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1.
To develop a novel catalyst system that has excellent olefin reduction capability for FCC gasoline without loss in octane number, different catalysts supported on multiple composite carriers consisting of SAPO-11, Hβ, HMOR and HZSM-5 were prepared and their catalytic performances for FCC gasoline upgrading were assessed in the present investigation. The pore structure and acidity of the catalysts were characterized by N2 adsorption and pyridine adsorption FTIR, respectively. Based on the results obtained over the catalysts supported on binary-zeolite carriers (Hβ/HZSM-5, HMOR/HZSM-5 and SAPO-11/HZSM-5) using FCC gasoline as the feedstock, various multiple-zeolite supported catalysts were developed from different combinations of the binary-zeolite systems. It was found that the SAPO-11/HMOR/β/ZSM-5 quadruple composite zeolite supported catalyst gave higher liquid yield, improved gasoline RON, and lower coke deposit amount for the hydro-upgrading of FCC gasoline and thus can be considered as a potential catalyst system. A comprehensive analysis based on the catalytic activities and acidity measurements revealed that acid strength and acid type were two very important factors influencing hydroisomerization and aromatization activities, and the difference in catalyst acid strength determined which factor predominates. 相似文献
2.
Nianhua Xue Lei Nie Dongmei Fang Xuefeng Guo Jianyi Shen Weiping Ding Yi Chen 《Applied Catalysis A: General》2009,352(1-2):87-94
Synergistic catalysis effects among tungsten, phosphorus and HZSM-5 on 1-butene cracking to propene and ethene have been demonstrated by catalytic tests. The tungsten–phosphorus-modified HZSM-5 (W–P/HZSM-5) catalyst, with very low density of acid sites, offers a fairly high conversion rate of butene and selectivity to propene. The status of doped tungsten is characterized by using techniques of D2/OH exchange, NH3 adsorption microcalorimetry, FT-IR spectroscopy, Raman spectroscopy, N2 adsorption and X-ray photoelectron spectroscopy. The tungsten would be monotungstate that interacted with phosphorus before steam treatment and partly congregated to polytungstate species during steaming process at high temperature. The enhanced performance of the catalyst for 1-butene cracking to propene and ethene can be correlated to the synergistic effect between the doped tungsten and phosphorous on the reaction network of the cracking process. The W–P/HZSM-5 is a promising catalyst for the 1-butene cracking to propene and ethene. 相似文献
3.
Cu–Fe–La/HZSM-5 and Cu–Fe–Ce/HZSM-5 bifunctional catalysts were prepared and applied for the direct synthesis of dimethyl ether (DME) from CO2 and H2. The catalysts were characterized by X-ray diffraction (XRD), N2 adsorption–desorption, H2-temperature programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS). The results showed that La and Ce significantly decreased the outer-shell electron density of Cu and improved the reduction ability of the Cu–Fe catalyst in comparison to the Cu–Fe–Zr catalyst, which may increase the selectivity for DME. The Cu–Fe–Ce catalyst had a greater specific surface area than the Cu–Fe–La catalyst. This promoted CuO dispersion and decreased CuO crystallite size, which increased both the DME selectivity and the CO2 conversion. The catalysts were stable for 15 h. 相似文献
4.
In order to develop a novel catalyst system that has excellent olefin reduction ability for FCC gasoline without loss in research
octane number (RON), different catalysts supported on single- and binary-zeolite carriers consisting of Hβ or/and HZSM-5 were
prepared and their catalytic performances for FCC gasoline upgrading were assessed in the present investigation. Acidity measurements
by pyridine-adsorbed Fourier transformed infrared spectroscopy (FTIR) showed that hydroisomerization and aromatization activities
were closely related to the density of acid sites and the ratios of medium Lewis acidity and strong Br?nsted acidity to total
acidity. Compared with the single HZSM-5 supported catalyst, the single Hβ supported catalyst was found to have much better
olefin reduction performance, but the product RON still suffered from a loss of 1.6. Compared to the single-zeolite supported
catalysts, the binary-zeolite Hβ/HZSM-5 supported catalysts with the mass ratio of Hβ to HZSM-5 at 6.6 offered much more stable
activity and selectivity to arene, which played an important role in preserving gasoline RON. 相似文献
5.
