scholarly journals Composite Nanostructure of Manganese Cluster and CHA-Type Silicoaluminaphosphates: Enhanced Catalytic Performance in Dimethylether to Light Olefins Conversion

Nanomaterials ◽  
2020 ◽  
Vol 11 (1) ◽  
pp. 24
Author(s):  
Guichen Ping ◽  
Kai Zheng ◽  
Qihua Fang ◽  
Gao Li

Light olefins, especially ethylene and propylene, are important chemicals in petrochemical industries with an increasing demand and play an essential role in the global consumption. In this regard, there have been extensive studies to design efficient catalysts for the light olefins productions. In this study, we report a new protocol to induce Mn nanoclusters (MnNC) into the mesopore of a CHA-type silicoaluminaphosphates via a one-pot synthesis of MnNC@SAPO-34 catalysts. The catalysts are characterized by a series of technology, such as TEM, XRD, NH3-TPD, 27Al MAS NMR, ICP-MS, XPS, and as well as N2-physical adsorption methods. The Mn nanoclusters of Mn2O3 and MnO2 species are well dispersed in the framework of the SAPO-34 silicoaluminaphosphates, modifying the porosity and acidic property of the SAPO-34: Giving rise to more mesoporous and improving the acid density. The MnNC@SAPO-34 catalysts exhibit decent 100% conversion and 92.2% olefins selectivity in the dimethyl ether to olefins (DTO) reactions, which is considerably higher than that for SAPO-34 silicoaluminaphosphates (79.6% olefins selectivity). The higher olefins selectivity over the MnNC@SAPO-34 is deemed to associate with the strong acid density and intensity of the silicoaluminaphosphates. Further, the Mn particles largely improve silicoaluminaphosphates’s durability.

2014 ◽  
Vol 68 (9) ◽  
Author(s):  
Su-Hong Zhang ◽  
Zhi-Xian Gao ◽  
Shao-Jun Qing ◽  
Sheng-Yu Liu ◽  
Yan Qiao

AbstractThe effect of Zn on the catalytic performance of ZSM-5 in the methanol-to-olefin conversion was investigated. The samples were characterised by X-ray diffraction, N2 adsorption, FTIR, temperature-programmed desorption of ammonia and water, and Py-IR. The experimental results revealed Znmodified ZSM-5 to show a lower selectivity to light olefin at the higher reaction temperature of 520°C but a higher selectivity to light olefin at lower temperatures. As a comparison, the catalytic performance of Ca-modified ZSM-5 for the methanol conversion is also given. From the above results, it is concluded that Zn may play another role in the methanol conversion in addition to tuning the surface acidic property after modification.


Catalysts ◽  
2019 ◽  
Vol 9 (11) ◽  
pp. 968
Author(s):  
Guangjian Wang ◽  
Ning Song ◽  
Kai Lu ◽  
Wentai Wang ◽  
Liancheng Bing ◽  
...  

The dehydrogenation of low-carbon alkane to obtain olefins is an effective way to meet the steadily increasing demand of these building blocks in chemical industry. In this study, Ca-doped CrOx/γ-Al2O3 catalysts were fabricated via a one-pot method by employing Cr(OH)3 as the precursor, and their catalytic performances were tested in the dehydrogenation of isobutane to isobutene (DITI) process. The prepared catalysts were intensively characterized by XRD, SEM, NH3-TPD, H2-TPR, low-temperature N2 adsorption–desorption, etc. These characterization results indicated that the doping of Ca into the CrOx/γ-Al2O3 catalysts could tune the acidity properties of the prepared catalysts and enhance the interaction between the active species and support. The Ca-doped CrOx/γ-Al2O3 catalysts, especially the Ca2-Cr/γ-Al2O3 catalyst with a Ca doping of 2 wt%, exhibited a superior catalytic performance in the DITI process in comparison with the undoped catalyst.


2020 ◽  
Vol 2 (1) ◽  
pp. 34
Author(s):  
Benjamín Torres Olea ◽  
Inmaculada Fúñez Nuñez ◽  
Cristina García Sancho ◽  
Juan Antonio Cecilia ◽  
Ramón Moreno Tost ◽  
...  

