新型抗积碳稀土烧绿石负载Ni重整制氢催化剂研究

Steam reforming of methane and low hydrocarbons is currently the industrialized technique for large scale hydrogen production. Together with dry reforming for hydrogen production, they are hot research topics currently. Ni-based catalysts are the most applicable catalysts for these processes due to their low cost. Although the presently used Ni-based catalysts possess very high activity, they still suffer from deactivation by easy coking and high energy consumption. Compared with catalysts from other countries, there is still some way to go. Therefore, it is necessary to further improve the performance of the catalysts. To solve this problem, in this project, the effective method to prepare various rare earth pyrochlore supports will be investigated. With the combination of plasma treatment technique, it is expected to prepare Ni-based catalysts with superior performance. By using different techniques, the bulk structure, thermal stability, active sites, valence states of the surface Ni species and coke resistance of the catalysts prepared with different rare earth pyrochlores will be studied systematically. The effects on the Ni active sites, Ni grain sizes, Ni dispersion percentage, high temperature stability and coke resistant ability by using plasma treatment and pyrochlore supports with different rare earth elements will also be elucidated. With the expectation to design catalysts having the potential for industrial application, the reaction, coking and deactivation mechanisms and the reaction model, which match the active sites and adsorbed intermediates, are to be clarified.

甲烷和低碳烃水蒸汽重整是工业制氢的有效方法，且和干气重整制氢一起是目前的研究热点。镍基催化剂由于价格低廉成为最理想的催化剂。Ni基催化剂虽然具有很高的催化活性，但存在反应过程中易积碳失活、能耗高等缺陷，与国际水平还有一定差距，有待进一步提高。针对上述问题，本课题拟探讨合成不同稀土烧绿石型复合氧化物载体的有效方法，并结合等离子体处理法制备高性能Ni基催化剂。同时系统深入表征不同稀土烧绿石负载的Ni基催化剂其体相结构、热稳定性、活性位、表面Ni 物种的价态分布和抗积碳性能等，致力探明等离子体处理和含各种不同稀土的烧绿石作为载体对 Ni 活性位的存在形式、颗粒尺寸、分散度、高温热稳定性和抗积碳性能的影响；探讨反应机理和失活机理，提出确切可信、与催化剂反应中心和吸附中间体相吻合的表面反应模型机、反应和积碳机理，以期设计出具有潜在应用价值的抗积碳稀土烧绿石负载Ni重整催化剂。

甲烷重整制氢是目前获得氢气的主要方式。镍基催化剂由于价格低廉成为最理想的催化剂。Ni基催化剂虽然具有很高的催化活性，但存在反应过程中易积碳失活、能耗高等缺陷，与国际水平还有一定差距，有待进一步提高。针对上述问题，本课题探讨合成不同稀土烧绿石型复合氧化物载体的有效方法及不同结构Ni基催化剂，并结合等离子体处理法制备高性能Ni基催化剂。系统深入研究了Ni基催化剂其体相结构、热稳定性、活性位、表面Ni 物种的价态分布和抗积碳性能等，探明了等离子体处理和含各种不同稀土的烧绿石作为载体及不同结构Ni基催化剂中Ni 活性位的存在形式、颗粒尺寸、分散度、高温热稳定性和抗积碳性能的影响；探讨了反应机理和失活机理，提出确切可信、与催化剂反应中心和吸附中间体相吻合的表面反应模型机制和积碳机理，制备得到多个具有潜在应用价值的抗积碳Ni基重整催化剂。在项目资金的支持下，已发表高水平研究论文15余篇，培养研究生6名，超额完成项目任务研究要求。