10 research outputs found

    SHIP1 DELETION ENHANCES ROS PRODUCTION AND DECREASES SURVIVAL OF THE S. AUREUS INFECTED MICE

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    Reactive oxygen species (ROS) production by neutrophils is essential for host innate immune defense. However, although ROS production is advantageous for killing various infectious organisms, excessive ROS can cause tissue damage. Thus, ROS production by neutrophils must be tightly controlled. In this study, we investigated a role for SH2 domain-containing inositol- 5-phosphatase 1 (SHIP1), a PtdIns(3,4,5)P3 phosphatase, in ROS production by neutrophils using ship1−/− mice. SHIP1 deletion enhanced ROS production as well as the bacterial killing capability of neutrophils. However, the ship1−/− mice showed decreases survival of the mice infected with Staphylococcus aureus (S. aureus). Our results suggest that SHIP1 controls appropriate host defenses against S. aureus infections in mice

    Effects of Surface Defects on Photocatalytic H<sub>2</sub>O<sub>2</sub> Production by Mesoporous Graphitic Carbon Nitride under Visible Light Irradiation

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    Photocatalytic production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) from ethanol (EtOH) and molecular oxygen (O<sub>2</sub>) was carried out by visible light irradiation (λ > 420 nm) of mesoporous graphitic carbon nitride (GCN) catalysts with different surface areas prepared by silica-templated thermal polymerization of cyanamide. On these catalysts, the photoformed positive hole oxidize EtOH and the conduction band electrons localized at the 1,4-positions of the melem unit promote two-electron reduction of O<sub>2</sub> (H<sub>2</sub>O<sub>2</sub> formation). The GCN catalysts with 56 and 160 m<sup>2</sup> g<sup>–1</sup> surface areas exhibit higher activity for H<sub>2</sub>O<sub>2</sub> production than the catalyst prepared without silica template (surface area: 10 m<sup>2</sup> g<sup>–1</sup>), but a further increase in the surface area (228 m<sup>2</sup> g<sup>–1</sup>) decreases the activity. In addition, the selectivity for H<sub>2</sub>O<sub>2</sub> formation significantly decreases with an increase in the surface area. The mesoporous GCN with larger surface areas inherently contain a larger number of primary amine moieties at the surface of mesopores. These defects behave as the active sites for four-electron reduction of O<sub>2</sub>, thus decreasing the H<sub>2</sub>O<sub>2</sub> selectivity. Furthermore, these defects also behave as the active sites for photocatalytic decomposition of the formed H<sub>2</sub>O<sub>2</sub>. Consequently, the GCN catalysts with relatively large surface area but with a small number of surface defects promote relatively efficient H<sub>2</sub>O<sub>2</sub> formation

    Graphitic Carbon Nitride Doped with Biphenyl Diimide: Efficient Photocatalyst for Hydrogen Peroxide Production from Water and Molecular Oxygen by Sunlight

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    Photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production from water and molecular oxygen (O<sub>2</sub>) by sunlight is a promising strategy for green, safe, and sustainable H<sub>2</sub>O<sub>2</sub> synthesis. We prepared graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) doped with electron-deficient biphenyl diimide (BDI) units by a simple calcination procedure. The g-C<sub>3</sub>N<sub>4</sub>/BDI catalyst, when photoirradiated by visible light (λ >420 nm) in pure water with O<sub>2</sub>, successfully promotes water oxidation by the photogenerated valence band holes and selective two-electron reduction of O<sub>2</sub> by the conduction band electrons, resulting in successful production of millimolar levels of H<sub>2</sub>O<sub>2</sub>. Electrochemical analysis, Raman spectroscopy, and ab initio calculation results revealed that, upon photoexcitation of the catalyst, the photogenerated positive holes are localized on the BDI unit while the conduction band electrons are localized on the melem unit. This spatial charge separation suppresses rapid recombination of the hole–electron pairs and facilitates efficient H<sub>2</sub>O<sub>2</sub> production. The solar-to-chemical energy conversion efficiency for H<sub>2</sub>O<sub>2</sub> production is 0.13%, which is comparable to that for photosynthetic plants. This metal-free photocatalysis therefore shows potential as an artificial photosynthesis for clean solar fuel production

    Mellitic Triimide-Doped Carbon Nitride as Sunlight-Driven Photocatalysts for Hydrogen Peroxide Production