Zhang Peiqing Wang Xiangsheng Guo Xinwen Guo Hongchen Zhao Leping Hu Yongkang 《Catalysis Letters》2004,92(1-2):63-68
Nanoscale HZSM-5 zeolite was hydrothermally treated with steam containing 0.8 wt% NH3 at 773 K and then loaded with La2O3 and NiO. Both the parent nanoscale HZSM-5 and the modified nanoscale HZSM-5 zeolites catalysts were characterized by TEM, XRD, IR, NH3-TPD and XRF, and then the performance of olefins reduction in fluidized catalytic cracking (FCC) gasoline over the modified nanoscale HZSM-5 zeolite catalyst was investigated. The IR and NH3-TPD results showed that the amount of acids of the parent nanoscale HZSM-5 zeolite decreased after the combined modification, so did the strong acid sites deactivating catalysts. The stability of the catalyst was still satisfactory, though the initial activity decreased a little after the combined modification. The modification reduced the ability of aromatization of nanoscale HZSM-5 zeolite catalyst and increased its isomerization ability. After 300 h onstream, the average olefins content in the gasoline was reduced from 56.3 vol% to about 20 vol%, the aromatics (C7–C9 aromatics mainly) and paraffins contents in the product were increased from 11.6 vol% and 32.1 vol% to about 20 vol% and 60 vol% respectively. The ratio of i-paraffins/n-paraffins also increased from 3.2 to 6.6. The yield of gasoline was obtained at 97 wt%, while the Research Octane Number (RON) remained about 90. 相似文献
6.
《Applied Catalysis A: General》2001,205(1-2):195-199
Reaction between ethanol and ammonia have been studied on various zinc oxide modified HZSM-5 (Si/Al=225) catalysts under various conditions of temperature, C/N ratio of the reactants and their WHSV. Two pure zinc oxides were taken for the study. One was a highly active acidic form Z1 and the other was a stoichiometric non acidic zinc oxide Z2. The activity of the catalysts for ammonolysis reaction followed the order Z2⪡Z1⪡HZSM-5. However, for composite catalysts containing 10–40% Z1 on HZSM-5, the activity increased synergistically and became maximum (∼81% conversion of alcohol) for the catalyst 40% Z1/HZSM-5 and about 50% conversion for the catalyst 40% Z2/HZSM-5. The products formed were mainly N-heterocycles. Some novel high molar mass N-heterocycles were also detected. The catalytic activity and product selectivity was crucially affected by the reaction conditions, particularly the effect of temperature; the optimum yield of the products was obtained at the catalyst temperature of 723 K, C/N ratio 0.3892 and WHSV of 2.5 h−1. 相似文献
7.
Xiuying Lin Yu Fan Zhihong Liu Gang Shi Haiyan Liu Xiaojun Bao 《Catalysis Today》2007,125(3-4):185-191
This article describes a novel modification method consisting of steaming and subsequent citric acid leaching to finely tune acidity and pore structure of HZSM-5 zeolite and thereby to enhance the on-stream stability of the zeolite derived fluid catalytic cracking (FCC) gasoline hydro-upgrading catalyst. A series of dealuminated HZSM-5 zeolites and their derived catalysts were prepared and characterized by X-ray diffraction (XRD), X-ray fluorescence spectroscopy (XRF), 27Al MAS NMR, nitrogen adsorption, temperature programmed desorption of ammonium (NH3-TPD) and infrared (IR) spectroscopy of chemisorbed pyridine. The results showed that the citric acid leaching could preferentially remove the extra-framework Al (EFAl) species formed by steaming treatment and thus reopen the EFAl-blocked pore channels of the steamed zeolite. The steaming treatment at a suitable temperature and subsequent citric acid leaching not only decreased the strength of acid sites to a desirable degree but also increased the ratio of medium and strong Lewis acidity to medium and strong Brönsted acidity, both of which conferred the resulting catalyst with superior selectivity to aromatics, good hydroisomerization activity and gasoline research octane number (RON) preservability, as well as enhanced on-stream stability. The results fully demonstrated that the treatments by steaming and followed citric acid leaching can serve as an important method for adjusting the physicochemical properties of HZSM-5 zeolite. 相似文献
8.
