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Robust Hydrogen Production via Pickering Interfacial Catalytic Photoreforming of n-Octanol-Water Biphasic System.

ABSTRACT: Pickering emulsion offers a promising platform for conducting interfacial reactions between immiscible reagents; it is particularly suitable for hydrogen production by photoreforming of non-water soluble biomass liquid and water. Herein, Pt-promoted (001)-facet-dominated anatase TiO₂ nanosheets were synthesized by a hydrothermal route associated with microfluidic technology for high activity and metal dispersion, and selective surface modification was carried out for preparing Janus particles. Photoreforming hydrogen production through n-octanol and water that formed O/W microemulsion with an average diameter of 540 µm was achieved to obtain amphiphilic catalyst. The as-prepared 2D Janus-type catalysts exhibited remarkably stable emulsification performance as well as photocatalytic activity. This finding indicates that triethoxyfluorosilane had negligible impact on the catalytic performance, yet provided a remarkable benefit to large specific surface area at microemulsion interface, thereby enhancing the H₂ yield up to 2003 μmol/g. The cyclic experiments indicate that the decrease in cyclic performance was more likely to be caused by the coalescence of the microemulsion rather than the decrease in catalytic activity, and the microemulsion could be easily recovered by simply hand shaking to more than 96% of the initial performance.

SUBMITTER: Wang C

PROVIDER: S-EPMC8339705 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Modulating Water Splitting Kinetics via Charge Transfer and Interfacial Hydrogen Spillover Effect for Robust Hydrogen Evolution Catalysis in Alkaline Media.

Project description:Designing and synthesizing advanced electrocatalysts with superior intrinsic activity toward hydrogen evolution reaction (HER) in alkaline media is critical for the hydrogen economy. Herein, a novel Ir@Rhene heterojunction electrocatalyst is synthesized via epitaxially confining ultrasmall and low-coordinate Ir nanoclusters on the ultrathin Rh metallene accompanying the formation of Ir/IrO2 Janus nanoparticles. The as-prepared heterojunctions display outstanding alkaline HER activity, with an overpotential of only 17 mV at 10 mA cm-2 and an ultralow Tafel slope of 14.7 mV dec-1 . Both structural characterizations and theoretical calculations demonstrate that the Ir@Rhene heterointerfaces induce charge density redistribution, resulting in the increment of the electron density around the O atoms in the IrO2 site and thus delivering much lower water dissociation energy. In addition, the dual-site synergetic effects between IrO2 and Ir/Rh interface trigger and improve the interfacial hydrogen spillover, thereby subtly avoiding the steric blocking of the active site and eventually accelerating the alkaline HER kinetics.

| S-EPMC10460870 | biostudies-literature

Hydrogen Production through Glycerol Photoreforming on TiO2/Mesoporous Carbon: Influence of the Synthetic Method.

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| S-EPMC7504067 | biostudies-literature

Hydrogen and Propane Production From Butyric Acid Photoreforming Over Pt-TiO<sub>2</sub>.

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Project description:In the present study, a novel catalytic route for the Knoevenagel condensation reaction has been developed by Pickering interfacial catalysis using magnesium oxide (MgO) as both an emulsion stabilizer and a base catalyst. MgO was prepared by the precipitation method using sodium hydroxide or ammonium hydroxide as the precipitating agent and calcined at different temperatures. The calcined samples were characterized by XRD, SEM, TEM, AFM, BET, and DLS techniques. The catalytic application of the emulsions stabilized by MgO was investigated for the Knoevenagel condensation reaction of benzaldehyde and its derivatives with malononitrile. All of the reactions were carried out at an ambient temperature (30 °C) under static conditions without stirring. Both the emulsion-stabilizing ability and the catalytic activity of MgO were found to be affected by the method of preparation, calcination temperature, and the nature of the oil phase. It was observed that the method of preparation varied the texture and morphology of MgO and thus the stability and droplet size of the emulsion formed. This was further reflected in the catalytic activity. The highest yield (87%) of the condensation product was obtained with MgO prepared by precipitation using a strong base (NaOH) and further calcined at 400 °C. The developed catalytic system offers several green chemistry advantages such as reusable solid-base catalyst and use of a single material as both emulsion stabilizer and catalyst. Room-temperature reaction under static conditions is an additional advantage of the developed catalytic system.

| S-EPMC7271354 | biostudies-literature

A Simple, Robust and Efficient Computational Method for n-Octanol/Water Partition Coefficients of Substituted Aromatic Drugs.

Project description:In this paper, multiple linear regression (MLR) was used to build quantitative structure property relationship (QSPR) of n-octanol-water partition coefficient (logPo/w) of 195 substituted aromatic drugs. The molecular descriptors were calculated for each compound by the VLifeMDS. By applying genetic algorithm/multiple linear regressions (GA/MLR) the most relevant descriptors were selected to build a QSPR model. The robustness of the model was characterized by the statistical validation and applicability domain (AD). The prediction results from MLR are in good agreement with the experimental values. The R2 and Q2LOO for MLR are 0.9433, 0.9341. The AD of the model was analyzed based on the Williams plot. The effects of different selected descriptors are described.

