Fabrication of a sinter-resistant Fe-MFI zeolite dragonfruit-like catalyst for syngas to aromatics conversion

Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.

Role of surface frustrated Lewis pairs on reduced CeO2(110)in direct conversion of syngas

Direct syngas conversion to light olefins on bifunctional oxide-zeolite(OX-ZEO)catalysts is of great interest to both academia and industry,but the role of oxygen vacancy(Vo)in metal oxides and whether the key intermediate in the reaction mechanism is ketene or methanol are still not well-understood.To address these two issues,we carry out a theoretical study of the syngas conversion on the typical reducible metal oxide,CeO2,using density functional theory calculations.Our results demonstrate that by forming frustrated Lewis pairs(FLPs),the VOs in CeO2 play a key role in the activation of H2 and CO.The activation of H2 on FLPs undergoes a heterolytic dissociative pathway with a tiny barrier of 0.01 eV,while CO is activated on FLPs by combining with the basic site(O atom)of FLPs to form CO2^2-.Four pathways for the conversion of syngas were explored on FLPs,two of which are prone to form ketene and the other two are inclined to produce methanol suggesting a compromise to resolve the debate about the key intermediates(ketene or methanol)in the experiments.Rate constant calculations showed that the route initiating with the coupling of two CO*into OCCO*and ending with the formation of ketene is the dominant pathway,with the neighboring FLPs playing an important role in this pathway.Overall,our study reveals the function of the surface FLPs in the activation of H2 and CO and the reaction mechanism for the production of ketene and methanol for the first time,providing novel insights into syngas conversion over OX-ZEO catalysts.

Copper oxide nanoparticles-loaded zeolite and its characteristics and antibacterial activities

In the present work, a simple and green co-precipitation method was used to prepare copper oxide-zeolite nanocomposites（CuO-zeolite NCs）. The weight ratio（1, 3, 5, 8 and 10 wt%） of CuO nanoparticles（NPs）loaded into zeolite was investigated to obtain the optimum CuO distribution for antibacterial activities.The prepared CuO-zeolite NCs were characterized by ultraviolet-visible（UV–vis） spectroscopy, Fourier transform infrared（FT-IR） spectroscopy, powder X-ray diffraction（XRD）, and energy dispersive X-ray fluorescence spectrometry（EDXRF）. The transmission electron microscopy（TEM） and field emission scanning electron microscopy（FE-SEM） revealed a uniform surface morphology of the CuO-zeolite NCs.The UV–vis spectrum of NCs showed absorption peaks between 230 and 280 nm for nano-CuO in the XRD patterns, and new peaks appeared between（36.56？–38.83？） related to the CuO. At weight ratio less than 10 wt%, the CuO nanoparticles loaded to the zeolite exhibited spherical shapes with average particle diameter of 6.5 nm measured by TEM and XRD. Antibacterial activities were tested against Gram-negative and Gram-positive bacteria. The obtained results showed that, CuO-zeolite NCs with 8 wt% CuO nanoparticles had the highest antibacterial activities against Bacillus Subtilis B29 and Salmonella Choleraesuis ATCC10708, which can be attributed to the good dispersion of CuO NPs on the zeolite surface.