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1.
Ailing Sun Zhangfeng Qin Shuwei Chen Jianguo Wang 《Journal of molecular catalysis. A, Chemical》2004,210(1-2):189-195
The dehydrogenation of ethylbenzene (EB) to styrene (ST) in the presence of carbon dioxide instead of steam is believed to be an energy-saving and environmentally friendly process. However, the reaction mechanism for this coupling system still remains unclear. Therefore, the role of carbon dioxide was investigated by means of catalytic reactions and temperature-programmed desorption (TPD) of carbon dioxide over a series of Fe and V supported catalysts as well as thermodynamic analysis. The results showed that the ethylbenzene conversion is associated with the conversion of carbon dioxide, and that there exists a synergistic effect between the ethylbenzene dehydrogenation and the reverse water–gas shift. However, the difference in the behaviour of the catalysts between the single reverse water–gas shift and the coupled ethylbenzene dehydrogenation may suggest that the catalysts are different in the reaction mechanisms for the coupled ethylbenzene dehydrogenation. Carbon dioxide can be activated through either basic sites or redox sites on the catalyst. Based on these results, the role of carbon dioxide and reaction mechanisms are proposed. 相似文献
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镧-镍复合氧化物纳米微粒的固相合成及其催化性能 总被引:4,自引:0,他引:4
The La-Ni complex oxide catalyst was prepared by solid state reactions under microwave. The structure and reducibility of the catalyst were characterized by using TG-DTA, XRD, TEM and TPR methods. At the same time the catalytic activity of oxidative dehydrogenation of ethylbenzene to styrene with carbon dioxide over the complex oxide nanoparticle was investigated.The Results show that the product is K2NiF4 nanoparticles,and the size is 13nm.The complex oxide sample had high activity for the oxidative dehydrogenation of ethylbenzene to styrene. 相似文献
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John M. Stubbs 《Fluid Phase Equilibria》2011,305(1):76-82
The partitioning of ethylbenzene between poly(ethylene glycol) (PEG) and supercritical carbon dioxide was studied at 308.15, 328.15 and 348.15 K and 10, 15.5 and 20 MPa with PEG-400, 600 and 900 using Monte Carlo molecular simulation. The effect of a cosolvent was also studied with either 5% ethane or 5% n-octane added. Ethylbenzene favored the supercritical phase most when the density was highest, and while ethane had little effect, the addition of n-octane increased the amount of solute dissolved in carbon dioxide. Increasing polymer molecular weight led to more solute in the PEG-rich phase. This coincides with a higher amount of dissolved carbon dioxide that preferentially solvates ethylbenzene. 相似文献
6.
Jong-San Chang Do-Young Hong Vladislav P. Vislovskiy Sang-Eon Park 《Catalysis Surveys from Asia》2007,11(1-2):59-69
Utilization of carbon dioxide as a soft oxidant for the catalytic dehydrogenation of ethylbenzene (CO2-EBDH) has been recently attempted to explore a new technology for producing styrene selectively. This article summarizes
the results of our recent attempts to develop effective catalyst systems for the CO2-EBDH on the basis of alumina-supported vanadium oxide catalysts. Its initial activity and on-stream stability were essentially
improved by the introduction of antimony oxide as a promoter into the alumina-supported catalyst. Insertion of zirconium oxide
into alumina support substantially increased the catalytic activity. Modification of alumina with magnesium oxide yielded
an increase of catalyst stability of alumina-supported V–Sb oxide due to the coking suppression. Carbon dioxide has been confirmed
to play a beneficial role of selective oxidant in improving the catalytic performance through the oxidative pathway, avoiding
excessive reduction and maintaining desirable oxidation state of vanadium ion (V5+). The positive effect of carbon dioxide in dehydrogenation reactions of several alkylbenzenes such as 4-diethylbenzene, 4-ethyltoluene,
and iso- and n-propylbenzenes was also observed. Along with the easier redox cycle between fully oxidized and partially reduced vanadium
species, the optimal surface acidity of the catalyst is also responsible for achieving high activity and catalyst stability.
