scholarly journals Synthesis of Ni-Modified ZSM-5 Zeolites and Their Catalytic Performance in n-Octane Hydroconversion

2020 ◽  
Vol 8 ◽  
Author(s):  
Qiang Wei ◽  
Pengfei Zhang ◽  
Xiaodong Liu ◽  
Wenbin Huang ◽  
Xiayun Fan ◽  
...  

Ni-modified ZSM-5 zeolites with different nickel contents were successfully prepared by the in situ synthesis method and the impregnation method. The synthesized samples were characterized by XRD, SEM, N2 adsorption–desorption isothermals, and Py-FTIR. The characterization results show that both the textural properties and crystallization of Ni-modified ZSM-5 zeolites were preserved well, and their acidic properties can be modulated after nickel modification. The corresponding NiMo catalysts supported on Ni-modified ZSM-5 zeolites were prepared by the incipient wetness co-impregnation method, and their catalytic performances were evaluated in n-octane hydroconversion. Compared to the those modified by the in situ synthesis method, ZSM-5 zeolite-supported catalysts modified by the impregnation method exhibit higher stability and higher isomerization selectivity. This is due to the synergistic effect between Brønsted acid sites and Lewis acid sites on the Ni-modified ZSM-5 zeolites, especially for the NiMo/1Ni-Z5 catalyst.

2020 ◽  
Vol 218 ◽  
pp. 03032
Author(s):  
Chenxi Li ◽  
Fanwei Meng ◽  
Qing Ye

A series of xCe-Fe/ZSM-5 (x = 0, 0.25, 0.5 wt%) samples were prepared by the impregnation method, and the catalytic activity was evaluated by the selective catalytic reduction of NOx with ammonia (NH3-SCR). The physicochemical properties of prepared samples were characterized by various techniques such as X-ray diffraction (XRD), Brunner-Emmet-Teller (BET) measurement, hydrogen temperatureprogrammed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), ammonia temperatureprogrammed desorption (NH3-TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). XRD and BET results demonstrated that Ce and Fe species were uniform dispersed on the surface of the ZSM-5 zeolite and the micropore structure of ZSM-5 was still maintained. H2-TPR analysis indicated that the doping of Ce created more isolated Ce4+ and Fe3+ on the surface of catalysts, and the abundant Ce4+ and Fe3+ could enhance the reduction ability of catalysts. XPS analysis suggested that the doping of Ce could generate more oxygen vacancies, thereby increasing the number of chemisorption oxygen. According to the in-situ DRIFTS and NH3-TPD results, Ce species provided more acidic sites, which is beneficial to the NH3 adsorption ability of ZSM-5 zeolite. Additionally, the abundant chemisorption oxygen, medium and strong Brønsted acid sites, excellent NH3 adsorption ability and outstanding reduction property are beneficial to the NH3-SCR reaction. Among all prepared samples, the 0.25Ce-Fe/ZSM-5 sample possessed the widest reaction temperature window and the best catalytic performance (NO conversion over 98% at 350-450 °C), which was associated with the abundant acid sites and remarkable adsorption ability of NH3, outstanding redox ability and abundant chemisorption oxygen after the doping of Ce.


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).


Catalysts ◽  
2018 ◽  
Vol 8 (11) ◽  
pp. 541 ◽  
Author(s):  
Haiping Xiao ◽  
Chaozong Dou ◽  
Hao Shi ◽  
Jinlin Ge ◽  
Li Cai

A series of poisoned catalysts with various forms and contents of sodium salts (Na2SO4 and Na2S2O7) were prepared using the wet impregnation method. The influence of sodium salts poisoned catalysts on SO2 oxidation and NO reduction was investigated. The chemical and physical features of the catalysts were characterized via NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). The results showed that sodium salts poisoned catalysts led to a decrease in the denitration efficiency. The 3.6% Na2SO4 poisoned catalyst was the most severely deactivated with denitration efficiency of only 50.97% at 350 °C. The introduction of SO42− and S2O72− created new Brønsted acid sites, which facilitated the adsorption of NH3 and NO reduction. The sodium salts poisoned catalysts significantly increased the conversion of SO2–SO3. 3.6%Na2S2O7 poisoned catalyst had the strongest effect on SO2 oxidation and the catalyst achieved a maximum SO2–SO3-conversion of 1.44% at 410 °C. Characterization results showed sodium salts poisoned catalysts consumed the active ingredient and lowered the V4+/V5+ ratio, which suppressed catalytic performance. However, they increased the content of chemically adsorbed oxygen and the strength of V5+=O bonds, which promoted SO2 oxidation.


Author(s):  
Nuno Batalha ◽  
Jean-Dominique Comparot ◽  
Anthony Le Valant ◽  
Ludovic Pinard

Acid sites, in particular Brønsted sites, are often reported to enhance the catalytic performance of metal catalysts, like platinum, in hydrogenation. The significant boost in catalytic performance suggests a bifunctional...


