Fiber glass supported catalysts and pure platinum: laser ignition of catalytic combustion of propane

A pure platinum (Pt) catalyst and a new industrial catalyst, the silica fiber glass catalyst (SFGC) doped with only 0.2% Pt, were studied and compared. For propane–air catalytic combustion, the ignition of the reaction and its stability were investigated. The reaction, ignited by a laser beam, propagated as a wave front with constant amplitude and velocity along both catalysts, 10 mm/s for Pt, and 1–2 mm/s for SFGC. Laser ignition thresholds and the parameter space for front propagation were determined for both catalysts. Spatial instability (resulting in the destruction of the homogeneous regime of combustion and in the formation of hot spots) was found for Pt, but not for SFGC. The new catalyst (SFGC) containing only 10^–3 of Pt has the same catalytic activity as pure Pt and better spatial stability.     

用于丙烷催化燃烧的PdxPty-ZSM-5/Cordierite整体式催化剂

以ZSM-5分子筛、铝溶胶、硝酸钯、硝酸铂和水为原料制备分子筛浆料，采用真空抽提-一次涂覆法在堇青石蜂窝陶瓷载体表面制备出Pd_xPt_y-ZSM-5/Cordierite整体式催化剂，考察了Pd负载量、ZSM-5分子筛的硅铝比和Pd/Pt质量比对整体式催化剂的丙烷催化燃烧性能的影响，并用超声波振荡、SEM、XRD、H₂-TPR和C₃H₈-TPD等手段对整体式催化剂进行了表征。当球磨时间为60 min，分子筛浆料固含量为38%时，整体式催化剂的涂层上载量可达到178 g?L^-1，涂层脱落率低于0.5%。Pd₂Pt₃-ZSM-5/Cordierite整体式催化剂（贵金属总负载量为1.2 g?L^-1）对于丙烷的催化燃烧具有较好的催化活性（T₅₀=259℃，T₉₀=323℃）和稳定性，具有良好的工业应用前景，其中较低的ZSM-5分子筛硅铝比以及Pd和Pt之间的相互作用增加了对丙烷的吸附能力和表面活性氧物种的数量，从而提高了整体式催化剂的催化活性。     

海泡石-Al２Ｏ３混合载体对铂催化剂环己烷脱氢反应的影响

以三氧化二铝或海泡石(Sepiolite)-三氧化二铝混合物为载体,金属铂为活性组分,采用浸渍法分别制备了Pt／Ａl_２Ｏ_３、Pt／Ｓep-Ａl_２Ｏ_３催化剂,并考察了它们对环己烷脱氢反应的性能、抗硫性能及催化剂活性中心的影响。结果表明,Pt／Ｓep-Ａl_２Ｏ_３催化活性及抗硫性能均高于工业用Pt／Ａl_２Ｏ_３催化剂,同时增大了铂催化剂上的活性中心数及分散度。     

Dehydrogenation of propane over a silica-supported vanadium oxide catalyst

The dehydrogenation of propane over a silica-supported vanadium oxide catalyst was investigated at 823 K under atmospheric pressure in the presence/absence of CO₂. The yield of propene and the selectivity to propene were higher in the dehydrogenation in the presence of CO₂ than those in the dehydrogenation in the absence of CO₂. On the other hand, the yield of aromatics and the selectivity to aromatics were much higher in the dehydrogenation in the absence of CO₂ than those in the dehydrogenation in the presence of CO₂. TPR measurements, NH₃ desorption studies and in-situ UV–vis studies on the catalyst were also performed to elucidate the effects of CO₂ on the behavior of the vanadium oxide in the catalyst during the dehydrogenation of propane.     

丙烷脱氢催化剂研究进展

综述了丙烷脱氢的铬催化剂、铂催化剂及其他催化剂的研究进展,重点从载体、助剂和催化剂制备方法的角度阐述了铂催化剂的研究现状,展望了丙烷脱氢催化剂的研究前景.     

