Abstract: The fly ash of waste incineration processes is usually hazardous and the disposal or reuse of waste incineration fly ash is difficult. In this study, the waste incineration fly ash was converted to useful zeolites by the alkali fusion and hydrothermal synthesis method. The influence of different operating conditions (the ratio of Si/Al, the ratio of hydrolysis liquid to solid, and hydrothermal time) was investigated to seek the optimum operating conditions for the synthesis of zeolite from waste incineration fly ash. The results showed that concentrations of heavy metals in the leachate of Toxicity Characteristic Leaching Procedure (TCLP) were all lower than the regulatory limits except lead. The optimum operating conditions for the synthesis of zeolite from waste incineration fly ash by the alkali fusion and hydrothermal synthesis method were Si/Al=40, NaOH/ash=1.5, alkali fusion at 400 oC for 40 min, hydrolysis with Liquid to Solid ratio (L/S)= 200 at 105 oC for 24 h, and hydrothermal synthesis at 105 oC for 24 h. The specific surface area of fly ash could be significantly increased from 8.59 m2/g to 651.51 m2/g (synthesized zeolite). The influence of different operating conditions on the synthesis of zeolite from waste incineration fly ash followed the sequence of Si/Al ratio > hydrothermal time > hydrolysis L/S ratio. The synthesized zeolites can be reused as good adsorbents to control the air or wastewater pollutants. The purpose of fly ash detoxification, reduction and waste recycling/reuse is achieved successfully.
Abstract: SSZ-13 materials with different Si/Al ratio were prepared by varying the composition of aluminosilicate precursor solutions upon hydrothermal treatment at 150 °C. The Si/Al ratio of the initial system was systematically changed from 12.5 to infinity in order to study the limits of Al composition in precursor solutions for constructing CHA structure. The intermediates and final products were investigated by complementary techniques such as XRD, HRTEM, FESEM, and chemical analysis. NH3-TPD was used to study the Brønsted acidity of SSZ-13 samples with different Si/Al ratios. The effect of the Si/Al ratio on the precursor species, ultimate crystal size, morphology and yield was investigated. The results revealed that Al species determine the nucleation rate and the number of nuclei, which is tied to the morphology and yield of SSZ-13. The size of SSZ-13 increased and the yield decreased as the Si/Al ratio was improved. Varying Si/Al ratio of the initial system is a facile, commercially viable method of tailoring SSZ-13 crystal size and morphology. Furthermore, SSZ-13 materials with different Si/Al ratio were tested as catalysts for the methanol to olefins (MTO) reaction at 350 °C. SSZ-13 with the Si/Al ratio of 35 shows the best MTO catalytic performance.
Abstract: Methanol-to-propylene conversion was carried out in a continuous-flow fixed-bed reactor over nano-sized HZSM-5 zeolites. The HZSM-5 catalysts were synthesized with different Si/Al ratio and silicon sources, and treated with NaOH. The structural property, morphology, and acidity of catalysts were measured by XRD, N2 adsorption, FE-SEM, TEM, and NH3-TPD. The results indicate that the increment of Si/Al ratio decreased the acidity of catalysts and then improved propylene selectivity, while silicon sources had slight impact on the acidity but affected the product distribution. The desilication after alkali treatment could increase intracrystalline mesopores and enhance propylene selectivity.
Abstract: This work details the generation of thin films of
structured zeolite catalysts (ZSM–5 and Y) onto the surface of a
metal substrate (FeCrAlloy) using in-situ hydrothermal synthesis. In
addition, the zeolite Y is post-synthetically modified by acidified
ammonium ion exchange to generate US-Y. Finally the catalytic
activity of the structured ZSM-5 catalyst films (Si/Al = 11, thickness
146 0m) and structured US–Y catalyst film (Si/Al = 8, thickness
230m) were compared with the pelleted powder form of ZSM–5 and
USY catalysts of similar Si/Al ratios.
The structured catalyst films have been characterised using a range
of techniques, including X-ray diffraction (XRD), Electron
microscopy (SEM), Energy Dispersive X–ray analysis (EDX) and
Thermogravimetric Analysis (TGA). The transition from oxide-onalloy
wires to hydrothermally synthesised uniformly zeolite coated
surfaces was followed using SEM and XRD. In addition, the
robustness of the prepared coating was confirmed by subjecting these
to thermal cycling (ambient to 550oC).
The cracking of n–heptane over the pellets and structured catalysts
for both ZSM–5 and Y zeolite showed very similar product
selectivities for similar amounts of catalyst with an apparent
activation energy of around 60 kJ mol-1. This paper demonstrates that
structured catalysts can be manufactured with excellent zeolite
adherence and when suitably activated/modified give comparable
cracking results to the pelleted powder forms. These structured
catalysts will improve temperature distribution in highly exothermic
and endothermic catalysed processes.
Abstract: The acidity of different raw Jordanian clays
containing zeolite, bentonite, red and white kaolinite and diatomite
was characterized by means of temperature programmed desorption
(TPD) of ammonia, conversion of 2-methyl-3-butyn-2-ol (MBOH),
FTIR and BET-measurements. FTIR spectra proved presence of
silanol and bridged hydroxyls on the clay surface. The number of
acidic sites was calculated from experimental TPD-profiles. We
observed the decrease of surface acidity correlates with the decrease
of Si/Al ratio except for diatomite. On the TPD-plot for zeolite two
maxima were registered due to different strength of surface acidic
sites. Values of MBOH conversion, product yields and selectivity
were calculated for the catalysis on Jordanian clays. We obtained that
all clay samples are able to convert MBOH into a major product
which is 3-methyl-3-buten-1-yne (MBYNE) catalyzed by acid
surface sites with the selectivity close to 70%. There was found a
correlation between MBOH conversion and acidity of clays
determined by TPD-NH3, i.e. the higher the acidity the higher the
conversion of MBOH. However, diatomite provided the lowest
conversion of MBOH as result of poor polarization of silanol groups.
Comparison of surface areas and conversions revealed the highest
density of active sites for red kaolinite and the lowest for zeolite and
diatomite.