2019 ◽  
Vol 45 ◽  
pp. 146867831988793
Author(s):  
Niloofar Atashi ◽  
Mohammad Hasan Peyrovi ◽  
Nastaran Parsafard

Platinum-carbonaceous catalysts were prepared by the wet impregnation method and tested for catalytic oxidation of toluene as a volatile organic compound. The textural properties of the constructed catalysts were considered by X-ray diffraction, X-ray fluorescence, inductively coupled plasma – optical emission spectroscopy, Fourier transform infrared, scanning electron microscope and N2 adsorption–desorption analysis. The catalytic assessments showed that the best activity (>99%) and high stability and selectivity to CO2 (>99%) are related to platinum-supported carbon nanotube. The curves of the conversion and selectivity demonstrate that the performance of catalysts to eliminate the volatile organic compound and turn it into CO2 conforms to the following descending order: platinum-supported carbon nanotube >platinum-supported graphene >platinum-supported activated carbon >platinum-supported carbon nanofibre. The kinetic of toluene oxidation has been evaluated as a function of toluene and oxygen partial pressures in different temperatures. Two kinetic models (Power Law and Mars–van Krevelen mechanisms) were applied to the reaction and compared with the experimental data. Mars–van Krevelen model is more appropriate than the Power Law model for this reaction as Mars–van Krevelen model showed better prediction of the behaviour of the reaction.


Catalysts ◽  
2019 ◽  
Vol 9 (2) ◽  
pp. 155 ◽  
Author(s):  
Zhenheng Diao ◽  
Lushi Cheng ◽  
Xu Hou ◽  
Di Rong ◽  
Yanli Lu ◽  
...  

Hierarchical HZSM-5 membranes were prepared on the inner wall of stainless steel tubes, using amphiphilic organosilane (TPOAC) and mesitylene (TMB) as a meso-porogen and a swelling agent, respectively. The mesoporosity of the HZSM-5 membranes were tailored via formulating the TPOAC/Tetraethylorthosilicate (TPOAC/TEOS) ratio and TMB/TPOAC ratio, in synthesis gel, and the prepared membranes were systematically characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), N2 adsorption–desorption, N2 permeation, inductively coupled plasma (ICP), in situ fourier transform infrared (FT-IR), ammonia temperature-programmed desorption (NH3-TPD), etc. It was found that the increase of the TPOAC/TEOS ratio promoted a specific surface area and diffusivity of the HZSM-5 membranes, as well as decreased acidity; the increase of the TMB/TPOAC ratios led to an enlargement of the mesopore size and diffusivity of the membranes, but with constant acid properties. The catalytic performance of the prepared HZSM-5 membranes was tested using the catalytic cracking of supercritical n-dodecane (500 °C, 4 MPa) as a model reaction. The hierarchical membrane with the TPOAC/TEOS ratio of 0.1 and TMB/TPOAC ratio of 2, exhibited superior catalytic performances with the highest activity of up to 13% improvement and the lowest deactivation rate (nearly a half), compared with the microporous HZSM-5 membrane, due to the benefits of suitable acidity, together with enhanced diffusivity of n-dodecane and cracking products.


Author(s):  
Susana Guadix-Montero ◽  
Alba Santos-Hernandez ◽  
Andrea Folli ◽  
Meenakshisundaram Sankar

We report the role of the acidity of support during the selectivity hydrogenolysis of glycerol over supported bimetallic palladium–ruthenium (PdRu) catalysts. The PdRu nanoparticles were supported on a series of metal oxides and zeolitic supports via the modified impregnation method and tested for the liquid-phase hydrogenolysis of glycerol using gaseous hydrogen. The relative acid site densities of selected catalysts were determined by ammonia temperature-programmed desorption and pyridine desorption experiments. Based on these studies, we report a direct correlation between the catalytic activity (conversion and 1,2 propane diol yield) and two different acid sites (strong acid sites and very strong acid sites). Besides zeolite-supported catalysts, TiO 2 supported PdRu nanoparticles exhibit moderate catalytic activity; however, this catalyst shows high selectivity for the desired C–O bond cleavage to produce C3 products over the undesired C–C bond cleavage to produce < C3 products. This article is part of a discussion meeting issue ‘Science to enable the circular economy’.


2013 ◽  
Vol 634-638 ◽  
pp. 696-700
Author(s):  
Lin Jiu Xiao ◽  
Peng Li ◽  
Yong Gang Sheng

A series of Ti(SO4)2/γ-Al2O3 catalysts were prepared by impregnation method and the catalytic performance of these catalysts in 1-butene oligomerization was investigated. The heat treatment temperature played great influences on the catalytic performance of these catalysts in the oligomerization. 90.1 wt.% conversion of 1-butene and 92.2 wt.% selectivity of dimers were obtained on Ti(SO4)2/γ-Al2O3(450) catalyst at 80 °C, 1.0 Mpa and LHSV=0.6 h−1. The heat treatment temperature determined the crystallinity of TiOSO4 and specific surface area of these catalysts, which affected the catalytic performance of these catalysts in 1-butene oligomerization. In addition, the physicochemical properties of these catalysts were comparatively characterized by powder X-ray diffraction (XRD), N2 isothermal adsorption-desorption techniques.


Author(s):  
Junan Gao ◽  
Song Gao ◽  
Jun Wei ◽  
Hong Zhao ◽  
Jie Zhang

In this paper, the catalytic combustion of DMDS (dimethyl disulfide, CH3SSCH3) over bimetallic supported catalysts were investigated. It was confirmed that Cu/&gamma;-Al2O3-CeO2 showed best catalytic performance among the five single-metal catalysts. Furthermore, six different metals were separately added into Cu/&gamma;-Al2O3-CeO2 to investigate the promoting effect. The experiments revealed Pt as the most effective promoter and the the best catalytic performance was achieved as the adding amount of 0.3 wt%. The characterization results indicated that high activity and resistance to sulfur poisoning of Cu-Pt/&gamma;-Al2O3-CeO2 could be attributed to the synergistic effect between Cu and Pt.


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