改性Mo/HZSM-5催化剂甲烷无氧芳构化反应条件研究

采用Mo担载的质量分数为6%、经过先碱后酸预处理的Mo/HZSM-5作为催化剂,在不同反应温度和反应空速下,比较了甲烷的转化率、苯的生成速率和积炭的收率.结果表明,当反应温度为700℃,反应空速为1 400 mL/(g·h)时,甲烷无氧芳构化性能最佳.     

Reforming of methane with carbon dioxide over supported bimetallic catalysts containing Ni and noble metal: I. Characterization and activity of SiO2 supported Ni–Rh catalysts

Cobalt catalysts supported on silica aerogel have been prepared using sol–gel chemistry followed by drying under supercritical ethanol conditions. Three different loadings of cobalt were synthesized: 2, 6, and 10% by weight. Transmission electron micrographs indicate that the metallic cobalt exists as discrete particles 50–70 nm in diameter for the 2 and 6% loadings. The 10% catalyst shows long needles of cobalt. BET and BJH measurements indicate that the catalysts retain the silica aerogel properties of high surface area (∼800 m²/g), large pore volume (∼5 cm³/g), and an average pore diameter in the mesoporous regime (∼25 nm). The catalysts were evaluated for Fischer–Tropsch activity in a laboratory-scale packed bed reactor. All three catalysts were active with the 10% Co catalyst achieving more than 20% CO conversion which corresponds to a rate of 1.53 g CO per g-cat per hour. The catalysts were selective for the C₁₀₊ hydrocarbons with more than 50% of the carbon contained within this fraction. A significant portion of the C₉–C₁₅ hydrocarbon product was observed as 1-olefins which reflects the enhanced mass transport within the very porous aerogel support.     

Partial oxidation of methane to synthesis gas over α-Al2O3-supported bimetallic Pt–Co catalysts

The partial oxidation of methane to synthesis gas was studied at atmospheric pressure and in the temperature range of 550–800°C over -Al₂O₃-supported bimetallic Pt–Co, and monometallic Pt and Co catalysts, respectively. Both methane conversion and CO selectivity over a bimetallic Pt_0.5Co₁ catalyst were higher than those over monometallic Pt_0.5 and Co₁ catalysts. Furthermore, the addition of platinum in Pt–Co bimetallic catalysts effectively improved their resistance to carbon deposition with no coking occurring on Pt_0.5Co₁ during 80 h reaction. The FTIR study of CO adsorption observed only linearly bonded CO on bimetallic Pt–Co catalysts. TPR and XPS showed enhanced formation of a cobalt surface phase (CSP) in bimetallic Pt–Co catalysts. The origins of the good coking resistivity of bimetallic Pt–Co catalysts were discussed.     

基于CaO引导的甲烷蒸汽重整化学链燃烧制氢系统

为在重整气中得到高纯H_2和降低尾气CO_2分离成本,建立了基于CaO引导的甲烷蒸汽重整化学链燃烧制氢系统,该系统在重整反应器中加入CaO吸收剂,用以吸收重整器内的CO_2,提高重整气中H_2浓度,形成的CaCO_3固体在煅烧器中受热分解重新生成CaO。利用Aspen Plus进行了过程模拟及热力学分析,并研究主要参数对系统性能的影响,得到优化的操作条件为:CaO循环量/CH_4比为0.5,CH_4(燃料)/CH_4比为0.35,NiO循环量/CH_4比为1.4。CaO循环量/CH_4比从0变化到0.5时,重整气中H_2浓度从0.60增长到0.99;CH_4(燃料)/CH_4比在0.25~0.45区间变化时,重整气中H_2浓度从0.86提高到0.99,产气量增加;NiO循环量/CH_4比在1~1.6区间变化时,重整气中H_2浓度从0.88增长到0.99,系统有效能效率变化较小。     

甲烷高温燃烧催化剂研究进展

催化燃烧具有环保、高效、节能等诸多优点.综述了甲烷高温催化燃烧的研究现状,对甲烷燃烧催化剂材料的研究进展做了较详细的介绍,并阐述了甲烷高温催化燃烧反应器的研究进展.     

CPE包覆纳米CaCO3对PVC／纳米CaCO3复合材料结构与性能的影响

研究了基体韧性、纳米CaCO3直接填充与用CPE包覆后填充PVC对复合材料力学性能的影响，并对其微观结构进行了探讨。结果表明，适当的基体韧性有助于获得较高的冲击强度；两种填充方法下，PVC复合材料的冲击强度和拉伸强度呈现出不同的变化趋势。包覆处理填充体系的冲击强度均要比未包覆处理填充体系的略低，而拉伸强度则相反，特别是在包覆小份量CaCO3(2份)时，所得复合材料的冲击强度甚至比PVC／CPE(8份)基体的低12％，而拉伸强度则出现最大值，比基体的高8．9％左右。     

甲烷部分氧化制合成气催化剂的研究进展

综述了甲烷部分氧化制合成气的研究意义和现状，从金属活性组分，载体效应，载量选择，助剂添加和制备方法等因素对催化剂活性的影响及研究进行了系统。结合本课题组的研究结果及文献报道，分析了Ni基催化剂的失活特性，并提出使用等离子体技术对Ni基催化剂进行改笥处理，以提高其催化稳定性的技术展望。     

Oxidative coupling of methane over LaCoO3−δ-based mixed oxides

The catalytic activity of LaCoO_3–-based mixed oxides for the oxidative coupling of methane has been tested by TPR and cyclic reaction. Characterization has been done by XRD, TGA and Mössbauer spectrometry. It is likely that the perovskite-crystal structure containing hypervalent metal ions has an important role and that unique structural oxygen species in the perovskite contribute to the partial oxidation of methane.     

Kinetics of methane hydrate formation in aqueous electrolyte solutions

Experimental data on the kinetics of methane hydrate formation in aqueous electrolyte solutions are reported. The experiments were carried out in a semi-batch stirred tank reactor in three NaCl and two KCl solutions as well as in a solution containing a mixture of NaCl and KCl at three different nominal temperatures from 270 to 274 K and at pressures ranging from 3.78 to 7.08 MPa. The kinetic model developed by Englezos et al. (1987a) was adapted to predict the growth of hydrates. The model is based on the crystallisation theory coupled with the two-film theory for gas absorption in the liquid phase. The kinetic rate constant which appears in the model was that obtained earlier for methane hydrate formation in pure water. The effect of the electrolytes was taken into account through the computation of the three-phase equilibrium conditions and the corresponding fugacities. Overall, the model predictions match the experimental data very well with the largest prediction error being less than 10%.