有序介孔限域的镍/钴基金属氧化物材料的构建及其催化甲烷二氧化碳重整反应性能研究

项目名称： 有序介孔限域的镍/钴基金属氧化物材料的构建及其催化甲烷二氧化碳重整反应性能研究

项目编号： No.21503113

项目类型： 青年科学基金项目

立项/批准年度： 2016

项目学科： 数理科学和化学

项目作者： 徐磊磊

作者单位： 南京信息工程大学

项目金额： 21万元

中文摘要： 本项目针对甲烷二氧化碳重整反应镍/钴非贵金属基催化剂易于发生金属活性组分热烧结和表面积碳而导致快速失活的缺点，拟采用软模板“一锅法”挥发诱导自组装策略构建一类具有孔结构优良、结晶性好、热稳定性高等优点的镍/钴基有序介孔金属氧化物材料用于催化甲烷二氧化碳重整反应，研究材料制备过程中各种因素对材料理化性质和催化性能的影响，确定制备化学规律与构效关系。该研究拟将镍、钴活性中心原位引入到有序介孔骨架之中，介孔骨架的“限域效应”可以有效抑制金属活性位的热烧结；通过对合成条件的调控，制备具有大比表面、大孔容、均一孔径等优点的材料，可以为气态反应物提供充足的活性位。因此，这一类有序介孔催化剂将会表现出优于传统负载型催化剂的催化活性和稳定性。此外，本项目拟发展一些原位动态表征技术，尝试从分子水平研究甲烷二氧化碳重整反应条件下稳定小分子CH4、CO2在介孔催化剂表面活化与定向转化机制及积碳行为。

中文关键词： 有序介孔；金属氧化物；限域效应；甲烷；二氧化碳重整

英文摘要： The traditional Ni, Co based non-noble metal catalysts for carbon dioxide reforming of methane reaction are commonly inclined to suffer rapid deactivation due to the thermal sintering of the metallic active sites and severe carbon deposition over the catalyst surface. In view of the disadvantages of traditional catalysts, the present project plans to construct a series of Ni, Co based ordered mesoporous metal oxides with excellent structural properties, such as excellent porosity structure, good crystallinity, superior thermal stability, via soft template assisted “one-pot” evaporation induced self-assembly (EISA) strategy, which will be directly utilized as the catalysts for carbon dioxide reforming of methane reaction. The influence of various factors during the preparation process on the physicochemical properties and catalytic properties of the materials will be investigated and the rule of the preparation chemistry and structure-efficacy relationship will be determined. This project will take the advantage of the “one-pot” strategy and in situ introduce the Ni, Co active sites into the ordered mesoporous framework, whose “confinement effect” will effectively suppress the thermal sintering of the metallic active sites under carbon dioxide reforming of methane reaction conditions. Besides, the obtained mesoporous materials are usually provided with large surface areas, big volumes, and uniform pore sizes by regulating preparation parameters, which will provide the gaseous reactants with sufficient “accessible” active centers. Therefore, these series mesoporous catalysts will promise outstanding catalytic activities and stabilities. Furthermore, some in situ dynamic characterization techniques will be also developed and used to investigate the activation mechanisms of CH4, CO2 stable molecules as well as carbon deposition behavior over these mesoporous catalysts surface from the molecular level.

英文关键词： Ordered mesopore;Metal oxides;Confinement effect;Methane;Carbon dioxide reforming