Marcelo J.B. Souza Fabiano A.N. Fernandes Anne M.G. Pedrosa Antonio S. Araujo 《Fuel Processing Technology》2008
This work presents a study on the catalytic cracking of natural gasoline (extracted from natural gas) over HZSM-5 zeolite. A factorial planning was carried out to evaluate the effect of temperature and W/F ratio on the cracking of natural gasoline, analyzing their effects on conversion and product distribution using an analysis based on surface response methodology. The process was optimized focusing on the maximization of the mass fractions and the production of specific products such as ethene, propene and butanes. The results have shown that the maximum selectivity and hourly mass production of ethene is obtained at high temperature (450 °C) and low catalyst weight to flow rate ratio (W/F) (7.2 to 8.2 gcat h/mol). Maximum selectivity of propene is obtained at 350 °C and 7.0 gcat h/mol, while the best condition for maximum mass production is found at 421 °C and 5.7 gcat h/mol. The highest mass production of butanes is favored by high temperature (450 °C) and mid range W/F ratios (12.1 gcat h/mol), while the highest selectivity is found at low temperature (350 °C). 相似文献
9.
A series of gallium-containing HZSM-5 zeolites with different Ga contents (Ga/(Al+Ga)?=?0.1?C0.6) were prepared by hydrothermal in situ synthesis and post synthesis. Their catalytic performance were compared in the aromatization of propane, butane and propane/butane mixture (1:1?molar). Galloaluminosilicate obtained via hydrothermal in situ synthesis exhibited high fraction of acidic framework Ga3+ with few dispersed extracrystalline Ga2O3. Ga/HZSM-5 obtained by post synthesis showed the presence of extracrystalline Ga2O3 and/or extra framework gallyl ions. The aromatization performance of Ga-containing HZSM-5 followed the following sequence; galloaluminosilicate > Ga/HZSM-5 (ion-exchange) > Ga/HZSM-5 (impregnation) ? HZSM-5. Optimum aromatization performance over galloaluminosilicate was achieved with Ga/(Al+Ga) ratio of 0.3. Propane conversion reached 50.9?wt% over galloaluminosilicate with Ga/(Al+Ga) of 0.3, as compared to 31.8 and 40.7?wt% for the corresponding Ga/HZSM-5 obtained by impregnation and ion-exchange, respectively, at gas hourly space velocity of 1,600?h?1, and 540?°C. Comparison of aromatic selectivity at the same conversion level (~10.0?wt%) revealed that galloaluminosilicate is more selective than Ga/HZSM-5. The superior performance of galloaluminosilicate was attributed to the presence of highly dispersed-reducible extra-framework Ga2O3 (Lewis-dehydrogenating sites) formed by degalliation in close proximity to zeolitic Br?nsted sites. Thus, hydrothermal in situ approach can thus be considered as an effective method for improving the aromatization performance of HZSM-5. 相似文献
10.
