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RSC Adv ; 11(12): 6667-6681, 2021 Feb 04.
Artigo em Inglês | MEDLINE | ID: mdl-35423191


Extensive effort has been focused on the advancement of an efficient catalyst for CO2 reforming of CH4 to achieve optimum catalytic activity together with cost-effectiveness and high resistance to catalyst deactivation. In this study, for the first time, a new catalytic support/catalyst system of bifunctional NiO/dolomite has been synthesized by a wet impregnation method using low-cost materials, and it shows unique performance in terms of amphoteric sites and self-reduction properties. The catalysts were loaded into a continuous micro-reactor equipped with an online GC-TCD system. The reaction was carried out with a gas mixture consisting of CH4 and CO2 in the ratio of 1 : 1 flowing 30 ml min-1 at 800 °C for 10 h. The physicochemical properties of the synthesized catalysts were determined by various methods including X-ray diffraction (XRD), N2 adsorption-desorption, H2 temperature-programmed reduction (H2-TPR), temperature-programmed desorption of CO2 (TPD-CO2), and temperature-programmed desorption of NH3 (TPD-NH3). The highest catalytic performance of the DRM reaction was shown by the 10% NiO/dolomite catalyst (CH4 & CO2 conversion, χCH4; χCO2 ∼ 98% and H2 selectivity, S H2 = 75%; H2/CO ∼ 1 : 1 respectively). Bifunctional properties of amphoteric sites on the catalyst and self-reduction behaviour of the NiO/dolomite catalyst improved dry reforming of the CH4 process by enhancing CH4 and CO2 conversion without involving a catalyst reduction step, and the catalyst was constantly active for more than 10 h.

Membranes (Basel) ; 9(7)2019 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-31319501


Hydrophobic pure-silica *BEA-type zeolite membranes with large pores were prepared on tubular silica supports by hydrothermal synthesis using a secondary growth method and were applied to the separation of alcohol/water mixtures by pervaporation (PV), an alternative energy-efficient process for production of biofuels. Amorphous pure-silica tubular silica supports, free of Al atoms, were used for preparing the membranes. In this study, the effects of the synthesis conditions, such as the H2O/SiO2 and NH4F/SiO2 ratios in the synthetic gel, on the membrane formation process and separation performance were systematically investigated. The successfully prepared dense and continuous membranes exhibited alcohol selectivity and high flux for the separation of ethanol/water and butanol/water mixtures. The pure-silica *BEA membranes obtained under optimal conditions (0.08SiO2:0.5TEAOH:0.7NH4F:8H2O) showed high PV performance with a separation factor of 229 and a flux of 0.62 kg·m-2·h-1 for a 1 wt % n-butanol/water mixture at 318 K. This result was attributed to the hydrophobicity and large pore size of the pure-silica *BEA membrane. This was the first successful synthesis of hydrophobic large-pore zeolite membranes on tubular supports with alcohol selectivity, and the obtained results could provide new insights into the research on hydrophobic membranes with high permeability.

Membranes (Basel) ; 9(4)2019 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-30939830


Silicalite-1 membranes with high pervaporation performance were prepared successfully on a silica-particle-coated tubular silica support using a gel-free steam-assisted conversion (SAC) method. The effects of the silica-particle layer formed on the top surface of the silica support and the physical properties of the silica particles themselves on the membrane-formation process were investigated. The silica particles coated served as the additional silica source for growing the silicalite-1 seed crystal layer into the silicalite-1 membrane. As a result, it was possible to form a dense and continuous membrane even under gel-free conditions. Furthermore, it was found that the properties of the silica particles, such as their primary particle diameter, had a determining effect on their solubility during the steam treatment, that is, on the supply rate of the silica source. The silicalite-1 membrane obtained using the spherical-silica-particle-coated support had an approximately 9-µm-thick separation layer and showed very high pervaporation performance, exhibiting a separation factor of 105 and a flux of 3.72 kg m-2 h-1 for a 10 wt % ethanol/water mixture at 323 K. Thus, the gel-free SAC method can be used with a silica support coated with silica particles to readily prepare high-performance membranes without producing any chemical waste.

ChemSusChem ; 11(11): 1756-1760, 2018 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-29673091


Dehumidification in CO2 adsorptive separation processes is an important issue, owing to its high energy consumption. However, available adsorbents such as low-silica zeolites show a significant decrease in CO2 adsorption capacity when water vapor is present. A core-shell-structured MFI-type zeolite with a hydrophilic ZSM-5 coated with a hydrophobic silicalite-1 shell layer was applied in CO2 adsorptive separation under wet conditions. This hybrid material demonstrated remarkably high water tolerance with stable CO2 adsorption performance without additional thermal treatment for regeneration, whereas a significant decrease in the CO2 adsorption amount because of water vapor was observed on the parent ZSM-5. The core-shell structure of zeolites with high pore volumes, such as LTA or CHA, could also be suitable candidates for high CO2 adsorption capacity and high water tolerance for practical applications.