Micro/Mesoporous Composites Based on Colloidal Zeolite Grown in Mesoporous Matrix

2005 ◽  
Vol 70 (11) ◽  
pp. 1829-1847 ◽  
Author(s):  
Pavla Prokešová ◽  
Nikolay Petkov ◽  
Jiří Čejka ◽  
Svetlana Mintova ◽  
Thomas Bein

Composite materials containing micro- and mesopores are prepared under instantaneous hydrothermal treatment of initial solutions generally used for zeolite Beta and precursor solutions for mesoporous Al-MCM-41 material. The resulting composites are compared with pure, highly crystalline colloidal microporous Beta zeolite and hexagonally ordered mesostructured samples. The porosity and morphological features of the composite materials are influenced by the conditions of hydrothermal synthesis of the initial colloidal solutions used for the preparation of Beta seeds, as well as by the conditions of the synchronized crystallization of the final composites. The embedding of Beta seeds in the mesoporous silica matrix is possible via immediate heating of mesoporous precursor solutions with Beta seeds primarily formed. The composite materials contain either microcrystalline Beta nanodomains with sizes of about 5-10 nm surrounded by mesoporous material or defined Beta nanocrystals (20-40 nm), and at the same time connected with mesostructured material. The presence of highly crosslinked silicate framework walls and tetrahedrally coordinated aluminum in the composite material are confirmed by solid-state 29Si and 27Al MAS NMR spectroscopy. The concentration of Brønsted acid sites in the micro/mesoporous composites is increased substantially in comparison with pure mesoporous Al-MCM-41 material proven by FTIR acetonitrile-d3 adsorption study.

2007 ◽  
Vol 72 (5-6) ◽  
pp. 728-746 ◽  
Author(s):  
Martina Bejblová ◽  
Josef Vlk ◽  
Dana Procházková ◽  
Helena Šiklová ◽  
Jiří Čejka

The role of the type of acid site (Broensted vs. Lewis) on the activity and selectivity of molecular sieve catalysts was investigated in ferrocene and toluene acylation. H-, Zn-, Fe-, Al- and La-forms of zeolite Beta, USY and mesoporous molecular sieves (Al)MCM-41, (Al)SBA-15 were tested. It was observed that addition of metal cations acting as Lewis acid sites can increase the acidity of various molecular sieve catalysts. No general relationship between the type of cation and conversion of individual substrate was found. While the highest activity in ferrocene acylation was observed after addition of Zn, in the case of toluene acylation Al-forms of catalysts were the most active. The results indicate that the acid strength of cationic Lewis sites controls their activity in acylation reactions.


Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 488
Author(s):  
Katarzyna Stawicka ◽  
Maciej Trejda ◽  
Maria Ziolek

Niobium containing SBA-15 was prepared by two methods: impregnation with different amounts of ammonium niobate(V) oxalate (Nb-15/SBA-15 and Nb-25/SBA-15 containing 15 wt.% and 25 wt.% of Nb, respectively) and mixing of mesoporous silica with Nb2O5 followed by heating at 500 °C (Nb2O5/SBA-15). The use of these two procedures allowed obtaining materials with different textural/surface properties determined by N2 adsorption/desorption isotherms, XRD, UV-Vis, pyridine, and NO adsorption combined with FTIR spectroscopy. Nb2O5/SBA-15 contained exclusively crystalline Nb2O5 on the SBA-15 surface, whereas the materials prepared by impregnation had both metal oxide and niobium incorporated into the silica matrix. The niobium species localized in silica framework generated Brønsted (BAS) and Lewis (LAS) acid sites. The inclusion of niobium into SBA-15 skeleton was crucial for the achievement of high catalytic performance. The strongest BAS were on Nb-25/SBA-15, whereas the highest concentration of BAS and LAS was on Nb-15/SBA-15 surface. Nb2O5/SBA-15 material possessed only weak LAS and BAS. The presence of the strongest BAS (Nb-25/SBA-15) resulted in the highest dehydration activity, whereas a high concentration of BAS was unfavorable. Silylation of niobium catalysts prepared by impregnation reduced the number of acidic sites and significantly increased acrolein yield and selectivity (from ca. 43% selectivity for Nb-25/SBA-15 to ca. 61% for silylated sample). This was accompanied by a considerable decrease in coke formation (from 47% selectivity for Nb-25/SBA-15 to 27% for silylated material).


Processes ◽  
2021 ◽  
Vol 9 (2) ◽  
pp. 400
Author(s):  
Xiaohua Cao ◽  
Jichang Lu ◽  
Yutong Zhao ◽  
Rui Tian ◽  
Wenjun Zhang ◽  
...  