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Nanoscopic characterization of the water vapor-salt interfacial layer reveals a unique biphasic adsorption process.

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| S-EPMC4985642 | biostudies-literature

Interfacial electronic structure engineering on molybdenum sulfide for robust dual-pH hydrogen evolution.

Project description:Molybdenum disulfide, as an electronic highly-adjustable catalysts material, tuning its electronic structure is crucial to enhance its intrinsic hydrogen evolution reaction (HER) activity. Nevertheless, there are yet huge challenges to the understanding and regulation of the surface electronic structure of molybdenum disulfide-based catalysts. Here we address these challenges by tuning its electronic structure of phase modulation synergistic with interfacial chemistry and defects from phosphorus or sulfur implantation, and we then successfully design and synthesize electrocatalysts with the multi-heterojunction interfaces (e.g., 1T0.81-MoS2@Ni2P), demonstrating superior HER activities and good stabilities with a small overpotentials of 38.9 and 95 mV at 10 mA/cm2, a low Tafel slopes of 41 and 42 mV/dec in acidic as well as alkaline surroundings, outperforming commercial Pt/C catalyst and other reported Mo-based catalysts. Theoretical calculation verified that the incorporation of metallic-phase and intrinsic HER-active Ni-based materials into molybdenum disulfide could effectively regulate its electronic structure for making the bandgap narrower. Additionally, X-ray absorption spectroscopy indicate that reduced nickel possesses empty orbitals, which is helpful for additional H binding ability. All these factors can decrease Mo-H bond strength, greatly improving the HER catalytic activity of these materials.

| S-EPMC8421379 | biostudies-literature

Bifunctional Janus Silica Spheres for Pickering Interfacial Tandem Catalysis.

Project description:Nature provides much inspiration for the design of multistep conversion processes, with numerous reactions running simultaneously and without interference in cells, for example. A key challenge in mimicking nature's strategies is to compartmentalize incompatible reagents and catalysts, for example, for tandem catalysis. Here, we present a new strategy for antagonistic catalyst compartmentalization. The synthesis of bifunctional Janus catalyst particles carrying acid and base groups on the particle's opposite patches is reported as is their application as acid-base catalysts in oil/water emulsions. The synthesis strategy involved the use of monodisperse, hydrophobic and amine-functionalized silica particles (SiO2 -NH2 -OSi(CH3 )3 ) to prepare an oil-in-water Pickering emulsion (PE) with molten paraffin wax. After solidification, the exposed patch of the silica particles was selectively etched and refunctionalized with acid groups to yield acid-base Janus particles (Janus A-B). These materials were successfully applied in biphasic Pickering interfacial catalysis for the tandem dehydration-Knoevenagel condensation of fructose to 5-(hydroxymethyl)furfural-2-diethylmalonate (5-HMF-DEM) in a water/4-propylguaiacol PE. The results demonstrate the advantage of rapid extraction of 5-hydroxymethylfurfural (5-HMF), a prominent platform molecule prone to side product formation in acidic media. A simple strategy to tune the acid/base balance using PE with both Janus A-B and monofunctional SiO2 -NH2 -OSi(CH3 )3 base catalysts proved effective for antagonistic tandem catalysis.

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Epitaxial Hexagonal Boron Nitride for Hydrogen Generation by Radiolysis of Interfacial Water.

Project description:Hydrogen is an important building block in global strategies toward a future green energy system. To make this transition possible, intense scientific efforts are needed, also in the field of materials science. Two-dimensional crystals, such as hexagonal boron nitride (hBN), are very promising in this regard, as it has been demonstrated that micrometer-sized flakes are excellent barriers to molecular hydrogen. However, it remains an open question whether large-area layers fabricated by industrially relevant methods preserve such promising properties. In this work, we show that electron-beam-induced splitting of water creates hBN bubbles that effectively store molecular hydrogen for weeks and under extreme mechanical deformation. We demonstrate that epitaxial hBN allows direct visualization and monitoring of the process of hydrogen generation by radiolysis of interfacial water. Our findings show that hBN is not only a potential candidate for hydrogen storage but also holds promise for the development of unconventional hydrogen production schemes.

| S-EPMC9951249 | biostudies-literature

Cation Effects on Interfacial Water Structure and Hydrogen Peroxide Reduction on Pt(111).

Project description:The interface between the Pt(111) surface and several MeF/HClO4 (Me+ = Li+, Na+, or Cs+) aqueous electrolytes is investigated by means of cyclic voltammetry and laser-induced temperature jump experiments. Results point out that the effect of the electrolyte on the interfacial water structure is different depending on the nature of the metal alkali cation, with the values of the potential of maximum entropy (pme) following the order pme (Li+) < pme (Na+) < pme (Cs+). In addition, the hydrogen peroxide reduction reaction is studied under these conditions. This reaction is inhibited at low potentials as a consequence of the build up of negative charges on the electrode surface. The potential where this inhibition takes place (E inhibition) follows the same trend as the pme. These results evidence that the activity of an electrocatalytic reaction can depend to great extent on the structure of the interfacial water adlayer and that the latter can be modulated by the nature of the alkali metal cation.

| S-EPMC9836069 | biostudies-literature

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