Synthesis of ZSM-5/SAPO-11 composite and its application in FCC gasoline hydro-upgrading catalyst 总被引:2,自引:0,他引:2
This article describes the synthesis, characterization and application of a novel aluminosilicate/silicoaluminophosphate composite zeolite ZSM-5/SAPO-11. The composite was synthesized by the in situ overgrowth of SAPO-11 on ZSM-5 and was characterized by means of X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transformed infrared (FT-IR) spectrometry, N2 adsorption and infrared spectroscopy of adsorbed pyridine. The results were compared with those of the mechanical mixture composed of individual ZSM-5 and SAPO-11. In the mechanical mixture, the ZSM-5 phase was morphologically separate from the SAPO-11 phase, while the ZSM-5/SAPO-11 composite existed in a form of a core-shell structure, with the ZSM-5 phase as the core and the SAPO-11 phase as the shell. Compared with the mechanical mixture, the composite had more mesopores and moderate acidity distribution, which could accelerate the diffusion of substances and enhance the synergetic effect between Brönsted and Lewis acids. The comparison of the catalytic performances of the mechanical mixture and the composite-based Ni–Mo catalysts for FCC gasoline hydro-upgrading showed that, due to the above advantages of the composite, the corresponding catalyst yielded improved gasoline research octane number, high liquid yield, good desulfurization activity and lower coke amount and thus could be considered as a potential catalyst system for hydro-upgrading FCC gasoline. 相似文献
11.
The preparation of light alkenes by the gas phase oxidative cracking (GOC) or catalytic oxidative cracking (COC) of model high hydrocarbons (hexane, cyclohexane, isooctane and decane in the GOC process and hexane in the COC process) was investigated in this paper. The selection for the feed in the GOC process was flexible. Excellent conversion of hydrocarbons (over 85%) and high yield of light alkenes (about 50%) were obtained in the GOC of various hydrocarbons including cyclohexane at 750°C. In the GOC process, the utilization ratio of the carbon resources was high; CO dominated the produced CO X (the selectivity to CO2 was always below 1%); and the total selectivity to light alkenes and CO was near or over 70%. In the COC of hexane over three typical catalysts (HZSM-5, 10% La2O3/HZSM-5 and 0.25% Li/MgO), the selectivity to CO X was hard to decrease and the conversion of hexane and yield of light alkenes could not compete with those in the GOC process. With the addition of H2 in the feed, the selectivity to CO X was reduced below 5% over 0.1% Pt/HZSM-5 or 0.1% Pt/MgAl2O4 catalyst. The latter catalyst was superior to the former catalyst due to its perfect performance at high temperature, and with the latter, excellent selectivity to light alkenes (70%) and the conversion of hexane (92%) were achieved at 850°C (a yield of light alkenes of 64%, correspondingly). 相似文献
12.
Xin Zhang Jin Zhong Jianwei Wang Linhui Zhang Junkui Gao Aisong Liu 《Fuel Processing Technology》2009,90(7-8):863-870
A series of Ni-doped HZSM-5 catalysts were prepared and the catalytic performance of these catalysts in n-butene trimerization was investigated. The Ni-loading, the Si/Al ratio of HZSM-5 and the reaction conditions (temperature, pressure and WHSV) played great influences on the catalytic performance of these catalysts in the reaction. 77.5 wt.% conversion of n-butene and 50.5 wt.% selectivity of trimers as well as 19.6 × 10? 2 gtrimers/(gcat h) yield of trimers were obtained on 1NiHZSM-5(320) catalyst up to 148 h at 420 °C, WHSV = 2 h? 1 and 1.0 MPa. In addition, the physicochemical properties of these catalysts were comparatively characterized by powder X-ray diffraction (XRD), N2 isothermal adsorption–desorption, infrared red spectroscopy (IR) and pyridine adsorbed infrared red spectroscopy (Py-IR) techniques. The doping of Ni into HZSM-5(320) modified the specific surface area and the acidity of these catalysts, which in turn affected the catalytic performance of these catalysts in n-butene trimerization. The acidic amount and the ratio of Lewis/Brönsted acid sites (L/B) on the external surface of these catalysts were close relative to the catalytic performance of these catalysts. 1NiHZSM-5(320) catalyst showed the highest catalytic performance in n-butene trimersization among the investigated catalysts because it had the proper acidic amount and the proper L/B ratio on its external surface. 相似文献
13.