Praseodymium (Pr)-promoted MCM-41 catalyst was investigated for the catalytic decomposition of methyl mercaptan (CH3SH). Various characterization techniques, such as X-ray diffraction (XRD), N2 adsorption–desorption, temperature-programmed desorption of ammonia (NH3-TPD) and carbon dioxide (CO2-TPD), hydrogen temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectrometer (XPS), were carried out to analyze the physicochemical properties of material. XPS characterization results showed that praseodymium was presented on the modified catalyst in the form of praseodymium oxide species, which can react with coke deposit to prolong the catalytic stability until 120 h. Meanwhile, the strong acid sites were proved to be the main active center over the 10% Pr/MCM-41 catalyst by NH3-TPD results during the catalytic elimination of methyl mercaptan. The possible reaction mechanism was proposed by analyzing the product distribution results. The final products were mainly small-molecule products, such as methane (CH4) and hydrogen sulfide (H2S). Dimethyl sulfide (CH3SCH3) was a reaction intermediate during the reaction. Therefore, this work contributes to the understanding of the reaction process of catalytic decomposition methyl mercaptan and the design of anti-carbon deposition catalysts.


2005 ◽  
Vol 23 (3) ◽  
pp. 255-266 ◽  
Author(s):  
J. O'Brien ◽  
T. Curtin ◽  
T.F. O'Dwyer

Zeolite beta, a large-pore zeolite, was investigated in this study with a view to examining it as a potential adsorbent for the removal of aniline from aqueous solutions. Two different metal-loaded zeolites were prepared by exchanging H-beta zeolite (SiO2/Al2O3 = 75:1) with copper. The influence of exchanged copper on the uptake level was assessed. The effect of varying the silica-to-alumina ratio of the H-beta zeolite on the aniline uptake level was also examined, using three different H-beta zeolites with ratios of 25:1, 75:1 and 150:1 as adsorbents. The sorption experiments indicated an uptake level of ca. 110–120 mg/g for each zeolite and this level was also adsorbed by the copper-modified H-beta zeolites (SiO2/Al2O3 = 75:1). In all cases, the adsorption process followed the Langmuir model for adsorption and the level of aniline adsorbed was largely unaffected by a change in temperature or the presence of extra framework copper. The stability of the exchanged copper on these zeolites was then examined by measuring the quantity of copper leached from each zeolite into solution as a function of pH. Minimum copper leaching was observed in the pH range 5–11. This provided a stable pH working range for the adsorbent materials.


2020 ◽  
Vol 539 ◽  
pp. 110983
Author(s):  
Baoqiang Zhang ◽  
Xiangshuai Zhu ◽  
Jiang Gao ◽  
Yingluo Zhu ◽  
Weihua Ma

2005 ◽  
Vol 12 (3) ◽  
pp. 193-199 ◽  
Author(s):  
Valeri Naydenov ◽  
Lubomira Tosheva ◽  
Johan Sterte
Keyword(s):  

2001 ◽  
Vol 667 ◽  
Author(s):  
Arnaud Huignard ◽  
Thierry Gacoin ◽  
Frédéric Chaput ◽  
Jean-Pierre Boilot ◽  
Patrick Aschehoug ◽  
...  

ABSTRACTAqueous colloidal solutions of well dispersed YVO4:Ln (Ln = Eu, Nd) nanoparticles are synthesized through precipitation reactions at room temperature. In the case of YVO4:Eu, a luminescence quantum yield of 15% is found, which is not as high as in the bulk due to the existence of residual crystalline defects and nonradiative relaxations from the hydroxylated surface. Appropriate hydrothermal annealing and deuteration of the surface allow to rise the yield up to 38%. Incorporation of the nanocrystals into a transparent silica matrix is achieved through preliminary coating of the particles with a functionnalized silicon alkoxide and further dispersion into a sol-gel precursor solution. Such sol-gel materials doped with YVO4:Nd nanocrystals are transparent and exhibit the typical emission at 1.06 μm of the Nd3+ ion.


2006 ◽  
Vol 510-511 ◽  
pp. 138-141 ◽  
Author(s):  
Shan Zheng ◽  
Lian Gao

Titanium oxynitride and molybdenum oxynitride assembled in the pores of mesoporous materials were achieved by nitriding titania-modified MCM-41 and molybdena-modified MCM-41 at 800°C for 3 hours under flowing NH3 atmosphere. XRD, XPS and N2 adsorption-desorption isotherms were employed to characterize the structure of the composite materials. The results showed that the nanosized TiOxNy and MoOxNy particles were assembled in mesoporous silica MCM-41 with the restrict mesopores. The hexagonal periodicity of the parent MCM-41 materials was maintained upon assembly at the provided nitridation temperature. The exact formation was TiO0.4N0.8 in MCM-TiOxNy, and MoO1.7N0.57 in MCM-MoOxNy, which were calculated from the data in XPS spectra of Ti 2p and Mo 3d.


2016 ◽  
Vol 6 (9) ◽  
pp. 3018-3026 ◽  
Author(s):  
Maura Koehle ◽  
Raul F. Lobo

Tin-, zirconium- and hafnium-containing siliceous Beta zeolite were investigated in the Meerwein–Ponndorf–Verley reduction of furfural under continuous flow conditions.


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