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    Generating hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) from water and dioxygen (O<sub>2</sub>) by photocatalysis is one ideal artificial photosynthesis for solar fuel production. Several early reported powdered photocatalysts, however, produce small amounts of H<sub>2</sub>O<sub>2</sub> (<0.1 mM). We prepared graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) doped with mellitic triimide (MTI) units by thermal condensation of melem and mellitic acid anhydride. The g-C<sub>3</sub>N<sub>4</sub>/MTI photocatalyst, when irradiated by visible light (λ > 420 nm) in pure water with O<sub>2</sub>, successfully produces millimolar levels of H<sub>2</sub>O<sub>2</sub> via water oxidation by valence band holes and selective two-electron reduction of O<sub>2</sub> by conduction band electrons. The incorporation of triply branched MTI units creates a condensed melem layer. This facilitates efficient intra- and interlayer transfer of photogenerated charge carriers and shows high electrical conductivity. The solar-to-chemical conversion efficiency for H<sub>2</sub>O<sub>2</sub> production on the catalyst is 0.18%, which is higher than that of natural photosynthesis (∼0.1%) and similar to the highest values obtained by semiconductor water-splitting catalysts

    Carbon Nitride–Aromatic Diimide–Graphene Nanohybrids: Metal-Free Photocatalysts for Solar-to-Hydrogen Peroxide Energy Conversion with 0.2% Efficiency

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    Solar-to-chemical energy conversion is a challenging subject for renewable energy storage. In the past 40 years, overall water splitting into H<sub>2</sub> and O<sub>2</sub> by semiconductor photocatalysis has been studied extensively; however, they need noble metals and extreme care to avoid explosion of the mixed gases. Here we report that generating hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) from water and O<sub>2</sub> by organic semiconductor photocatalysts could provide a new basis for clean energy storage without metal and explosion risk. We found that carbon nitride–aromatic diimide–graphene nanohybrids prepared by simple hydrothermal–calcination procedure produce H<sub>2</sub>O<sub>2</sub> from pure water and O<sub>2</sub> under visible light (λ > 420 nm). Photoexcitation of the semiconducting carbon nitride–aromatic diimide moiety transfers their conduction band electrons to graphene and enhances charge separation. The valence band holes on the semiconducting moiety oxidize water, while the electrons on the graphene moiety promote selective two-electron reduction of O<sub>2</sub>. This metal-free system produces H<sub>2</sub>O<sub>2</sub> with solar-to-chemical energy conversion efficiency 0.20%, comparable to the highest levels achieved by powdered water-splitting photocatalysts

    Rapamycin-sensitive mechanisms confine the growth of fission yeast below the temperatures detrimental to cell physiology

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    Summary: Cells cease to proliferate above their growth-permissible temperatures, a ubiquitous phenomenon generally attributed to heat damage to cellular macromolecules. We here report that, in the presence of rapamycin, a potent inhibitor of Target of Rapamycin Complex 1 (TORC1), the fission yeast Schizosaccharomyces pombe can proliferate at high temperatures that usually arrest its growth. Consistently, mutations to the TORC1 subunit RAPTOR/Mip1 and the TORC1 substrate Sck1 significantly improve cellular heat resistance, suggesting that TORC1 restricts fission yeast growth at high temperatures. Aiming for a more comprehensive understanding of the negative regulation of high-temperature growth, we conducted genome-wide screens, which identified additional factors that suppress cell proliferation at high temperatures. Among them is Mks1, which is phosphorylated in a TORC1-dependent manner, forms a complex with the 14-3-3 protein Rad24, and suppresses the high-temperature growth independently of Sck1. Our study has uncovered unexpected mechanisms of growth restraint even below the temperatures deleterious to cell physiology

    Nitrogen Fixation with Water on Carbon-Nitride-Based Metal-Free Photocatalysts with 0.1% Solar-to-Ammonia Energy Conversion Efficiency

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    Ammonia (NH<sub>3</sub>), which is an indispensable chemical, is produced by the Haber–Bosch process using H<sub>2</sub> and N<sub>2</sub> under severe reaction conditions. Although photocatalytic N<sub>2</sub> fixation with water under ambient conditions is ideal, all previously reported catalysts show low efficiency. Here, we report that a metal-free organic semiconductor could provide a new basis for photocatalytic N<sub>2</sub> fixation. We show that phosphorus-doped carbon nitride containing surface nitrogen vacancies (PCN-V), prepared by simple thermal condensation of the precursors under H<sub>2</sub>, produces NH<sub>3</sub> from N<sub>2</sub> with water under visible light irradiation. The doped P atoms promote water oxidation by the photoformed valence-band holes, and the N vacancies promote N<sub>2</sub> reduction by the conduction-band electrons. These phenomena facilitate efficient N<sub>2</sub> fixation with a solar-to-chemical conversion (SCC) efficiency of 0.1%, which is comparable to the average solar-to-biomass conversion efficiency of natural photosynthesis by typical plants. Thus, this metal-free catalyst shows considerable potential as a new method of artificial photosynthesis
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