressing the energy-intensive and low-selective processes of thermal catalysis, as well as the slow reaction rates of photocatalysis. In this study, a ternary photothermal catalyst, Ni/CeO2/CdS, was synthesized using a simple calcination and solvothermal method. The catalyst demonstrated remarkable improvement in reaction rates and achieved nearly 100% selectivity in converting benzyl alcohol to benzaldehyde through photothermal catalysis at normal pressure. The reaction rates were 5.9 times and 63 times higher than those of CdS and Ni/CeO2 individually. XPS analysis confirmed that the thermal catalysis followed the Mars-Van Krevelen (MVK) mechanism and also proved that photocatalysis facilitated the MVK cycle. Additionally, DFT calculations showed that Ni acted as an electron transfer channel, facilitating efficient Z-scheme charge transfer. The in situ infrared technique was used to dynamically monitor the reaction process and explain the high selectivity of the product. Furthermore, detailed explanations of photocatalysis, thermocatalysis, and photothermal synergistic catalysis were proposed based on the aforementioned characterization and theoretical calculations. This approach establishes a theoretical foundation for the development of efficient photothermal catalysts.

Protective effect of FOXP3-mediated miR-146b-5p/Robo1/NF-κB system on lipopolysaccharide-induced acute lung injury in mice.

BACKGROUND: As a key transcription factor, forkhead box protein 3 (FOXP3) plays an important role in the development and function of natural cluster of differentiation 4 [CD4 (+)] regulatory T cells (Treg cells). However, the function of FOXP3 in Lipopolysaccharide (LPS)-induced acute lung injury (ALI) through regulating miR-146b-5p is unclear. This research aimed to disclose the regulatory effect of the FOXP3-mediated miR-146b-5p/Roundabout 1 (Robo1)/NF-κB system on LPS-induced ALI in mice. METHODS: The mice were subjected to 5 mg/kg of LPS via intratracheal instillation to induce ALI and generate the ALI model. Mice was divided into five group, including control group, ALI group, ALI + FOXP3 group, the ALI + miR antagomir group and ALI + miR antagomir+ FOXP3 group. Lung tissue injury were detected by hematoxylin and eosin (HE) staining. Lung wet/dry weight ratio, total cells in bronchoalveolar lavage fluid (BALF), total protein in BALF and the polymorphonuclear leukocyte (PMN) in BALF were detected. The levels of tumor necrosis factor-α (TNF-α), Interleukin 6 (IL-6) and IL-1ß were detected by enzyme-linked immunosorbent assay (ELISA) kit. The dual-luciferase reporter assay were used to detect the target relationship between FOXP3 and Robo1. Mice was divided into five group, including control group, ALI group, ALI + FOXP3 group, ALI + Robo1 group and ALI + FOXP3+ Robo1 group. The protein levels of FOXP3, Robo1 and p-p65 were detected by western bolt. The mRNA levels of miR-146b-5p and Robo1 were detected by quantitative reverse transcription polymerase chain reaction (qRT-PCR). RESULTS: Although protein expression levels of FOXP3 were significantly down-regulated in the ALI model, the increased FOXP3 levels promoted an increase in miR-146b-5p. Compared with the control group, the ALI model group exhibited severe histopathologic injury, such as thickening of the alveolar wall, pulmonary congestion, and decreased alveolar numbers. By mediating the overexpression of miR-146b-5p, FOXP3 also increased alveolar clearance and inhibited inflammatory responses in the ALI model. Importantly, Robo1 is a potential target of miR-146b-5p. CONCLUSIONS: FOXP3 could inhibit NF-κB activation, reduce lung pathological damage, and inhibit inflammatory responses by mediating the miR-146b-5p/Robo1/NF-κB system in the ALI model. These results may provide a new potential target for the treatment of ALI disease.

Ultra-low content of Pt modified CdS nanorods: Preparation, characterization, and application for photocatalytic selective oxidation of aromatic alcohols and reduction of nitroarenes in one reaction system.

