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1.
Ind Eng Chem Res ; 60(18): 6676-6686, 2021 May 12.
Artigo em Inglês | MEDLINE | ID: mdl-35308821

RESUMO

Several structured catalytic reactors for the direct synthesis of the DME reaction are compared with regard to catalyst hold-up, thermal conductivity, and volumetric productivity. Adherent and homogeneous catalyst layers were obtained by washcoating independent of the substrates' shape and alloy. Moreover, the substrate nature (FeCrAl, brass, or aluminum) and shape (parallel cell monoliths and open foams) do not modify in great extent the CO conversion values and selectivity to the different compounds. This is reasonable since the catalytic phases are the same in all cases and the existence of mass and heat-transfer limitations was negligible in the experimental conditions studied. Structuring by washcoating exhibits less catalyst inventory per reactor volume than a packed-bed monolith. However, completely packing a monolith with powder catalyst produced a decrease in the CO conversion of around 25% with respect to the coated monolith. Moreover, by means of using the obtained highest catalyst hold-up by washcoating (0.33 gcat/cm3) in a brass monolith and by increasing the reaction temperature, the temperature profiles are only slightly affected. This allows to work in an almost isothermal reactor with a volumetric productivity up to 0.20 LDME/h·cm3 at 573 K.

2.
RSC Adv ; 10(64): 38805-38817, 2020 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-35518418

RESUMO

The increasing amount of organic dye-polluted wastewater from the textile industry makes the development of techniques for the efficient purification and reuse of wastewater an urgent issue. Accordingly, solid adsorbents based on three-dimensional (3D) reduced graphene oxide (rGO) aerogels combined with magnetic nanoparticles (rGO@Fe3O4) appear to be potential materials, which offer fast and efficient discoloration of dye solutions by dye adsorption, simultaneously acting as Fenton reaction nanocatalysts, and thus may eliminate organic dyes. In this work, 3D rGO@Fe3O4 aerogel nanocatalysts were synthesized via a low-energy, simple, one-step in situ method, in which GO and FeSO4·7H2O were simultaneously reduced. Consequently, monolithic porous nanocatalyst 3D structures were obtained, with a specific surface area of 241 m2 g-1 and pore volume 0.39 cm3 g-1. The nanocatalysts were applied for the degradation of Acid Red 1 azo-dye in aqueous solution in the presence of hydrogen peroxide, without the need for external energy. The effect of the adsorbent dose, and concentration of dye and peroxide on the dye removal was studied. The degradation of the dye was monitored by matrix-assisted laser desorption/ionization time-of-flight mass spectrometry. It was found that an increase in the amount of peroxide allowed complete degradation of the dye together with high molar mass side-products with a conjugated aromatic structure. The good nanocatalyst performance was explained based on the charge-transfer complex established between rGO and the magnetic nanoparticles, allowing the regeneration of ferrous ions during the Fenton process.

3.
Angew Chem Int Ed Engl ; 56(24): 6946-6951, 2017 06 06.
Artigo em Inglês | MEDLINE | ID: mdl-28318084

RESUMO

Twisted two-dimensional aromatic frameworks have been prepared by overcrowding the nodes with bulky and rigid substituents. The highly distorted aromatic framework with alternating out-of-plane substituents results in diminished interlayer interactions that favor the exfoliation and dispersion of individual layers in organic media.

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