Final Report Summary - ICKARUS (Intrinsic Catalytic Kinetics Analyzed and Reconciled with Industrial Conditions)
Interactions of hydrocarbon molecules with active sites on the surface of Pt-based catalysts determine the efficiency of many megaton-per-year processes in chemical industry, ultimately affecting the global sustainability of modern life-style. The ICKARUS project set out to improve our understanding of some of these molecular-scale processes and to develop more efficient catalysts for hydrocarbon processing. The focus of the ICKARUS project was on the dehydrogenation of light alkanes, propane in particular, over a novel class of bimetallic Pt-based catalysts containing Ga, In, or Sn. Propane dehydrogenation was chosen as a model reaction of the ICKARUS project because it has recently attracted considerable attention as a source of high-quality propylene, one of the most important base-chemicals of modern industry. Conventional Pt-based catalysts currently used in industry to drive this process suffer from deactivation due to coke formation and sintering. The catalysts investigated in the ICKARUS project address these issues and exhibit better performance as a result of innovative way by which active Pt nanoparticles on their surfaces are alloyed with modifying elements (Ga, In, Sn).
After two years of research efforts involving a number of complementary experimental and theoretical methods, we achieved the following three major results. First, we have determined that the highly-selective state of Pt-based bimetallic catalysts emerges as a result of blocking of certain non-selective catalytic sites by carbon deposits formed on the catalyst during the initial period of alkane dehydrogenation. Second, we elucidated a highly dynamic picture of the formation and segregation of Pt-M alloys on the catalytic surface (where M stands for either Ga, In, ar Sn), which is induced by switching between reductive and oxidative gas environments. The catalysts undergo such periodic changes of the gas environment during their industrial life-times whereby reductive periods of alkane dehydrogenation are interrupted by oxidative periods of catalyst regeneration via coke burn-off. Finally, as part of the ICKARUS project, we have deployed and validated a 3rd-generation Temporal Analysis of Products (TAP) instrument used for advanced kinetic characterization of catalytic reactions (http://en.wikipedia.org/wiki/Temporal_analysis_of_products). The start-up of this cutting-edge facility within the European Research Area will have a lasting impact on the field of heterogeneous catalysis in Europe.
As a result of this IIF Marie Curie Fellowship, I have acquired multiple additional skills which made me a better scientist and improved my prospects as academic researcher. I have engaged in scientific collaboration with outstanding researchers in Belgium and throughout the globe, presented my work at international congresses, and published several peer-reviewed articles. Last but not least, I transferred some of my own skills to my colleagues at the host laboratory.
After two years of research efforts involving a number of complementary experimental and theoretical methods, we achieved the following three major results. First, we have determined that the highly-selective state of Pt-based bimetallic catalysts emerges as a result of blocking of certain non-selective catalytic sites by carbon deposits formed on the catalyst during the initial period of alkane dehydrogenation. Second, we elucidated a highly dynamic picture of the formation and segregation of Pt-M alloys on the catalytic surface (where M stands for either Ga, In, ar Sn), which is induced by switching between reductive and oxidative gas environments. The catalysts undergo such periodic changes of the gas environment during their industrial life-times whereby reductive periods of alkane dehydrogenation are interrupted by oxidative periods of catalyst regeneration via coke burn-off. Finally, as part of the ICKARUS project, we have deployed and validated a 3rd-generation Temporal Analysis of Products (TAP) instrument used for advanced kinetic characterization of catalytic reactions (http://en.wikipedia.org/wiki/Temporal_analysis_of_products). The start-up of this cutting-edge facility within the European Research Area will have a lasting impact on the field of heterogeneous catalysis in Europe.
As a result of this IIF Marie Curie Fellowship, I have acquired multiple additional skills which made me a better scientist and improved my prospects as academic researcher. I have engaged in scientific collaboration with outstanding researchers in Belgium and throughout the globe, presented my work at international congresses, and published several peer-reviewed articles. Last but not least, I transferred some of my own skills to my colleagues at the host laboratory.