Fuel ( IF 6.7 ) Pub Date : 2022-05-21 , DOI: 10.1016/j.fuel.2022.124536 Li Zhang , Peipei Ai , Zhihua Gao , Wei Huang
Using mesoporous silica with different structures and morphologies as support, a series of copper-based catalysts was prepared for dimethyl oxalate (DMO) hydrogenation to ethylene glycol (EG). The results showed that the structure and morphology of supports had a significant effect on the catalytic stability of Cu-based catalysts. The Cu-based catalyst prepared by using MS-3 with hexagonal prism-like structure as support, exhibited excellent catalytic activity and enhanced stability (DMO conversion of ∼100%, EG selectivity up to 98%, and stability over 400 h). The enhanced catalytic performance of Cu/MS-3 catalyst could be attributed to the strong interaction between copper species and MS-3 support. MS-3 with narrowed pore size and larger specific surface area was not only beneficial to the dispersion and limitation of Cu nanoparticles, but also conducive to the formation of copper phyllosilicate structures from the copper ammonia complex and the silicon support, which provides a large number of stable active copper species. These attributes collectively promote the catalytic stability of Cu-based catalyst for DMO hydrogenation.
中文翻译:
增强铜基催化剂草酸二甲酯加氢的催化稳定性
以不同结构和形貌的介孔二氧化硅为载体,制备了一系列铜基催化剂,用于草酸二甲酯(DMO)加氢制乙二醇(EG)。结果表明,载体的结构和形貌对Cu基催化剂的催化稳定性有显着影响。以六方棱柱状结构的 MS-3 为载体制备的 Cu 基催化剂表现出优异的催化活性和增强的稳定性(DMO 转化率约为 100%,EG 选择性高达 98%,稳定性超过 400 小时)。Cu/MS-3催化剂的增强催化性能可归因于铜物种和MS-3载体之间的强相互作用。MS-3孔径变窄,比表面积较大,不仅有利于Cu纳米粒子的分散和限制,也有利于铜氨络合物与硅载体形成层状硅酸铜结构,提供大量稳定的活性铜物种。这些属性共同提高了用于 DMO 加氢的铜基催化剂的催化稳定性。