双孔载体改性铜铁基低碳醇合成催化剂及其构效关系研究

项目名称： 双孔载体改性铜铁基低碳醇合成催化剂及其构效关系研究

项目编号： No.51206172

项目类型： 青年科学基金项目

立项/批准年度： 2013

项目学科： 工程热物理与能源利用学科

项目作者： 定明月

作者单位： 中国科学院广州能源研究所

项目金额： 25万元

中文摘要： 本项目针对Cu-Fe基催化剂双活性金属协同作用难于调控，低碳醇合成反应活性和高级醇产物选择性偏低的共性关键问题，提出利用具有不同纳米孔径结构的双孔载体来改性低碳醇合成反应活性位和高级醇产物分布的构思。通过大孔凝胶和小孔溶胶制备具有纳米孔径结构的双孔载体，探索双孔结构形成和孔径尺寸变化规律，研究双孔载体孔道限域效应对Cu、Fe双活性金属的颗粒尺寸调节机制，分析H2和CO等探针分子在不同孔道中的扩散和空间位阻效应，揭示甲醇活性中心Cu组元和碳链增长活性中心Fe组元与双孔载体的相互作用关系，阐明碱性金属对Cu-Fe协同作用的改性和高级醇产物的调节机理，构建Cu-Fe双活性组元微观结构与低碳醇合成反应性能的构效关系，为高活性高选择性具有优良稳定性的低碳混合醇催化剂的工业开发和应用提供基础理论支撑。

中文关键词： 低碳混合醇；双孔载体；铜铁基催化剂；构效关系；

英文摘要： Higher alcohols synthesis (HAS), as an important technology in the production of liquid fuels and chemicals from syngas derived from coal and biomass, is receiving a renewed interest for both industrial and academic applications because of the emergency of transportation fuel shortage in the whole world. In order to solve the key issues of the difficulty to adjust the synergy effect of Cu-Fe, low HAS activity and C2+OH selectivity over the Cu-Fe based catalyst, a support with a distinct bimodal pore structure is used to modify the catalyst, because the large pores provide pathways for rapid molecular transportation and small pores provide a large area of active surface, contributing to high diffusion efficiency and enhance dispersion of supported metal simultaneously. Adjustment mechanism of bimodal support nano-pore structure size, formation and variation of particle size of copper and iron species in the pore structures, diffusion and steric effect of H2 and CO probe molecules in the bimodal support, and regulatory mechanism of higher alcohols via modification of alkaline metals are investigated together for illustrating the synergy effect of Cu-Fe-bimodal support and establishing the relationship between the structure and HAS performance of the Cu-Fe bimodal catalyst. All of these studies provide the theoreti

英文关键词： Higher alcohols synthesis；bimodal support；Cu-Fe based catalyst；structure and performance；