OpeSpeKin · Combined operando spectroscopy with model-based experimental design to study the mechanism of catalytic surface reactions

Global warming from CO2 emissions is one of the greatest challenges facing mankind. Catalysis offers the potential to utilize CO2 as a carbon source, however improved catalysts are required. To unlock the potential of catalytic CO2 conversion, it is neccessary to observe catalysts in-action ‘in-operando’ to design improved active sites and more active/selective and energy efficient processes. Operando spectroscopy is an effective technique in investigating the reactions that take place on catalyst surface. Combining operando spectroscopy with kinetics (spectrokinetics) offers a powerful approach for studying the underlying mechanism of the reaction. This approach can enhance our understanding of the surface reactions and further elucidate the role of surface intermediates in real time of reaction. In this work, the evolution of the concentration of reactants, surface species and products will be used jointly in kinetic modelling to understand the mechanism of the reaction. In most kinetic studies, the procedure leading to a possible reaction mechanism is experiment- and time-intensive. Therefore, in this research, model-based design of experiment (MBDoE) techniques will be employed in designing a set of experiments to obtain the most informative data for development of kinetic model.Overall, this research project intends to integrate operando spectroscopy with microkinetic modelling to rational design and optimization of new efcient catalytic systems for conversion of CO2.The project aims at:1.Optimizing operando spectroscopy set-up2.Developing alternative kinetic models from microkinetic analysis3.Employing MBDoE techniques to operando spectroscopy system4.Identification of reaction mechanism and precise estimation of kinetic parameters5.Investigating the correlation of surface species with observed reactivity