It is highlighted that supra-equilibrium EBDH conversions were obtained over alumina-supported V–Sb oxide catalyst in CO2-EBDH as compared with those in steam-EBDH in the absence of carbon dioxide. 相似文献
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Styrene (STY) is now produced industrially in fairly large quantities by the dehydrogenation of ethylbenzene (EB) using promoted iron oxide catalyst with superheated steam.In this case, small amount of carbon dioxide formed as a by-product was known to inhibit the catalytic activity of commercial catalyst. Recently, there have been some reports which carbon dioxide showed positive effects to promote catalytic activities on the reaction over several catalysts.In this study, we attempted to combine the dehydrogenation of EB to STY with the carbon dioxide shift-reaction. The combine reaction (EB + CO2 → STY + H2O + CO) can be considered as one of the ways of using CO2 resources and can yield simultaneously STY and Carbon oxide.Alumina oxide catalysts such as Al2O3, Na2O/Al2O3 and K2O/Al2O3 were prepared by the usual impregnation method with an aqueous solution of NaNO3 and KNO3, and then calcined at 650℃ for 5 h in a stream of air. The reaction condition is 600℃, flow of CO2 38ml/mon and space velocity (EB) 1.28h-1. 相似文献
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G. V. Isagulyants L. I. Kovalenko A. A. Greish T. N. Shakhtakhtinskii F. V. Aliev R. R. Khankishev A. D. Kuliev 《Russian Chemical Bulletin》1986,35(4):707-710
Conclusions It has been shown by application of the kinetic isotope method that in the oxidative dehydrogenation of ethylbenzene to styrene on a magnesium ferrite catalyst, benzene and toluene are formed from ethylbenzene and also from styrene. Carbon dioxide appears mainly as a result of exhaustive oxidation of the side chain of the aromatic hydrocarbon.Translated from Izvestiya Akademii Nauk SSSR, Seriya Khimicheskaya, No. 4, pp. 778–781, April, 1986. 相似文献
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The dehydrogenation of isobutane (IB) to produce isobutene coupled with reverse water gas shift in the presence of carbon dioxide was investigated over the catalyst Cr2O3 supported on active carbon (Cr2O3/AC). The results illustrated that isobutane conversion and isobutene yield can be enhanced through the reaction coupling in the presence of carbon dioxide. Moreover, carbon dioxide can partially eliminate carbonaceous deposition on the catalyst and keep the active phase (Cr2O3), which are then helpful to alleviate the catalyst deactivation. 相似文献
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《Reaction Kinetics and Catalysis Letters》2003,80(2):359-364
The effect of zinc on the performance of hematite-based catalysts in ethylbenzene dehydrogenation was studied. Zinc acts as
a structural promoter stabilizing the active phase of the catalysts.
This revised version was published online in June 2006 with corrections to the Cover Date. 相似文献
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Cuong Duong-Viet Housseinou Ba Yuefeng Liu Lai Truong-Phuoc Jean-Mario Nhut Cuong Pham-Huu 《催化学报》2014,35(6):906-913
A hierarchical metal-free catalyst consisting of nitrogen-doped carbon nanotubes decorated onto a silicon carbide (N-CNTs/SiC) macroscopic host structure was prepared. The influence of N-CNTs incorporation on the physical properties of the support was evaluated using different characterization techniques. The catalyst was tested as a metal-free catalyst in the selective oxidation of H2S and steam-free dehydrogenation of ethylbenzene. The N-CNTs/SiC catalyst exhibited extremely good desulfurization performance compared to a Fe2O3/SiC catalyst under less conducive reaction conditions such as low temperature, high space velocity, and a low O2-to-H2S molar ratio. For the dehy-drogenation of ethylbenzene, a higher dehydrogenation activity was obtained with the N-CNTs/SiC catalyst compared to a commercial K-Fe/Al2O3 catalyst. The N-CNTs/SiC catalyst also displayed good stability as a function of time on stream for both reactions, which was attributed to the strong anchoring of the nitrogen dopant in the carbon matrix. The extrudate shape of the SiC support allowed the direct macroscopic shaping of the catalyst for use in a conventional fixed-bed reactor without the problems of catalyst handling, transportation, and pressure drop across the catalyst bed that are encountered with nanoscopic carbon-based catalysts. 相似文献
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The role of lattice oxygen in the catalytic dehydrogenation of ethylbenzene over industrial iron-oxide-based catalysts has been investigated mainly by means of isotopic exchanges attending the dehydrogenation reaction.The results indicated that although the exchange of lattice oxygen with steam oxygen appeared to take place to an appreciable extent,the direct catalytic dehydrogenation of ethylbenzene appeared to be the major reaction pathway,with catalytic dehydrogenation by oxygen-transfer reaction pathway playing only a minor role,as revealed different extents of hydrogeh-deute-rium isotopic exchange between ethylbenzene and steam D2Q at low and very high space velocities.The mechanisms of these two reaction pathways are discussed.For the oxygen-transfer dehydrogenation mechanism,electron transport between neighboring Active-sites operating cooperatively in opposite phases of their redox cycles may be a requisite factor. 相似文献