Selective ammoxidation of propane over multicomponent oxide catalysts

The ammoxidation of propane to acrylonitrile was investigated over various multicomponent mixed oxidecatalysts. Bi₃GaMo₂ oxide, Bi_0.85V_0.55Mo_0.45 oxide and Bi₂TiMo oxide showed a good selectivity to acrylonitrile. The catalytic performance was strongly dependent on the components constituting the oxides due to the concentration of defects, the nature of the component and the mixed oxide phases. The effect of support type on the catalytic performance of Bi_0.85V_0.55Mo_0.45 oxide showed that selectivity to acrylonitrile decreased in the order silica > alumina > magnesia. The catalytic performance of Bio_0.85V_0.55Mo_0.45 oxide was improved by the addition of a small amount of a component such as magnesium, calcium and tellurium. The catalytic performance of Bi₃GaMo₂, oxide catalyst, however, decreased significantly with the addition of a smallamount of alkali metal (Li, Na, K, Cs).     

MoOx/SBA-15丙烷选择氧化催化剂的研究

采用浸渍法制备了一系列不同Mo含量的MoOx/SBA-15催化剂,并考察了丙烷选择氧化生成醛类含氧化合物（甲醛、乙醛和丙烯醛）的催化剂性能,利用FT-IR和XRD等技术对催化剂及载体的物化性能进行了表征。结果表明,催化剂的活性主要取决于Mo的负载量,当x(Mo)=1.75%［n(Mo)∶n(Si)=1.75∶100］时,醛类选择性约30%,总醛收率为10.4%,高分散催化剂尤其有利于醛类含氧化合物的定向生成。     

Electrochemical promotion of the oxidation of propane on Pt/YSZ and Rh/YSZ catalyst-electrodes

The effect of electrochemical promotion (EP) or non-faradaic electrochemical modification of catalytic activity (NEMCA) was studied in the catalytic reaction of the total oxidation of propane on Pt and Rh films deposited on Y₂O₃-stabilized-ZrO₂ (or YSZ), an O²⁻ conductor, in the temperature range 420–520 °C. In the case of Pt/YSZ and for oxygen to propane ratios lower than the stoichiometric ratio it was found that the rate of propane oxidation could be reversibly enhanced by application of both positive and negative overpotentials (“inverted volcano” behavior), by up to a factor of 1350 and 1130, respectively. The induced rate increase Δr exceeded the corresponding electrochemically controlled rate I/2F of O²⁻ transfer through the solid electrolyte, resulting in absolute values of the apparent faradaic efficiency Λ=Δr/(I/2F) up to 2330. The Rh/YSZ system exhibited similar EP behavior. Abrupt changes in the oxidation state of the rhodium catalyst, accompanied by changes in the catalytic rate, were observed by changing the O₂ to propane ratio and catalyst potential. The highest rate increases, by up to a factor of 6, were observed for positive overpotentials with corresponding absolute values of faradaic efficiency Λ up to 830. Rate increases by up to a factor of 1.7 were observed for negative overpotentials. The observed EP behavior is explained by taking into account the mechanism of the reaction and the effect of catalyst potential on the binding strength of chemisorbed reactants and intermediates and on the oxidative state of the catalyst surface.     

The influence of sulfur dioxide on propane oxidation activity over supported platinum and palladium

Earlier studies have shown that sulfur dioxide and metal-support interaction can strongly influence propane oxidation over platinum. In particular, oxidation activity is enhanced when platinum is supported on sulfated -alumina or zirconia compared to -alumina. Therefore, it is of interest to compare the performance of palladium under the same experimental conditions. Four model catalysts were examined: Pt/-alumina, Pt/zirconia, Pd/-alumina and Pd/zirconia. The metal loading was kept at or below 0.05 wt% to emphasize changes in activity attributable to metal-support interaction. Reaction rates were measured with and without sulfur dioxide. Surface sulfation was analyzed by measuring acid strength and evaluating spectra obtained by Fourier-transform infrared spectroscopy. In contrast to platinum, sulfation does not promote propane oxidation on Pd/-alumina, and Pd/zirconia is less active than Pd/-alumina.     

丙烷脱氢制丙烯催化剂中国专利技术进展

介绍了近几年丙烷脱氢制丙烯催化剂中国专利技术,分别论述了铂系催化剂、铬系催化剂和其它催化剂专利技术进展,对丙烷脱氢制丙烯催化剂的发展方向进行了推测。     

丙烷氨氧化制丙烯腈催化剂设计进展

丙烷氨氧化制丙烯腈反应工艺是潜在的具有较大经济效益的丙烯腈生产路线。介绍了丙烷氨氧化制丙烯腈催化剂的设计、催化反应机理、典型催化剂组成和结构的研究进展。     

Propane dehydrogenation to propylene over Pt-based catalysts

Propane catalytic dehydrogenation to propylene was investigated over novel platinum-based catalysts, and the BET, H₂-chemisorption, H₂-TPR, H₂-TPD, C₃H₆-TPD and O₂-pulse techniques were used for catalyst characterization in this paper. The results showed that the addition of Zn and Ce promoters into Pt-based catalyst could remarkably improve the performances of dehydrogenation. Highly propylene selectivity, about 99%, was obtained in the dehydrogenation reaction. This improvement in catalytic performances could be attributed to the strong surface interactions, which modified the surface properties of the active platinum metal and the support, and further improved the catalytic performance of Pt-based catalyst.     