In this work, acidic ion-exchange resins with strong Brönsted sulphonic groups were assessed in the catalytic etherification of the platform molecule 5-(hydroxymethyl)furfural (HMF) to 5-(ethoxymethyl)furfural (EMF), a biofuel with an energy density close to that of gasoline (30 MJ/L) which also reduces emissions of NOx and SOx and solid particles respect to fossil-derived fuels. Catalytic performance was optimized modifying experimental parameters such as reaction time, temperature, and concentration of reagent employed. This process was carried out in batch reactors using ethanol 96% as solvent. Among different cation-exchange resins tested, Purolite CT275DR provided the fastest HMF conversion together with Purolite PD206, and the highest selectivity to EMF, achieving above 70% selectivity at 100 °C. Over time, strong acid sites favoured product hydrolysis opening the furan ring originating ethyl levulinate (EL) to the detriment of EMF selectivity. Purolite CT275DR was also utilised to realize the transformation from sugars directly to EMF in the same reaction medium, in a one-pot process, obtaining relevant results from fructose (37% HMF yield, 21% EMF yield after 5 h), but originating selectively ethylglucosides and ethylgalactosides in the presence of glucose and galactose, respectively, due to the absence of necessary Lewis acid sites to isomerize aldose and proceed with dehydration.


Author(s):  
Parisa Sadeghpour ◽  
Mohammad Haghighi ◽  
Mehrdad Esmaeili

Aim and Objective: Effect of two different modification methods for introducing Ni into ZSM-5 framework was investigated under high temperature synthesis conditions. The nickel successfully introduced into the MFI structures at different crystallization conditions to enhance the physicochemical properties and catalytic performance. Materials and Methods: A series of impregnated Ni/ZSM-5 and isomorphous substituted NiZSM-5 nanostructure catalysts were prepared hydrothermally at different high temperatures and within short times. X-ray diffraction (XRD), Field emission scanning electron microscopy (FESEM), Energy dispersive X-ray (EDX), Brunner, Emmett and Teller-Barrett, Joyner and Halenda (BET-BJH), Fourier transform infrared (FTIR) and Temperature-programmed desorption of ammonia (TPDNH3) were applied to investigate the physicochemical properties. Results: Although all the catalysts showed pure silica MFI–type nanosheets and coffin-like morphology, using the isomorphous substitution for Ni incorporation into the ZSM-5 framework led to the formation of materials with lower crystallinity, higher pore volume and stronger acidity compared to using impregnation method. Moreover, it was found that raising the hydrothermal temperature increased the crystallinity and enhanced more uniform incorporation of Ni atoms in the crystalline structure of catalysts. TPD-NH3 analysis demonstrated that high crystallization temperature and short crystallization time of NiZSM-5(350-0.5) resulted in fewer weak acid sites and medium acid strength. The MTO catalytic performance was tested in a fixed bed reactor at 460ºC and GHSV=10500 cm3 /gcat.h. A slightly different reaction pathway was proposed for the production of light olefins over impregnated Ni/ZSM-5 catalysts based on the role of NiO species. The enhanced methanol conversion for isomorphous substituted NiZSM-5 catalysts could be related to the most accessible active sites located inside the pores. Conclusion: The impregnated Ni/ZSM-5 catalyst prepared at low hydrothermal temperature showed the best catalytic performance, while the isomorphous substituted NiZSM-5 prepared at high temperature was found to be the active molecular sieve regarding the stability performance.


Catalysts ◽  
2021 ◽  
Vol 11 (1) ◽  
pp. 55
Author(s):  
Katarzyna Świrk ◽  
Ye Wang ◽  
Changwei Hu ◽  
Li Li ◽  
Patrick Da Costa ◽  
...  

Copper and iron promoted ZrO2 catalysts were prepared by one-pot synthesis using urea. The studied catalysts were characterized by XRD, N2 physisorption, XPS, temperature-programmed desorption of NH3 (NH3-TPD), and tested by the selective catalytic reduction by ammonia (NH3-SCR) of NO in the absence and presence of water vapor, under the experimental conditions representative of exhaust gases from stationary sources. The influence of SO2 on catalytic performance was also investigated. Among the studied catalysts, the Fe-Zr sample showed the most promising results in NH3-SCR, being active and highly selective to N2. The addition of SO2 markedly improved NO and NH3 conversions during NH3-SCR in the presence of H2O. The improvement in acidic surface properties is believed to be the cause.


