Assistant professor Irene M.N. Groot
Leiden Institute of Chemistry
Leiden University
the Netherlands

Seeing is believing: atomic-scale imaging of catalysts under reaction conditions

The atomic-scale structure of a catalyst under reaction conditions determines its activity, selectivity, and stability. Recently it has become clear that essential differences can exist between the behavior of catalysts under industrial conditions (high pressure and temperature) and the (ultra)high vacuum conditions of traditional laboratory experiments. Differences in structure, composition, reaction mechanism, activity, and selectivity have been observed.

These observations indicated the presence of the so-called pressure gap, and made it clear that meaningful results can only be obtained at high pressures and temperatures. However, most of the techniques traditionally used to study catalysts and their reactions were designed to operate under (ultra)high vacuum conditions. To bridge the pressure gap, the last years have seen a tremendous effort in designing new instruments and adapting existing ones to be able to investigate catalysts in situ under industrially relevant conditions.

In this talk, I will give an overview of the in situ imaging techniques we use to study the structure of model catalysts under industrial conditions of atmospheric pressures and elevated temperatures. We have developed set-ups that combine an ultrahigh vacuum environment for model catalyst preparation and characterization with a high-pressure flow reactor cell, integrated with either a scanning tunneling microscope or an atomic force microscope.

With these set-ups we are able to perform atomic-scale investigations of well-defined model catalysts under industrial conditions. Additionally, we combine the structural information from scanning probe microscopy with time-resolved mass spectrometry measurements on the gas mixture that leaves the reactor. In this way, we can correlate structural changes of the catalyst due to the gas composition with its catalytic performance. Furthermore, we use other in situ imaging techniques such as transmission electron microscopy, surface X-ray diffraction, and optical microscopy, all combined with mass spectrometry.

This talk highlights a short overview of the instruments we developed and illustrates their performance with results obtained for different model catalysts and reactions. As a proof of principle, results for the fruit fly of surface science, i.e. CO oxidation, will be shown. But additionally, results for more complex reactions such as NO oxidation and reduction, Fischer-Tropsch synthesis, and hydrodesulfurization will be discussed.

Host: Associate professor Jeppe Vang Lauritsen, iNANO and Department of Physics and Astronomy.