59 research outputs found
Ferrosilicate-Based Heterogeneous Fenton Catalysts: Influence of Crystallinity, Porosity, and Iron Speciation
Different ferrosilicate samples have been prepared with varying degrees of crystallinity, porous texture, and speciation of the Fe sites by both hydrothermal and solâgel procedures: Fe-silicalite-1 with microcrystals (2â10 ”m) and nanocrystals (180 nm), Fe-containing composite material consisting of silicalite-1 and amorphous silica, and two samples of mesoporous Fe-containing amorphous silica FeâSiO2. The resulting solids have been tested for their potential as organic pollutants removal under Fenton-like conditions in heterogeneous catalytic wet peroxide oxidation of phenol and clarithromycin lactobionate. Our results indicate that the three aforementioned parameters show a strong interplay towards the abatement of pollutants in liquid phase. Thus, samples with high crystallinity show an improved performance in the oxidation of organic contaminants over amorphous samples in which the Fe speciation is very well controlled.The work was financially supported by the Ministry of Education and Science of the Russian Federation (RFMEFI60417âXâ0159, title of the agreement: âDevelopment of methods for hydrotreating of vacuum residue into high-quality marine fuels on macroporous catalystsâ). The authors from Spanish side thank the Spanish Ministry of Economy and Competitiveness (MINECO), Generalitat Valenciana and FEDER (CTQ2015-66080-R MINECO/FEDER and PROMETEOII/2014/010) for financial support. J.G.A. thanks the Spanish Ministry of Economy and Competitiveness (MINECO) for his fellowship (BES-2013-063678)
Establishing ZIF-8 as a reference material for hydrogen cryoadsorption: An interlaboratory study
Hydrogen storage by cryoadsorption on porous materials has the advantages of low material cost, safety, fast kinetics, and high cyclic stability. The further development of this technology requires reliable data on the H2 uptake of the adsorbents, however, even for activated carbons the values between different laboratories show sometimes large discrepancies. So far no reference material for hydrogen cryoadsorption is available. The metal-organic framework ZIF-8 is an ideal material possessing high thermal, chemical, and mechanical stability that reduces degradation during handling and activation. Here, we distributed ZIF-8 pellets synthesized by extrusion to 9 laboratories equipped with 15 different experimental setups including gravimetric and volumetric analyzers. The gravimetric H2 uptake of the pellets was measured at 77â
K and up to 100â
bar showing a high reproducibility between the different laboratories, with a small relative standard deviation of 3â4 % between pressures of 10â100â
bar. The effect of operating variables like the amount of sample or analysis temperature was evaluated, remarking the calibration of devices and other correction procedures as the most significant deviation sources. Overall, the reproducible hydrogen cryoadsorption measurements indicate the robustness of the ZIF-8 pellets, which we want to propose as a reference material.M. Maiwald, J.â
A. Villajos, R. Balderas and M. Hirscher acknowledge the EMPIR programme from the European Union's Horizon 2020 research and innovation programme for funding. F. Cuevas and F. Couturas acknowledge support from France 2030 program under project ANR-22-PEHY-0007. D. Cazorla and A. Berenguer-Murcia thank the support by PID2021-123079OB-I00 project funded by MCIN/AEI/10.13039/501100011033, and âERDF A way of making Europeâ. K.â
N. Heinselman, S. Shulda and P.â
A. Parilla acknowledge the support from the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. Funding provided by U.S. Department of Energy Office of Energy Efficiency and Renewable Energy Hydrogen and Fuel Cell Technology Office through the HyMARC Energy Materials Network
Gold supported on mesoporous titania thin films for application in microstructured reactors in low-temperature water-gas shift reaction
Au (1 wt.%)/TiO2 catalytic thin films were prepared on a surface-modified titanium substrate for application in a water-gas shift (WGS) microstructured reactor. Au-containing mesoporous titania films were synthesized using Pluronic 127 surfactant as a structure directing agent and titanium tetrabutoxide as titania source. Colloidal gold nanoparticles of 4 nm diameter were added to the synthesis sol prior to spin-coating. The resulting thin films were characterized by X-ray diffraction, transmission electron microscopy, ethanol adsorptionâdesorption isotherms and spectroscopic ellipsometry. Catalytic activity and selectivity were measured for the WGS reaction at temperatures between 220 and 290 °C. The reaction rate measured at CO conversions of below 10% was similar to that reported for gold supported on mesoporous titania and on ceria modified mesoporous titania pelletized catalysts prepared via depositionâprecipitation
Thin catalytic coatings on microreactor walls A way to make industrial processes more efficient
Current trends in the development of microstructured reactors with thin catalytic films (from 100 nm up to several microns) that have self-assembled nanostructures are discussed. A major technique that is used to prepare such films is sol-gel processing. This involves depositing a complex fluid on a microstructured substrate by dip, spin, or spray coating, followed by surfactant removal to form the porous nanostructures. A novel methodology has been developed by which a uniform coating containing controlled amounts of (poly)metallic nanoparticles can be obtained. This elegant strategy is based on the condensation of metal oxide species by self-assembly in the presence of metallic colloids. The potential microreactor applications brought forth by this innovative protocol are placed in perspective in the light of its versatility
Wall coated capillary microreactors with confined metallic nanoparticles for chemicals synthesis
No abstract
Selective hydrogenation of phenylacetylene to styrene on a Pd/TiO2 coating in a microreactor
The selective hydrogenation of phenylacetylene to styrene by hydrogen was studied in the 25-50 oC temperature range in a continuous flow microchannel of 250 ”m i.d. with a Pd supported on mesoporous TiO2 catalyst. The inner wall of the microreactor was dip-coated with a prehydrolyzed titania precursor solution containing an EOxPOyEOx amphiphilic triblock copolymer (EO = ethylene oxide, PO = propylene oxide, x = 106, y = 70) and suspended palladium nanoparticles with an average diameter of 4 nm. Solvent was withdrawn from the channel at a rate of 1 cm/s yielding a 120 nm continuous titania layer with a cubic mesostructure after drying and calcination. The organic copolymer was removed by calcination at 300oC under a residual pressure of 15 mbar. The coating porosity was 0.4, resulting in overall coating mass of 1.32 mg with a 1 wt.% Pd content. The liquid flow was varied between 1 and 10 ”L/min and the hydrogen flow between 250 and 550 ”L/min (STP). This corresponds to superficial velocities of 0.034-0.34 cm/s and 8-18 cm/s for liquid and gas, respectively. The maximum selectivity to styrene of 95 % was observed at a phenylacetylene conversion of 88%. The reaction rate in terms of TOF was found to be up to 2 s-1
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