Molecular catalyst data driven reaction monitoring and control in homogeneous catalysis

• Applicants: Professor Dr.-Ing. Christof Hamel; Privatdozent Dr. Andreas Vorholt
• Subject Area: Chemical and Thermal Process Engineering ; Technical Chemistry
• Term: since 2024
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 537105915

Studies of catalyst deactivation in homogeneous catalysis need to be intensified and integrated into comprehensive catalyst design. Especially considering the use of renewables as feedstock with fluctuating quality the problem of catalyst deactivation should be addressed. A fundamental understanding of the deactivation mechanisms and the mathematical description of catalyst deactivation is the basis for a future feedstock substitution in the chemical industry. It enables to design suitable feedstock/catalyst combinations for sustainable catalyzed chemical processes. The main objective of this project is to provide a deeper understanding of deactivation mechanisms in homogeneous catalysis and how to avoid accompanying negative effects on catalyzed reactions for continuous reaction processes. Four deactivation modes will be covered in detail during this project 1) long-term deactivation (ageing), 2) catalyst losses due to leaching of continuous process, 3) deactivation induced by gas/liquid mass transport limitations, 4) impurity-induced deactivation. Methodically, this will be achieved by using multi-spectroscopic measurements combined with advanced chemometric analysis during kinetic and continuous experiments, including catalyst separation and recycling, on process level. The resulting time-resolved molecular data of catalyst species and reactants will be used to develop, reduce and parametrize new mechanistic kinetic models of deactivation. These models serve as basis for model-based process control and optimization, e.g. by catalyst dosing strategies, as a countermeasure for negative effects on catalyzed reactions that will be validated in long-term continuous reaction campaigns in miniplants. Consequently, a comprehensive approach should address deactivation mechanism identification, quantification and model-based compensation/prevention. Such an approach is still underrepresented in homogeneous catalysis and is proposed in that project applied for covering the following procedure a) operando multi-spectroscopic deactivation studies combining complementary techniques (FTIR, Raman, NMR, GC-MS), b) kinetic deactivation studies addressing 4 deactivation modes in short-term batch and long-term continuous operation applying process dynamics (perturbations), c) mechanistic kinetic modelling of deactivation modes to predict catalyst dosing, d) validation of dosing strategies in long-term, continuous operated miniplant campaigns, e) total process simulation/control to assess further countermeasures for catalyst deactivation.

• DFG Programme: Research Grants
• Co-Investigator: Dr.-Ing. Martin Gerlach