Dry reforming - from understanding the elementary steps to better catalysts

催化干法甲烷重整制取富CO合成气是一条重要的高吸热路线。因为在所有条件下，碳的生成在热力学上都是有利的，所以只能通过动力学控制来稳定反应。我们建议匈牙利科学院同位素研究所(IoI)、维也纳工业大学(TUW)和明兴工业大学(TUM)的实验室进行合作研究，以阐明和理解在各种反应条件下甲烷与二氧化碳在负载型铂和镍催化剂(Au改性)上的基本反应，并利用这些知识来探索新一代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知识，这些颗粒固定在载体上并与其相互作用的方式，以及在这种复杂和多重耦合反应中的基本步骤的速率。超高真空模型研究(TUW)通过表面科学方法研究氧化物载体和金属纳米颗粒的特殊性质，重点研究与反应物和产物的相互作用和反应的性质。利用溶胶凝胶法(IoI)将合成出新型的坚固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。分散催化剂的动力学和光谱表征(TUM)将为分散催化剂的制备和反应的主要阶段提供必要的定量信息。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所经历的变化。稳态和暂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.