Fundamental Studies on Catalyst Deactivation and Corrosion Phenomena under Biomass Feed and the Interaction with Polar Biomass-Derived Molecules

生物质和生物质衍生原材料的转化和价格稳定对未来能源和基本化学品的可持续供应至关重要，特别是在原油、天然气和煤炭资源不断减少的情况下。与石化反应相反，由于这些分子的极性，生物质的催化转化通常在液相中进行。将研究极性分子与液相中的非均相催化剂表面的相互作用，以便更深入地了解导致催化剂腐蚀和失活的分子过程。重要的失活途径是活性相和载体的浸出、颗粒烧结、强吸附反应中间体和产物的中毒以及焦炭和低聚物的形成。这些过程将在明确定义的模型催化剂上进行研究，即具有负载催化剂颗粒的平坦基底，其允许通过显微镜，光学和电子光谱方法进行高级表征，优选在原位或操作条件下。作为反应体系，甘油、葡萄糖、琥珀酸和马来酸以及纤维素的转化将用作典型的模型体系，其含有原型官能团（即，分子水平的理解稍后将转移到在高压/高温反应器中应用负载型催化剂颗粒的工业相关反应条件，并对工作催化剂进行操作光谱分析。基于所获得的知识，将开发用于稳定所应用的催化剂的新概念。

The conversion and valorization of biomass and biomass-derived raw materials is of major importance for the future sustainable supply of energy and basic chemicals, especially with regard to the continuously shrinking crude oil, natural gas and coal resources. In contrast to petrochemical reactions, catalytic conversion of biomass often proceeds in the liquid phase, due to the polarity of these molecules. The interaction of polar molecules with heterogeneous catalyst surfaces in the liquid phase will be studied in order to gain more insight into the molecular processes that lead to catalyst corrosion and deactivation. Important deactivation pathways are leaching of the active phase and the support, particle sintering, poisoning by strong adsorbing reaction intermediates and products as well as the formation of coke and oligomeric species. These processes will be investigated on well-defined model catalysts, i.e. flat substrates with supported catalyst particles, which allow for advanced characterization by microscopic, optical and electronic spectroscopy methods, preferentially under in-situ or operando conditions. As reaction systems the conversions of glycerol, glucose, succinic and maleic acid as well as cellulose will be used as typical model systems, containing the prototype functional groups (i.e., ROH, HRC=O, R2C=O and RCOOH) for biomass related conversions.The molecular level understanding will be later transferred to industrially relevant reaction conditions applying supported catalyst particles in high pressure/high temperature reactors with operando spectroscopic analysis of the working catalysts. Based on the gained knowledge, new concepts for the stabilization of the applied catalysts will be developed.