2010 ◽  
Vol 148-149 ◽  
pp. 924-928
Author(s):  
Xue Min Yan ◽  
Yuan Zhu Mi

Two kinds of mesoporous HPW/SiO2 composites, which have been synthesized respectively by the amino-functionalized (AF) method and evaporation-induced self-assembly (EISA) method, have been used as catalysts in the oxidative desulfurization process of dibenzothiophene(DBT). The catalytic performance results show that the catalyst synthesized by EISA method holds higher catalytic activity than that synthesized by the AF method. The difference of catalytic activity can be attributed to the different synthesis mechanism of two kinds of composites. In the AF method, the bonding force between HPW and SiO2 is strong acid-base interaction, which damages the Keggin structure. Whereas in the EISA process, electrostatic force and hydrogen bonds between W=O groups and Si-OH groups are main bonding forces. The hydrogen bond holds the electron-withdrawing effect, which increases the activity of nonbonding W=O groups in HPW and then results in the enhancement of the catalytic activity.


Author(s):  
Rima Tedjini ◽  
Raquel Viveiros ◽  
Teresa Casimiro ◽  
Vasco D.B. Bonifácio

Mechanosynthesis is an emergent green technology that proceeds under solventless or vestigial solvent conditions. Major advantages relay in waste reduction and lower energy consumption, without compromising or enhancing reaction conversion....


Author(s):  
Sameer Amereih ◽  
Thomas Meisel ◽  
Wolfhard Wegsheider

Two independent digestion techniques (microwave acid digestion with HF and HCl, HNO3 and Na2O2 sintering, respectively) were applied to determine the total Sb concentration in a real soil sample and in reference materials: Icelandic Basalt (BIR-1), Cody Shale (SCo-1) and (Soil-7). ICP-MS was used to determine total antimony concentrations in the digested and the extracted solutions using external calibration and isotope dilution technique. The recoveries of Sb using HF in the acids digestion mixture in closed-vessels microwave digestion system were excellent and the concentrations are in very good agreement with certified or reported concentrations of reference materials. Using closed-vessels combined with microwave heating systems probably prevents the loss of volatile Sb compounds. The use of hydrogen fluoride with other strong acid can help dissociating insoluble antimony silicates. Different extraction reagents were tested for their ability to extract antimony using an ultrasonic bath namely: EDTA disodium salt, potassium hydroxide, citric acid monohydrate, pyridine-2,6-dicarboxylic acid, ammonium acetate, ammonium oxalate, ammonium thiocyanate, ammonium persulphate and di-ammonium hydrogen citrate. A 500 mmol L-1 solution of citric acid pH 1.08 proved to be the most efficient extractant. Optimization of the extraction conditions were investigated by studying the effect of pH, concentration, temperature, time of extraction, the ratio of sample mass to the volume of extractant and the number of consecutive extractions. As a result three consecutive extractions for a total time of 45 min at 80 ˚C was the most efficient condition for Sb extraction. Using these extraction conditions 61%, 3.7% RSD and 42%, 2.2% RSD (n=6) of the total antimony in the real soil and Soil-7 samples, respectively could be extracted.


2019 ◽  
Vol 12 (01) ◽  
pp. 1850089
Author(s):  
Hou Lin Yu ◽  
Wenliang Shi ◽  
Shuaishuai Li ◽  
Junma Zhang ◽  
Xiaobo Zhang ◽  
...  

A facile, one-pot solvent-mediated hydrothermal process was adopted to prepare nickel sulfide nanoparticles decorated on reduced graphene oxide (NixSy/rGO) as electrocatalysts for hydrogen evolution reaction (HER). The designed solvent (ethylene glycol and deionized water) played a decisive role in controlling both crystalline phase and morphology of NixSy/rGO composites, leading to pure [Formula: see text]-NiS nanoparticles uniformly distributed on rGO sheets under suitable volume ratio of ethylene glycol and deionized water (2:1). The optimized [Formula: see text]-NiS/rGO showed prominent HER catalytic performance with a rather small Tafel slope of 93[Formula: see text]mV/decade and prominent current density of 10[Formula: see text]mA/cm2 at the overpotential of 177[Formula: see text]mV in alkaline environments when compared to pristine [Formula: see text]-NiS and NiS2/rGO catalysts. The excellent catalytic performance and long-term durability even after 8000 cycles confirmed the potential of [Formula: see text]-NiS/rGO composites as efficient electrocatalysts for HER in the alkaline media.


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