Reactive Mapping of Transition Metal Catalyst Decoration by Modifiers

用乙烷氢解反应的稳态同位素瞬时动力学分析(SSITKA)研究了改性剂(钾和铜)在负载型Ru催化剂中的分散情况。由于该反应对结构高度敏感，因此可以用来检测改性剂在活性金属表面引起的破坏。事实上，从同位素瞬变过程中，可以直接确定修饰物种如何影响活跃系综位的数量。除了解释SSITKA得出的这些部位的反应性分布外，该项目还解决了有关修饰剂位置和修饰剂分散的基本问题。催化剂助剂常用于提高工业催化剂的活性和选择性。尽管它们被广泛使用，但其影响的性质尚不清楚，导致缺乏选择修饰剂的合理依据。

This is an investigation of the dispersion of modifiers (potassium and copper) in supported ruthenium catalysts using steady-state isotopic transient kinetic analysis (SSITKA) of the ethane hydrogenolysis reaction. Since this reaction is highly structure sensitive, it can be used to detect modifier- induced disruptions in the surface of the active metal. In fact, from isotopic transients, it is possible to determine directly how the modifier adspecies affects the population of active ensemble sites. Along with the interpretation of SSITKA-derived reactivity distributions of these sites, the project addresses fundamental questions regarding modifier location and modifier dispersion. Catalyst promoters are often used to improve activities and selectivities of industrial catalysts. Despite their wide use, the nature of their influence is unknown, resulting in a lack of a rational basis for selection of modifiers.