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中文摘要：
首先制备了一系列的单元（CeO2,TiO2,ZrO2）、双元（Ce-Ti,Ti-Zr）和三元（Ce-Ti-Zr）载体,然后通过浸渍法在载体表面负载Co,考察了载体组成和焙烧温度对该催化剂的甲烷部分氧化（POM）催化性能的影响.利用N2物理吸附、X射线粉末衍射、H2-程序升温还原、扫描电子显微镜和热重分析等手段对反应前后催化剂的物理化学性质进行了表征.实验结果表明,载Co催化剂的催化性能按三元＞双元＞单元的顺序依次降低.700℃焙烧制备的Co/Ce-Ti-Zr-700三元载体催化剂表现出最高的CH4转化率和H2、CO的选择性,同时该催化剂具有较高的稳定性.在Ce-Ti-Zr三元载体催化剂中,CeO2-TiO2-ZrO2之间产生了较强的相互作用,从而抑制了非活性相CoTiO3的生成,产生了更多的活性中心;同时这种载体之间的作用可以防止催化剂在反应过程中发生相变生成CoZr2和ZrC之类的物质.
英文摘要：
A series of single （CeO2, TiO2, ZrO2）, binary （Ce-Ti, Ti-Zr） and ternary （Ce-Ti-Zr） composite supports were synthetized to prepare cobalt containing catalysts for the partial oxidation of methane. The catalysts were then obtained by impregnation method using the as-synthesized supports. The effects of support composition and calcination temperature on the catalytic performance of the catalysts in partial oxidation of methane （POM） were investigated. The fresh and used catalysts were characterized by physicochemical characterization methods such as N2 physical adsorption, X-ray diffraction （XRD）, H2-temperature programmed reduction （TPR）, scanning electron microscopy （SEM） and therrnogravimetry （TG）. Experimental results show that the performance of the cobalt-based catalysts decreases according to the following orders： ternary 〉 binary 〉 single. Co/Ce-Ti-Zr-700 catalyst calcined at 700℃ exhibites the highest CH4 conversion and selectivity to CO and H2, as well as the best stability. The strong interactions between CeO2, TiO2, and ZrO2 in the ternary support effectively restrain the formation of non-active phase of CoTiO3 and promote the formation of active sites. Furthermore, during the POM reaction, the interactions can inhibit the phase transformation of catalyst to generate the non-active phase of CoZr2 or ZrC.
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