High temperature catalytic combustion of methane and propane over hexaaluminate catalysts: NOx emission characteristics

Several hexaaluminate-related materials were prepared via hydrolysis of alkoxide and powder mixing method for high temperature combustion of CH₄ and C₃H₈, in order to investigate the effect of the concentration of the fuels, O₂ and H₂O on NO_x emission and combustion characteristics. Among the hexaaluminate catalysts, Sr_0.8La_0.2MnAl₁₁O₁₉₋ prepared by the alkoxide method exhibited the highest activity for methane combustion and low NO_x emission capability. NO_x emission at 1500 °C was increased linearly with O₂ concentration, whereas water vapor addition decreased NO_x emission in CH₄ combustion over the Sr_0.8La_0.2MnAl₁₁O₁₉₋ catalyst. In the catalytic combustion of C₃H₈ over the Sr_0.8La_0.2MnAl₁₁O₁₉₋ catalyst, the amount of NO_x emitted was raised in the temperature range between 1000 and 1500 °C when the C₃H₈ concentration increased from 1 to 2 vol.%. It was found that NO_x emission in this temperature range was reduced effectively by adding water vapor.     

BiOCl催化剂的丙烷氧化脱氢催化性能

以_L-赖氨酸为模板剂,采用沉淀法制备了BiOCl催化剂,对催化剂进行了X射线衍射、N₂吸附-脱附和H₂-TPR等表征,并测试了BiOCl催化剂对丙烷氧化脱氢制丙烯反应的催化性能。结果表明,制备的BiOCl催化剂为四面体结构,500 ℃焙烧3 h后,催化剂比表面积为11.2 m²·g^-1,未完全还原氧物种的含量较多。随着反应温度升高,丙烷转化率和丙烯选择性增加,丙烷转化率为20%时,丙烯选择性达64.5%。     

丙烷催化脱氢反应宏观动力学模型

在温度580～640 ℃、压力0.1 MPa、原料气空速1000～6000 h－1条件下,采用Pt-Sn催化剂,在固定床积分反应器中进行了丙烷催化脱氢实验,建立了脱氢反应宏观动力学模型。根据实验数据,采用多元线性回归分析得到宏观动力学模型的参数,丙烷脱氢反应的活化能约为78.4 kJ/mol。经统计检验,结果表明所建立的丙烷催化脱氢宏观动力学方程是可靠的。     

新型丙烷脱氢催化剂制备及其活性评价

以MIL-101(Cr)为载体,异丙醇铝为铝前驱体,通过添加助剂钾制备新型Cr_2O_3/Al_2O_3脱氢催化剂。考察反应温度、气时空速及钾含量等因素对脱氢过程的影响。结果表明,该催化剂对丙烷脱氢过程表现出较好的催化活性。在反应温度615℃、进料量60 mL·min~(-1)、钾质量分数3.2%的条件下,丙烷转化率39.6%,丙烯选择性90.0%。     

SAPO-34 supported Pt–Sn-based novel catalyst for propane dehydrogenation to propylene

The Pt–Sn-based catalyst was intensified using SAPO-34 as support for direct propane dehydrogenation to propylene. The catalyst was prepared by sequential impregnation method and characterized by XRF, BET, XRD, NH₃-IR, NH₃-TPD, H₂-TPR, HR-TEM and O₂-pulse coke analysis. NH₃-TPD, IR spectra and XRD results suggested that the doping of metals on SAPO-34 did not affect its acidic strength and structural topology of support, respectively. Propylene selectivity of 94% and total olefins selectivity greater than 97% was achieved using Pt–Sn/SAPO-34. The results were compared with Pt–Sn/ZSM-5 under identical conditions. The possible reasons for improvement were the larger surface area, shape selectivity and particular by suitable acidity of SAPO-34.