The ERC project SHAPE aims to develop a hierarchical multiscale methodology to account for the prediction of the nature of the active sites and the structure of the catalyst material for the first time fully integrated in first-principles-based multiscale simulations of supported-metal catalytic processes of technological relevance.
WP 1. Derivation of semi-empirical correlations and development of microkinetic models
WP1 deals with the first-principles assessment and refinement of scaling relations and semi-empirical models for the computationally affordable prediction of kinetic parameters on different relevant sites of the nanoparticles (different facets, steps, corners, defects).
Milestone 1: the successful achievement of WP1 will make possible the development of multi-site and coverage-dependent microkinetic models in close agreement with respect to first-principles calculations.
WP 2. Prediction of the shape and size of the nanoparticle.
The primary purpose of WP2 is that of revisiting and adapting models for the prediction of nano-particle shape and size as a function of the operating conditions, such as pressure, temperature and composition. As such, first the models are analysed and tested in the specific framework of catalyst engineering.
Milestone 2: the successful achievement of WP2 will allow for the validation and development of a structure-dependent multiscale framework, which will be used in the hierarchical microkinetic analysis of the experiments.
WP 3. Preparation, characterization and kinetic experiments.
WP3 deals with collection of experimental data, which will be used in the hierarchical multiscale methodology. In particular, WP3 is in charge of performing the kinetic test in annular reactor in order to derive a comprehensive exploration of the macroscopic kinetic behaviour of the reacting systems. This includes tests at different gas-hourly-space-velocity (GHSV) and relative co-feed of reactants and products to gain insights into the macroscopic reaction orders. The catalyst structure is also being monitored during reaction conditions, in order to make sure that structural changes of the material do not occur at particular operating conditions, with particular reference to carbonaceous material. Therefore, the strict kinetically controlled data in annular reactor are integrated with the operando Raman spectroscopy (operando-Raman annular reactor), in order to monitor possible changes of the structure (oxide formation, carbon deposition, …) in reacting conditions.
Milestone 3: WP3 will provide a strict kinetically controlled and comprehensive investigation of the kinetic behaviour of the reacting system along with a detailed experimental information concerning the characterization of the catalyst (prior, during, and after reaction) in terms of shape and size of the nanoparticles.
WP 4. Simulation of the experiments and application of the hierarchical methodology for the development of the structure-based microkinetic model.
The primary purpose of WP4 is the simulation of the experimental data in annular reactor (performed by WP3) using the methodologies developed and tested by WP1 and WP2. The simulation of the experiments allows for the identification of the reaction mechanism and the shape/size of the nanoparticle by the application of the hierarchical methodology. Specific methodologies are being developed to make possible the full integration of atomistic calculations in reactor modelling.
Milestone 4: WP4 will test and apply the hierarchical methodology for the development of the structure-based microkinetic models for the different processes.
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