Dry reforming - from understanding the elementary steps to better catalysts

甲烷催化干重整是一种重要的、高吸热的富CO合成气制备方法。因为在所有条件下碳的形成都是有利的，所以只能通过动力学控制来稳定反应。我们提议在匈牙利科学院同位素研究所（IoI）的实验室进行一项合作研究，维也纳工业大学（TUW）和慕尼黑工业大学（TUM）阐明和理解甲烷与CO2在负载型Pt和Ni催化剂上重整的基元反应（用Au改性）在各种反应条件下的反应，并利用这一知识寻求新一代的高活性和稳定的催化剂。设计催化剂所需的洞察力将包括对金属颗粒的性质和几何性质的了解，这些颗粒固定在载体上并与载体相互作用的方式，以及这种复杂和多重耦合反应中基本步骤的速率。UHV模型研究（TUW）通过表面科学方法解决氧化物载体和金属纳米颗粒的特定性质，重点是与反应物和产物的相互作用和反应的性质。将使用溶胶-凝胶方法（IoI）合成新型耐用且稳定的纳米结构催化剂，并有望促进从贵金属到贱金属的成功过渡。分散型催化剂的动力学和光谱表征（TUM）将在制备和反应的主要阶段提供关于分散型催化剂的必要的定量信息。原位光谱表征不仅有助于开发可扩展的合成，而且还有助于了解催化剂在反应过程中发生的变化。在稳态和瞬态条件下的动力学评价将提供一个严格的动力学模型来解释催化剂的行为，并为催化剂的合成提供反馈。

Catalytic dry methane reforming is an important, highly endothermic route to CO rich synthesis gas. Because carbon formation is thermodynamically favored under all conditions, the reaction can only be stabilized by kinetic control. We propose a collaborative study of laboratories at the Institute of Isotopes of the Hungarian Academy of Sciences (IoI), the Technische Universität Wien (TUW) and the Technische Universität München (TUM) to elucidate and understand the elementary reactions of methane reforming with CO2 on supported Pt and Ni catalysts (modified with Au) under a wide variety of reaction conditions and to use this knowledge in the quest for a new generation of highly active and stable catalysts. The insight required for designing catalysts will include the knowledge of the nature and geometrical properties of the metal particles, the way these are anchored to and interact with the support, as well as the rates of elementary steps in this complex and multiply coupled reaction. UHV model studies (TUW) address the specific properties of oxide supports and metal nanoparticles via surface science methods, focusing on the nature of interaction and reaction with reactants and products. Novel robust and stable nanostructured catalysts will be synthesized using a sol-gel approach (IoI) and are expected to facilitate a successful transition from noble to base metals. The kinetic and spectroscopic characterization (TUM) of dispersed catalysts will provide the necessary quantitative information on the dispersed catalysts at the main stages of preparation and reaction. In situ spectroscopic characterization will help not only to develop a scalable synthesis, but will also serve to understand the changes the catalyst undergoes during the reaction. The kinetic evaluation under stationary and transient conditions will provide a rigorous kinetic model to explain catalytic behavior and give feedback to catalyst synthesis.