Aromatization of hexane and propane was investigated over Pt promoted mesoporous gallium-containing HZSM-11 with controlled mesoporosity generated by desilication. Prepared catalysts were characterized by nitrogen adsorption, X-ray powder diffraction, scanning electron microscopy, Fourier transform infrared of chemisorbed pyridine, and NH3 temperature programmed desorption confirming the development of intracrystalline mesoporosity of Ga-containing HZSM-11. The catalytic activities, which were compared in the aromatization of n-hexane and propane, increased upon desilication. The aromatization of n-hexane decreased in the following order, Pt/mesoporous GaZSM-11 ? Pt/conventional GaZSM-11 ? mesoporous GaZSM-11 > conventional GaZSM-11. Hexane conversion reached 70.1% over mesoporous Pt/GaZSM-11 with Si/Ga of 61, as compared with 29.6 and 24.9% for corresponding mesoporous and conventional GaZSM-11 (Si/Ga = 94), respectively, for experiments at liquid hour space velocity of 3.6 h−1, and 540 °C. Comparison of BTX (benzene-toluene-xylene) selectivity at the conversion level of ∼21.0% revealed that Pt/mesoporous GaZSM-11 is more selective than corresponding mesoporous and conventional GaZSM-11. The BTX selectivity over Pt/mesoporous GaZSM-11 (Si/Ga = 94), which showed strong dependence on the conversion, reached 28.2%, whereas over corresponding mesoporous and conventional GaZSM-11catalysts reached 19.1% and 5.5%, respectively. A higher conversion and better selectivity can be attributed to the improved accessibility to the active extra-framework Ga species owing to the generation of mesopores inside the zeolite particles and shortening the contact time. It is worth mentioning that the prepared catalysts exhibited quite low activity in propane aromatization but exhibiting similar trends as for hexane aromatization. 相似文献
14.
Catalytic synthesis of ethylbenzene by alkylation of benzene with diethyl oxalate was carried out over HZSM-5 with Si/Al ratios from 50 to 250. The catalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), ammonia temperature-programmed desorption (NH3-TPD) and pyridine IR techniques. As revealed by the results of NH3-TPD and pyridine IR spectra, a significant decrease in acidic strength and the number of acidic sites is observed with increasing Si/Al ratio from 50 to 250. The benzene conversion and ethylbenzene selectivity increases obviously with increasing Si/Al ratio from 50 to 200. With a further increase in Si/Al ratios, a slight decrease in the conversion of benzene and selectivity for ethylbenzene is detected, indicating that a proper acidic strength was required in this reaction. In addition, the effects of temperature and feed ratio on the catalytic activity and product distributions are also investigated in this study. 相似文献
15.
Iron-modified HZSM-5 materials were prepared by the impregnation techniques at ambient temperature and characterized by X-ray powder diffraction (XRD) and ICP-MS to determine the phase structure and loadings of iron dioxide. This material was tested for solvent-free catalytic oxidation of toluene under mild conditions. The result shows that Fe2O3/HZSM-5 is an effective catalyst, exhibiting 17.3% conversion of toluene, 51.4% selectivity to benzaldehyde at 90 °C. Furthermore, the catalyst can be easily recovered and reused for three times without a significant loss in its activity and selectivity. 相似文献
16.
17.
Nanoscale HZSM-5 zeolite was hydrothermally treated with ammonia water at different temperatures and then loaded with La2O3 and ZnO. The parent and the modified nanoscale HZSM-5 catalysts were characterized by SEM, NH3-TPD, IR and XRF. The performance of the modified HZSM-5 catalysts for FCC gasoline upgrading was evaluated in a fixed bed reactor in the presence of hydrogen. The results indicated that the modified catalyst which was hydrothermally treated at 400 °C exhibited excellent aromatization activity, isomerization activity and higher ability of reducing olefin content in FCC gasoline. Under the given reaction conditions, the olefin content in FCC gasoline could be decreased from 49.6 to 8.1 vol.%. The catalytic performance of the modified nanoscale ZSM-5 catalyst hardly changed within 300 h time on stream, and the research octane number (RON) of gasoline was preserved. 相似文献
18.
