Modulated thermo- and electro-catalytic reactors for fast catalyst and kinetic model screening

Catalyst development is slow because each catalyst is tested at steady state, one condition at a time, and the kinetic model is built afterward from a limited data set. Forced dynamic operation changes this. Periodic modulation of feed composition, pressure, temperature, or electrode potential produces transient responses that contain information on adsorption, surface reaction steps, and catalyst restructuring. With fast online analysis and operando characterization, one modulated experiment can replace many steady-state tests and discriminate between kinetic models in a fraction of the time. MuRE work on CO2 hydrogenation and dry reforming of methane has shown that periodic switching changes the catalyst structure and its coking behavior. The intern will work with modulated reactors for thermocatalytic reactions (CO2 hydrogenation to methanol, reverse water-gas shift, dry reforming of methane) and electrocatalytic reactions (CO2 reduction in flow cells). Tasks, according to the background: - Design and implementation of modulation sequences: concentration steps and pulses, isotopic switches, temperature and pressure cycles, potential steps and pulses. - Transient experiments with online mass spectrometry and gas chromatography. - In situ and operando characterization linked to the transient data, for example DRIFTS, Raman, XRD, electrochemical impedance spectroscopy, and synchrotron X-ray absorption where beamtime is available. - Microkinetic and data-driven models, model discrimination, and model-based design of experiments.

- Modulation protocol for one catalyst family and reaction, including timing, amplitudes, and analysis settings. - Transient data sets and their comparison with steady-state data for the same catalyst. - Correlation of transient kinetics with operando characterization. - Microkinetic or data-driven model with parameter estimates and a model discrimination result. - Internship report and presentation; contribution to a peer-reviewed publication where results allow.