Final Report Summary - I-CAD (Innovative Catalyst Design for Large-Scale, Sustainable Processes)
Our society is facing various challenges of different kinds. In the area of ‘chemicals and fuels’ sustainable feedstock supply and utilization are burning hot topics. Conventional fossil sources are becoming harder to be exploited economically and, more importantly, are inherently equivalent with an open-ended economy. Following up on climate action, circularity should be pursued, e.g. by employing feeds that can be generated in a time-frame of one or a few seasons, rather than eons. Renewable biomass or waste (including plastics), hence, constitute a promising starting point for a more sustainable production of chemicals and fuels.
The conversion processes involved in the transformation of such feeds to the desired products rely on catalysts to ensure sufficiently high conversion rates and selectivities. The design of such catalysts has typically been an intuition guided trial and error process. By acquiring a fundamental understanding of the chemical conversion steps and how the catalysts intervenes at the molecular level, a strategic advantage can be achieved. It’s a point of discussion, however, whether a purely experimental strategy should be adopted or whether this should include modeling and if so, what kind of modeling?
As part of the i-CaD project, the so-called microkinetic modeling route has been adopted to more rationally design new generations of catalysts. Despite the term ‘modeling’, it combines experimental and simulation work, aiming at acquiring detailed information on the elementary chemical kinetics of the conversion processes. Such specific information allows for the construction of elementary steps based reaction mechanisms and the quantification of the impact of the catalyst properties on the kinetics. E.g. the impact of properties such as acid or base strength of the active sites on the rate of various elementary steps can be determined for optimizing a reaction selectivity, yield, etc.
Within the context of i-CaD, this microkinetic modeling based methodology has been applied to a variety of reactions such as hydrodeoxygenation (or, more generally, hydrotreatment), hydrogenolysis, ethanol dehydrogenation, aldol condensation, etc. all serving a specific role in the conversion of renewable feeds into chemicals and fuels which can substitute the present, fossil based ones. More particularly for the aldol reactions, the research has lead to a stable catalyst exhibiting a significant reaction rate. Deactivation by site blocking and support degradation has been, for the first time, successfully mitigated and opportunities for further enhancement of the catalytic performance have still been identified. Thanks to the ERC support, bridges have been laid with other top research groups in the field, such as the Chris Jones group at Georgia Tech (USA – editor in chief of ACS Catalysis). The ERC funds were not simply used as such but additional funding, e.g. for a long stay abroad by the Flemish science foundation have been requested and achieved. For hydrodeoxygenation on the other hand, the behavior of a wide variety of model components on an extended range of catalysts has been mapped. It generated crucial insight in preferential adsorption and, hence, conversion, behavior, allowing to reliably extrapolate the elementary kinetics as observed for model components to more complex mixtures. Such basic reaction engineering knowledge represents a solid corner stone for the design of next generation materials, e.g. the Picula catalysts as developed by the Boreshkov Institute of Catalysis (prof. Vadim Yakovlev) with whom a collaboration has been established that is being extended beyond the horizon of the ERC project thanks to funding opportunities by the Russian and Flemish science foundation.
From the methodological point of view, the ERC consolidator grant i-CaD has allowed me to further develop the software package ‘microkinetic engine’ which aims at popularizing microkinetic modeling among non-expert modelers. It does so by eliminating the need for programming by the user. The potential value of the tool was specifically recognized by the ERC via 2 Proof of Concept grants for the development of a graphical user interface for the tool, as well as for rendering the mathematical convergence more stable. During the course of the project a start-up, i.e. ShARP Engineering, has been founded aiming at generating further awareness on basic reaction and reactor engineering in support of microkinetic modeling.
The ERC project has granted me unprecedented possibilities for the development of my career. It has boosted my scientific output and I’ve been able to acquire a well-recognized position. It has opened doors for consecutive projects of all kinds, ranging from bilateral collaborations with industry to large-scale government funded projects. It has allowed me to guarantee long term stability in my research group, not only during the course of the project, but even beyond. I’m, hence, extremely grateful for the opportunities the ERC has offered me
The conversion processes involved in the transformation of such feeds to the desired products rely on catalysts to ensure sufficiently high conversion rates and selectivities. The design of such catalysts has typically been an intuition guided trial and error process. By acquiring a fundamental understanding of the chemical conversion steps and how the catalysts intervenes at the molecular level, a strategic advantage can be achieved. It’s a point of discussion, however, whether a purely experimental strategy should be adopted or whether this should include modeling and if so, what kind of modeling?
As part of the i-CaD project, the so-called microkinetic modeling route has been adopted to more rationally design new generations of catalysts. Despite the term ‘modeling’, it combines experimental and simulation work, aiming at acquiring detailed information on the elementary chemical kinetics of the conversion processes. Such specific information allows for the construction of elementary steps based reaction mechanisms and the quantification of the impact of the catalyst properties on the kinetics. E.g. the impact of properties such as acid or base strength of the active sites on the rate of various elementary steps can be determined for optimizing a reaction selectivity, yield, etc.
Within the context of i-CaD, this microkinetic modeling based methodology has been applied to a variety of reactions such as hydrodeoxygenation (or, more generally, hydrotreatment), hydrogenolysis, ethanol dehydrogenation, aldol condensation, etc. all serving a specific role in the conversion of renewable feeds into chemicals and fuels which can substitute the present, fossil based ones. More particularly for the aldol reactions, the research has lead to a stable catalyst exhibiting a significant reaction rate. Deactivation by site blocking and support degradation has been, for the first time, successfully mitigated and opportunities for further enhancement of the catalytic performance have still been identified. Thanks to the ERC support, bridges have been laid with other top research groups in the field, such as the Chris Jones group at Georgia Tech (USA – editor in chief of ACS Catalysis). The ERC funds were not simply used as such but additional funding, e.g. for a long stay abroad by the Flemish science foundation have been requested and achieved. For hydrodeoxygenation on the other hand, the behavior of a wide variety of model components on an extended range of catalysts has been mapped. It generated crucial insight in preferential adsorption and, hence, conversion, behavior, allowing to reliably extrapolate the elementary kinetics as observed for model components to more complex mixtures. Such basic reaction engineering knowledge represents a solid corner stone for the design of next generation materials, e.g. the Picula catalysts as developed by the Boreshkov Institute of Catalysis (prof. Vadim Yakovlev) with whom a collaboration has been established that is being extended beyond the horizon of the ERC project thanks to funding opportunities by the Russian and Flemish science foundation.
From the methodological point of view, the ERC consolidator grant i-CaD has allowed me to further develop the software package ‘microkinetic engine’ which aims at popularizing microkinetic modeling among non-expert modelers. It does so by eliminating the need for programming by the user. The potential value of the tool was specifically recognized by the ERC via 2 Proof of Concept grants for the development of a graphical user interface for the tool, as well as for rendering the mathematical convergence more stable. During the course of the project a start-up, i.e. ShARP Engineering, has been founded aiming at generating further awareness on basic reaction and reactor engineering in support of microkinetic modeling.
The ERC project has granted me unprecedented possibilities for the development of my career. It has boosted my scientific output and I’ve been able to acquire a well-recognized position. It has opened doors for consecutive projects of all kinds, ranging from bilateral collaborations with industry to large-scale government funded projects. It has allowed me to guarantee long term stability in my research group, not only during the course of the project, but even beyond. I’m, hence, extremely grateful for the opportunities the ERC has offered me