Direct synthesis of hydrogen peroxide (DSHP) was studied over Pd loaded on HZSM-5 nanosheets (Pd/ZN). Pd nanoparticles with average size of ca. 4.3 nm were introduced into the adjacent nanosheet layers (thickness of ca. 2.9 nm) by impregnation method. Pd/ZN with theoretical Si/Al molar ratio of 25 showed the highest selectivity for H2O2 among the prepared catalysts, together with highest formation rate of H2O2 (38.0 mmol·(g cat)−1·h−1), 1.9 times than that of Pd supported on conventional HZSM-5 zeolite (Pd/CZ-50). Better catalytic performance of nanosheet catalysts was attributed to the promoted Pd dispersion which promoted H2 dissociation, more Brønsted acid sites and stronger metal-support interaction which inhibited the dissociation of OO bond in H2O2. The embedded structure sufficiently protected the Pd nanoparticles by space confinement which restrained the Pd leaching, leading to a better catalytic stability with 90% activity retained after 3 cycles, which was almost 3 times than that of Pd/CZ-50 (30.4% activity retained). 相似文献
19.
An investigation of the potential interest of α-alumina-hematite foams, as opposed to powders, as starting materials for the synthesis of carbon nanotubes (CNTs) by catalytic chemical vapor deposition method was performed. The oxide powders and foams as well as the corresponding CNT-Fe-Al2O3 composite powders and foams are studied by X-ray diffraction, specific surface area measurements, electron microscopy, Raman spectroscopy and Mössbauer spectroscopy. The latter technique revealed that four components (corresponding to α-Fe, Fe3C, γ-Fe-C and Fe3+) were present in the Mössbauer spectra of the composite powders, and that an additional sextet, possibly due to an Fe1−yCy alloy, is also present in the Mössbauer spectra of the composite foams. Contrary to some expectations, using foams do not lead to an easier reduction and thus to the formation of more α-Fe, Fe3C and/or γ-Fe-C potentially active particles for the formation of CNTs, and hence to no gain in the quantity of CNTs. However, using foams as starting materials strongly favors the selectivity of the method towards SWCNTs (60% SWCNTs and 40% DWCNTs) compared to what is obtained using powders (5% SWCNTs, 65% DWCNTs and 30% MWCNTs). 相似文献
20.
Qiang Sun Hongxia Gao Yu Mao Teerawat Sema Sen Liu Zhiwu Liang 《American Institute of Chemical Engineers》2022,68(8):e17706
High heat duty is an urgent challenge for industrial applications of amine-based CO2 capture. The temperature (>110°C) of carbamate breakdown in amine regeneration requires large energy consumption. In this work, we report a novel, stable, efficient, and inexpensive Ni-HZSM-5 catalyst to improve the CO2 desorption rate and reduce the heat duty. The impregnation method was applied for varying nickel content in the catalysts from 2.16 to 9.80 wt% in HZSM-5. The catalysts were characterized by scanning electron microscope, X-ray powder diffraction, N2 adsorption–desorption, inductively coupled plasma-optical emission spectrometry, ultraviolet-visible diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, NH3-temperature programmed desorption (TPD), Infrared spectroscopy of pyridine adsorption, and Fourier transform infrared spectroscopy. The catalytic performance was evaluated by CO2 desorption of rich amine solvent at 90°C. It was found that the introduction of nickel increased the acid sites of catalysts compared with parent HZSM-5. This phenomenon plays a key role on improving the CO2 desorption rate. The density functional theory (DFT) calculations successfully explain the catalytic performance. The catalytic activity associates with the combined properties of MSA × B/L × Ni2+. The 7.85-Ni-HZ catalyst presents an excellent catalytic activity for the CO2 desorption: it increases the amount of desorbed CO2 up to 36%, reduces the relative heat duty by 27.07% with the same reaction time, and possesses high stability during five cyclic tests. A possible catalytic mechanism for the Ni-HZSM-5 catalysts through assisting carbamate breakdown and promoting CO2 desorption is proposed based on experimental results and theoretical calculations. Therefore, the results present that the 7.85-Ni-HZ catalyst significantly accelerates the protons transfer in CO2 desorption and can potentially apply in industrial CO2 capture. 相似文献