A series of Pt nanoparticles (with size of 3-4 nm) decorated CdS nanorods were prepared via a simple solvothermal method. The samples were then used for photocatalytic selective oxidation (SO) of aromatic alcohols and reduction (SR) of nitroarenes in one reaction system. The platinized samples showed enhanced activity for the conversions than pristine CdS as Pt can serve as e- trapping and reaction sites, by which the recombination of photoinduced charge carriers can be suppressed and the adsorption of reactants and the SR of nitroarenes can be promoted. The sample loaded with only of 0.03% Pt showed the highest performance and, after irradiation for 4 h, the conversions of p-methoxybenzyl alcohol and nitrobenzene are as high as 92.7% and 94.8%, while the yields of p-methoxybenzaldehyde and aniline are 80.5% and 36.0%. The activities are about 2.0 times higher than that of CdS. The coupling reaction mechanism for the SO of aromatic alcohols to aldehydes and SR of nitroarenes to anilines in the reaction system was finally proposed.

Freeze the Moment: High Speed Capturing of Weakly Bonded Dynamic Nanoparticle Assemblies in Solution by Ag Ion Soldering.

Despite the versatile forms of colloidal aggregates, these spontaneously formed structures are often hard to find a suitable application in nanotechnology and materials science. A determinate reason is the lack of a suitable method to capture the transiently formed and quickly evolving colloidal structures in solution. To address this challenge, a simple but highly efficient strategy is herein reported to capture the dynamic and metastable colloidal assemblies formed in an aqueous or nonaqueous solution. This process takes advantage of a recently developed Ag ion soldering reaction to realize a rapid fixation of as-formed metastable assemblies. This method works efficiently for both solid (3D) nanoparticle aggregates and weakly bonded fractal nanoparticle chains (1D). In both cases, very high capturing speed and close to 100% efficiency are achieved to fully retain a quickly growing structure. The soldered nanochains further enable a fabrication of discrete, uniform, and functionalizable nanoparticle clusters with enriched linear conformation by mechanical shearing, which would otherwise be difficult to make. The captured products are water dispersible and mechanically robust, favoring an exploration of their properties toward possible applications. The work paves a way to previously untouched aspects of colloidal science and thus would create new chances in nanotechnology.

Pt supraparticles with controllable DNA valences for programmed nanoassembly.

Supraparticles are self-limiting nanoparticle ensembles with attractive properties from their unique hierarchical (primary and secondary) structures. Aiming at relieving the bottleneck of the very limited material building blocks in DNA nanotechnology, we herein demonstrate Pt-based supraparticles as catalytic materials for valence-controllable and high density DNA functionalizations toward DNA-programmed nanoassembly.

Hydrogel-derived non-precious electrocatalysts for efficient oxygen reduction.

The development of highly active, cheap and robust oxygen reduction reaction (ORR) electrocatalysts to replace precious metal platinum is extremely urgent and challenging for renewable energy devices. Herein we report a novel, green and especially facile hydrogel strategy to construct N and B co-doped nanocarbon embedded with Co-based nanoparticles as an efficient non-precious ORR catalyst. The agarose hydrogel provides a general host matrix to achieve a homogeneous distribution of key precursory components including cobalt (II) acetate and buffer salts, which, upon freeze-drying and carbonization, produces the highly active ORR catalyst. The gel buffer containing Tris base, boric acid and ethylenediaminetetraacetic acid, commonly adopted for pH and ionic strength control, plays distinctively different roles here. These include a green precursor for N- and B-doping, a salt porogen and a Co(2+) chelating agent, all contributing to the excellent ORR activity. This hydrogel-based process is potentially generalizable for many other catalytic materials.

Self-Assembly Synthesis of N-Doped Carbon Aerogels for Supercapacitor and Electrocatalytic Oxygen Reduction.

The rational design of high-performance and cheap nanomaterials for multiple sustainable energy storage applications is extremely urgent but remains challenging. Herein, a facile commercial melamine-sponge-directed multicomponent surface self-assembly strategy has been reported to synthesize N-doped carbon aerogels (NCAs) with low density (0.01 g cm(-3)), large open pores, and high surface area (1626 m2 g(-1)). The commercial melamine sponge simultaneously serves as a green N source for N-doping and a 3D scaffold to buffer electrolytes for reducing ion transport resistance and minimizing ion diffusion distance. With their tailored architecture characteristics, the NCAs-based supercapacitor and oxygen reduction electrocatalyst show excellent performance.