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采用快速动态法制备了具有MFI结构的硅铁沸石分子筛,研究了该分子筛上乙苯脱氢反应的瞬变行为.结合表面吸附态的红外、顺磁结果发现,苯乙烯通过化学活性吸附的乙苯脱氢形成.通过这个模型可满意地解释瞬态曲线和稳态下的动力学行为. 相似文献
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Carbon mediated catalysis has gained an increasing attention in both areas of nanocatalysis and nanomaterials. The progress in carbon nanomaterials provides many new opportunities to manip-ulate the types and properties of active sites of catalysts through manipulating structures, function-alities and properties of carbon surfaces. The present review focuses on progresses in carbon medi-ated oxidative dehydrogenation reactions of ethylbenzene, propane, and butane. The state-of-the-art of the developments of carbon mediated catalysis is discussed in terms of fundamental studies on adsorption of oxygen and hydrocarbons, reaction mechanism as well as effects of carbon nano-material structures and surface functional groups on the catalytic performance. We highlight the importance and challenges in tuning of the electron density of carbon and oxygen on carbon surfac-es for improving selectivity in oxidative dehydrogenation reactions. 相似文献
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Summary The dehydrogenation of isobutane to isobutene in the presence of carbon dioxide was carried out over supported vanadium oxide
catalysts. The influence of the support on the catalytic performance was investigated. The isobutane conversion and isobutene
selectivity in the presence of carbon dioxide were compared with the results obtained during the dehydrogenation reaction
in the presence of helium (inert gas). The catalysts were characterized by temperature-programmed techniques (TPR, TPD-NH3, TPD-CO2). 相似文献
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采用TG、XRD、SEM、EDAX和脉冲色谱技术,研究了Ni/Al2O3和Ni/ARM催化剂的甲烷脱氢积炭反应特征。结果指出,甲烷脱氢反应的积炭行为与催化剂上镍的分散状态有关。Ni-2催化剂上Ni的分散度小,晶粒大,甲烷脱氢形成的炭丝较长,主要以石墨型炭游离存在:而Ni/ARM催化剂上Ni的分散度大,镍晶粒小,甲烷脱氢形成的炭丝较短,主要覆盖在催化剂活性中心表面。甲烷脱氢主要产生无定型炭和石墨型炭,其中无定型炭可以被CO2部分消除。在催化剂制备时,通过提高镍在催化剂表面的分散度,减小镍的晶粒大小,不仅可以提高催化剂的活性,而且可以提高CO2对积炭的消炭性能。 相似文献
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The activity of the vanadium-magnesium oxide catalyst was tested in the reaction of isobutane dehydrogenation reaction in
the presence and absence of carbon dioxide. The data were compared with the results obtained in the Boudouard and the reverse
water gas shift reactions. It has been found that carbon oxide is produced with both RWGS reactions coupled with the simple
dehydrogenation of isobutane (i.e., two-step pathway) and the one-step oxidative dehydrogenation reaction. 相似文献
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XRD研究表明 ,作为乙苯脱氢催化剂中的氧化铁活性组分 ,具有反式尖晶石结构的Fe3O4 比刚玉型的α Fe2O3 更易与钾助催化剂发生相互作用 :α Fe2O3-K2O需经850℃煅烧才能生成多铁酸钾 ,但在Fe3O4 -K2O体系中只需700℃即可.而且 ,钾还可抑制Fe3O4 被氧化为α Fe2O3 的进程 ,在空气中 ,Fe3O4 只需300℃煅烧即可明显转化为α Fe2O3 ,但同样的转化在Fe3O4 K2O体系中要经700℃煅烧才会明显地发生.实验结果表明 ,某种形态的多铁酸钾可能是催化剂中的储钾相. 相似文献
20.
Yoshihiko Ohishi Tomonori Kawabata Tetsuya Shishido Ken Takaki Qinghong Zhang Ye Wang Katsuomi Takehira 《Journal of molecular catalysis. A, Chemical》2005,230(1-2):49-58
M-MCM-41 catalysts (M: V, Cr, Fe, and Ga) prepared by direct hydrothermal synthesis (DHT) have been tested for dehydrogenation of ethylbenzene with CO2. The synthesized materials were characterized by X-ray diffraction (XRD), N2 adsorption (77 K), and diffuse reflectance UV–vis spectroscopic measurements. Cr-MCM-41 showed the highest activity among M-MCM-41 catalysts tested, resulting in the production of styrene with the conversion of 65% and the selectivity above 90%. The rate of styrene formation increased with increasing Cr loading up to 1.7 wt.%. It is suggested that Cr(VI)O4 in tetrahedral coordination is formed as an active monochromate species and reduced to Cr(III)O6 in octahedral coordination as a less active polychromate species during the reaction. Deactivated catalyst was regenerated by a treatment with gaseous oxygen or CO2, during which redistribution as well as reoxidation of polymeric Cr(III)O6 octahedra to monomeric Cr(VI)O4 tetrahedra was observed. The rate of CO formation increased together with that of styrene formation, while the rate of H2 formation decreased, with increasing partial pressure of CO2. It was confirmed that reverse water-gas shift reaction took place over Cr-MCM-41 by a separate experiment. The rate of CO formation during the dehydrogenation of ethylbenzene with CO2 over Cr-MCM-41 was well accounted for by assuming parallel occurrence of two reactions, i.e., direct oxidative dehydrogenation of ethylbenzene with CO2 and simple dehydrogenation of ethylbenzene thermodynamically assisted by reverse water-gas shift reaction. 相似文献