Project Details
Projekt
Tackling irreversible catalyst deactivation: knowledge-driven design and operation of dynamic responsive methanation catalysts
Applicants
Professorin Dr. Tanja Franken; Professor Dr.-Ing. Hannsjörg Freund; Dr.-Ing. Michael Rubin
Subject Area
Technical Chemistry
Term
since 2018
Project identifier
Deutsche Forschungsgemeinschaft (DFG) - Project number 406911435
The general objective of this project is to enable a holistic, fundamental yet mathematically manageable description of the methanation reaction under transient and potentially deactivating conditions taking forced changes of the catalyst into account. This objective is pursued for two different catalyst systems, the SPP’s industrial methanation reference catalyst (IMRC) and a novel dynamic responsive methanation (DRM) catalyst which holds potential to overcome irreversible deactivation of conventional Ni-based CO2 methanation catalysts. Therefore, this project combines synthesis, characterization and exploration of a spinel based DRM catalyst. Enabled by optimized reducibility of the material, the DRM catalyst developed in this project responds to externally applied forced changes by formation and reintegration of active Ni particles.Methods and results obtained in funding phase I for the SPP’s Ni/Al2O3 based IMRC will be extended for the DRM catalyst in phase II. For this, two dedicated experimental set-ups for spatially-resolved DRIFTS (SRD) operando analysis of species adsorbed on the catalyst surfaces as well as a dedicated kinetic set-up (KIN reactor) from phase I are utilized to validate and explore dynamic models that consider the change of active sites (deactivating or activating) during transient reaction conditions. A novel DRM catalyst will be synthetized and catalytically investigated in a catalytic performance (PER) test reactor which allows for the realization of highly transient reaction conditions by fast changes of applied gas mixtures. A thorough characterization of an ideal DRM catalyst by ex situ, in situ and operando methods within this consortium and in cooperation with further SPP2080 consortia allows to establish a solid state kinetic model, which can be integrated into the reaction kinetic model. This way, kinetic models of different complexity are established, including steady-state kinetic models, extensions of the latter for including mechanisms to describe catalyst deactivation and regeneration as well as dynamic kinetic models considering surface coverages for describing the reaction under transient conditions. On this model basis, optimization methods will be developed that reveal optimal operation policies to enable both, high methane yields and long term catalyst operation.The close collaboration of experts within this project consortium covering the areas “operando/spectroscopy” (A), ”kinetic modelling” (C), ”targeted material design” (D) and ”reactor concepts” (E) not only contributes to the description and understanding of catalysts under dynamic operation, but also contributes to a novel approach to exploit unwanted transients to enable enhanced long term performance of catalysts.
DFG Programme
Priority Programmes
