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A silver NP-dispersed water extract of fly ash as a green and efficient medium for oxidant-free dehydrogenation of benzyl alcohols.

ABSTRACT: Herein, a green, efficient, and new catalytic system for dehydrogenative oxidation of benzyl alcohols using Ag nanoparticles (NPs) dispersed in water extract of fly ash (WEFA) has been developed. Various characterization techniques were performed to authenticate the formation of Ag@WEFA. The as-prepared Ag NPs (10-20 nm) were found to be dispersed in WEFA, as indicated by transmission electron microscopy (TEM) and scanning electron microscopy (SEM) images. With Ag@WEFA, a variety of substituted benzyl alcohols were efficiently converted to carbonyl compounds in high yields. All the reactions were deliberately carried out without using any ligand or hazardous organic solvent. This catalytic system involving WEFA is a genuinely new concept. It is, therefore, expected to attract attention from researchers working in the areas of sustainable chemistry.

SUBMITTER: Bhuyan B

PROVIDER: S-EPMC9076987 | biostudies-literature | 2018 Jan

REPOSITORIES: biostudies-literature

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A silver NP-dispersed water extract of fly ash as a green and efficient medium for oxidant-free dehydrogenation of benzyl alcohols.

Bhuyan Bishal B Paul Arijita A Devi Meghali M Dhar Siddhartha Sankar SS

RSC advances 20180102 3

Herein, a green, efficient, and new catalytic system for dehydrogenative oxidation of benzyl alcohols using Ag nanoparticles (NPs) dispersed in water extract of fly ash (WEFA) has been developed. Various characterization techniques were performed to authenticate the formation of Ag@WEFA. The as-prepared Ag NPs (10-20 nm) were found to be dispersed in WEFA, as indicated by transmission electron microscopy (TEM) and scanning electron microscopy (SEM) images. With Ag@WEFA, a variety of substituted ...[more]

PMID: 35540896

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Project description:Fly ash (FA) fractions with a particle size of 63 µm < FA < 250 µm obtained by sieve fractionation were used as a partial carbon black (CB) replacement in a rubber mixture based on styrene-butadiene rubber (SBR). In order to improve the interactions at the interface between rubber and fractionated ash, at the stage of preparing the rubber mixtures, two different vinyl silanes were added to the system: Vinyltrimethoxysilane (U-611) or Vinyl-tris (2-methoxy-ethoxy) silane (LUVOMAXX VTMOEO DL50), silane with epoxy groups: 3-(glycidoxypropyl)trimethoxysilane (U-50) or sulfur functionalized silanes: containing sulfide bridges: Bis(triethoxysilylpropyl)polysulfide silane (Si-266) or mercapto groups: Mercaptopropyltrimethoxysilane (Dynaslan MTMO). The conducted research confirmed the effectiveness of silanization with selected functional silanes, from the point of view of improving the processing and operational properties of vulcanizates, in which CB is partially replaced with the finest fractions of fly ash. The silanization generally increased the interaction at the rubber-ash interface, while improving the degree of filler dispersion in the rubber mixture. The results of TGA and FTIR analyses confirmed the presence of silanes chemically bonded to the surface of fly ash particles. SEM tests and determination of the bound rubber (BdR) content show that the introduction of the silanes to the mixture increases the degree of ash dispersion (DI) and the Payne effect, which is the greatest when mercaptosilane was used for modification. The highest increase in torque, which was recorded in the case of rubber mixtures containing sulfur silanes and silane with epoxy groups, may be due to their participation in the vulcanization process, which is confirmed by the results of vulcametric studies. The lowest values of mechanical strength, elongation at break, and the highest hardness of vulcanizates obtained in this case may be the result of the over-crosslinking of the rubber. The addition of sulfur-containing silanes significantly slowed down the vulcanization process, which is particularly visible (up to three times extension of the t90 parameter, compared to mixtures without silane) in the case of Si-266. The addition of silanes, except for Si-266 (with a polysulfide fragment), generally improved the abrasion resistance of vulcanizates. The Dynaslan MTMO silane (with mercapto groups) performs best in this respect. Proper selection of silane for the finest fraction of fly ash in the rubber mixtures tested allows for an increase in the mechanical strength of their vulcanizates from 9.1 to 17 MPa, elongation at break from 290 to 500%, hardness from 68 to 74 °ShA, and reduction in abrasion from 171 to 147 mm3.

Project description:Solid/liquid heterogeneous photocatalysis was often considered to occur on the active sites of a solid catalyst surface. Herein, we report that the selectivity of photocatalytic dehydrogenative oxidations of aliphatic primary alcohols in acetonitrile solution into corresponding aldehydes exhibits an anomalous relationship with adsorption behavior of the alcohols. By using Pt-loaded TiO2 photocatalyst in an inert atmosphere under UV light illumination, primary short-chain alcohols (SCAs) with strong adsorption were dehydrogenated into aldehydes in very poor selectivity, whereas weak-adsorbable long-chain alcohols (LCAs) were transformed into corresponding aldehydes with much higher selectivity. More than 20 examples of primary LCAs (C4-C10) were successfully transformed into their corresponding aldehydes with satisfactory selectivity and yield. Both solid-state magic-angle-spinning 13C NMR and attenuated total reflectance-Fourier transform infrared spectroscopy studies provided concrete differences in adsorption behaviors on the Pt-TiO2 photocatalyst surface between SCA ethanol and LCA n-octanol. To further uncover the mechanism for different selectivities of SCAs and LCAs in photodehydrogenation, in situ electron paramagnetic resonance (EPR) experiments (at 8 K temperature) were employed to observe the oxidation features of photogenerated hole in the valance band of Pt-TiO2 (hvb +). The EPR experimental studies exhibited that unlike ethanol, either n-octanol or solvent acetonitrile alone all could not scavenge photogenerated hvb + on Pt-P25 photocatalyst and only n-octanol dissolved in acetonitrile solvent could smoothly react with photoinduced hole. This indicated that selective oxidations of LCAs were achieved by solvent-delivered oxidation rather than directly destructive oxidation of photogenerated hvb +. Our results may open an alternative way in selective dehydrogenative oxidation of various substrates sensitive to both dioxygen and high-temperature treatments.

Dataset Information

A silver NP-dispersed water extract of fly ash as a green and efficient medium for oxidant-free dehydrogenation of benzyl alcohols.

Publications

A silver NP-dispersed water extract of fly ash as a green and efficient medium for oxidant-free dehydrogenation of benzyl alcohols.

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