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中文摘要 CO加氢合成低碳混合醇的多相催化反应是催化剂表面碳碳链增长和CO插入功能的协同作用过程，催化剂活性组分的紧密接触，颗粒大小及织构组成在很大程度上决定反应中间体的调控与转归，从而影响低碳混合醇的活性、选择性和稳定性。将催化剂活性组分纳米化并通过多孔载体的包覆限域作用，是在纳米尺度上实现活性组分的高度分散，抑制催化剂烧结及相分离，提高催化剂的稳定性及调控混合醇选择性的有效途径之一。 本课题着眼于提升CO加氢合成低碳混合醇催化剂的选择性和稳定性，创新性地设计多孔氧化锆包覆CuFe纳米催化剂，通过对多相催化剂活性组分纳米化及包覆结构制备参数的优化，制备一系列不同结构和组成的包覆型CuFe催化剂，探寻CO加氢性能与催化剂结构的构效关系，进一步明确包覆结构催化剂表面CO加氢反应机理。本研究将为实现多相催化剂的性能调控开辟一条新思路，并在CO加氢选控合成反应的网络构建和拓展规模化应用方面奠定重要的科学基础。 Abstract The mixed alcohols synthesis via CO hydrogenation is a kind of heterogeneous catalytic process between the synergetic functions of associative/dissociative adsorption of CO and carbon chain growth over the catalyst.The close contact, particle size and textural structure of the active species largely determine the adjustment and transformation of the reaction intermediates, and then affect the activity, selecticity and stablity of the catalyst.One of the efficient ways to enhance the catalyst stability and control the selectivity of mixed alcohols is to design the confined structure of the porous support coated nanosized active species. This project innovatively designs the porous zirconia coated CuFe nano-catalyst for the purpose of enhancing the alcohols selectivity and reaction stability for CO hydrogenation. We will prepare a series of coated CuFe catalysts with different structure and composition through the preparation parameter optimization of the nanosized active species and coated structure, exploring the structure-performance relationship between the catalyst structure and CO hydrogenation,and then further to elucidate the reaction mechanism over the catalysts. This study will provide a new idea to adjust the catalytic properties of the heterogenous catalyst, and lay an important scientific foundation and act as theoretical guidence for constructing the reaction network and extending the scalable application of the selective synthesis in CO hydrogenation. |
2楼2023-08-17 16:40:25