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2005年06月17日

【期刊论文】反应条件对Mo2C/Al2O3催化的POM制合成气的影响

季生福, 朱全力, 杨建, 季生福*, 王嘉欣, 汪汉卿

分子催化,2003,17(5):363~366,-0001,():

-1年11月30日

摘要

考察了反应温度、气体空速和进料中CH4∶O2比值对Mo2C/Al2O3催化的POM反应制合成气的影响。结果发现较高的温度具有较高的甲烷转化率、CO和H2的选择性;而在较低的温度下,对CO的选择性比对H2的影响更大。反应气体的空速较小时对于甲烷的转化率、CO和H2的选择性是有利的;而在较高的气体空速下,氢气的选择性则更低。进料中CH4∶O2 比值稍高于2∶1时有利于获得高的甲烷转化率、CO和H2的选择性,并且还可以增加催化剂的稳定性。当CH4∶O 2比值低于2∶1时,甲烷转化率、CO和H2选择性随反应的进行急剧下降,而当此比值调整到高于2∶1时,转化率和选择性都可以得到恢复。

Mo2C/, Al2O3催化剂, 甲烷部分氧化, 合成气, 反应条件的影响

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2005年06月17日

【期刊论文】The relationship between the structure and the performance of Na-W-Mn/SiO2 catalysts for the oxidative coupling of methane

季生福, Sheng-fu Ji a, b, Tian-cun Xiao b, Shu-ben Li a, Chuan-zhi Xu a, Rui-ling Hou a, Karl S. Coleman b, Malcolm L.H. Green b, *

Applied Catalysis A: General 225 (2002) 271-284,-0001,():

-1年11月30日

摘要

A series of Na-W-Mn/SiO2 catalysts with different sodium, tungsten, and manganese contents (wt.%) were prepared and their catalytic performance for the oxidative coupling of methane (OCM) was evaluated in a continuous micro-reactor. The structural properties of the catalysts have been characterised using XPS, laser Raman spectroscopy (LRS), and X-ray diffraction (XRD). The results show that the catalysts containing Na, W, and Mn between the range of 0.4-2.3, 2.2-8.9, and 0.5-3.0 wt.%, respectively, had high CH4 conversion and high selectivity to C2 hydrocarbons in the OCM reaction. The addition of sodium to the catalyst is believed to bring about the migration of manganese to the catalyst surface, as both elements are found in high concentrations in this area. CH4 conversion and the selectivity to C2H4 are closely related to the surface Mn concentration of the catalysts. Both Na-O-Mn and Na-O-W act as the active centres of the catalysts for the oxidative coupling of methane. The catalyst surface is mainly covered with Na and O, while the Mn and W are present in the sub-surface of the catalyst. There is a synergic effect of sodium, tungsten, and manganese components, and the Na2W2O7 crystalline phase is active for the oxidative coupling of methane.

Oxidative coupling of methane, Na-W-Mn/, SiO2 catalyst, Structure

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2005年02月24日

【期刊论文】Catalytic combustion of methane over cobalt-magnesium oxide solid solution catalysts

季生福, Sheng-Fu Ji a, b, Tian-Cun Xiao b, Hai-TaoWang b, Emmanuel Flahaut b, Karl S. Coleman b and Malcolm L.H. Green b, ∗

Catalysis Letters Vol. 75, No. 1-2, 2001,-0001,():

-1年11月30日

摘要

in a continuousflow microreactor. The Co content has a significant effect on the activity of the cobalt-magnesium oxide solid solution catalysts. The catalysts containing 5 and 10% Co have the lowest light-off temperature in methane combustion. In the preparation of cobalt-magnesium oxide solid solution catalysts, higher urea to metal ratio favors the formation of the catalysts with smaller crystal particles and leads to a better catalytic performance for methane combustion. Addition of lanthanum nitrate to the solution of Co and Mg nitrate depressed the formation of the cobaltmagnesium oxide solid solution and decreased the activity of the catalysts for methane combustion. The cobalt-magnesium oxide solid solution catalysts are very stable when the calcination or reaction temperature is no more than 900◦C. However, the catalytic activity decreases rapidly after high temperature (>1000℃) calcination, possibly due to sintering of the catalyst and thus decrease of the surface area.

cobalt-magnesium oxide solid solution catalyst, methane combustion, laser Raman, XRD

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2005年02月24日

【期刊论文】Na-W-Mn/SiO2催化剂晶格氧的扩散行为

季生福, 李树本, 许传芝, 薛锦珍

分子催化,2002,16(5):369~373,-0001,():

-1年11月30日

摘要

制备了不同组分Na、W、Mn/SiO2催化剂,在ITD(Ion Trap Detector)装置上进行了催化剂表面CO恒温脉冲反应(CO-CTPR)。 研究结果表明,单组分Na、W、Mn/SiO2催化剂体相晶格氧向表面扩散的速度顺序为Mn/SiO2/Na/S iO2/W/SiO2;与CO反应的表面晶格氧数量的顺序为M n/SiO2/Na/SiO2≈W/SiO2。多组分Na、W、Mn/SiO2催化剂体相晶格氧向表面扩散的速度顺序为Na-W/SiO2/Na-Mn/SiO2/W-Mn/SiO2/Na-W-Mn/SiO2,且Na与W、Mn的结合对体相晶格氧向表面的扩散有促进作用;与CO反应的表面晶格氧数量的顺序为Na-W-Mn/SiO2/Na-Mn/SiO2/W-Mn/SiO2/Na-W/S iO2。

担载型催化剂, 晶格氧, 扩散, 一氧化碳, 脉冲反应

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2005年06月17日

【期刊论文】The promotion of nickel to Mo2C/Al2O3 catalyst for the partial oxidation of methane to syngas

季生福, Zhu Quanli, Zhang Bing, Yang Jian, Wang Jiaxin, Zhao Jun, Ji Shengfu* and Wang Hanqing*

New J. Chem., 2003, 27, 1633-1638,-0001,():

-1年11月30日

摘要

Alumina-supported molybdenum carbide and its modifier with small amounts of nickel were evaluated and characterized. The evaluation results showed that a nickel-doped carbide catalyst exhibited a much higher conversion of methane and selectivity to CO and H2for the partial oxidation of methane (POM) to syngas. Also, the addition of a small amount of nickel resulted in significant improvement of catalysis stability. Characterization by temperature programmed surface reaction (TPSR) indicated that the addition of nickel promoted the carburization of molybdenum oxide. Especially under the conditions of the POM to syngas, this promotion resulted in more active phases being held. The nickel doped catalyst had small particles, larger specific area and greater ability to resist sintering. All these improved the catalytic stability. The other characterizations by XRD, XPS, SEM as well as BET surface area measurement also confirmed these promotions of nickel. In addition, the doped nickel made possible the increase of the intrinsic activity of catalytic centers over molybdenum carbide catalyst.

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    北京化工大学,北京

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