Periodic Reporting for period 1 - DynaMMO (Tackling limitations of future relevant thermo-chemical reactions by exploiting the dynamic surface behaviour of complex mixed metal oxides)
Période du rapport: 2023-08-01 au 2026-01-31
For a sustainable future highly active, selective and stable catalyst are of utmost importance for the chemical industry. The conventional steady-state operation of catalytic reactors reaches its limit.
This project opens up new perspectives on the opportunities of tailored oxide surfaces. We aim to develop a dynamic responsive catalysts (DRC) that change their surface structure dependent on the oxidizing or reductive character of the reactant mixture. Combined with oscillation between reducing and oxidizing atmosphere in forced periodic operation (FPO) our concept opens unprecedented opportunities for surface engineering: At low reduction degree, the DRC-FPO concept allows activation and net stabilization of active/selective metastable sites that are thermodynamically not accessible under conventional steady-state operation. Furthermore, at high reduction degrees, the DRC-FPO concept enables reversible formation of highly dispersed active nanoparticles out of the mixed metal oxide host structure. Upon oxidative treatment, the atoms of nanoparticles can reintegrate into the host structure at ultimate dispersion. This is a unique way to overcome irreversible catalyst deactivation by nanoparticle sintering.
With our expertize on mixed metal oxides based like spinels and perovskites we will enable the DRC functionality by compositional tailoring and resolve general trends. To leverage the full potential of this approach, we aim to explore all relevant effects in four future relevant demonstrator reactions at low and high temperatures as well as oxidizing and reductive environment by a combination of synthetic, analytic, reaction engineering and operando characterization methodologies.
The acquired basic knowledge and proven feasibility of the DRC-FPO concept opens a paradigm-shift in the operation of catalysts. It generates ground-breaking ways to create defined active surface sites and avoid catalyst deactivation. This novel approach tackles current limitations of heterogeneous catalysis.
This project opens up new perspectives on the opportunities of tailored oxide surfaces. We aim to develop a dynamic responsive catalysts (DRC) that change their surface structure dependent on the oxidizing or reductive character of the reactant mixture. Combined with oscillation between reducing and oxidizing atmosphere in forced periodic operation (FPO) our concept opens unprecedented opportunities for surface engineering: At low reduction degree, the DRC-FPO concept allows activation and net stabilization of active/selective metastable sites that are thermodynamically not accessible under conventional steady-state operation. Furthermore, at high reduction degrees, the DRC-FPO concept enables reversible formation of highly dispersed active nanoparticles out of the mixed metal oxide host structure. Upon oxidative treatment, the atoms of nanoparticles can reintegrate into the host structure at ultimate dispersion. This is a unique way to overcome irreversible catalyst deactivation by nanoparticle sintering.
With our expertize on mixed metal oxides based like spinels and perovskites we will enable the DRC functionality by compositional tailoring and resolve general trends. To leverage the full potential of this approach, we aim to explore all relevant effects in four future relevant demonstrator reactions at low and high temperatures as well as oxidizing and reductive environment by a combination of synthetic, analytic, reaction engineering and operando characterization methodologies.
The acquired basic knowledge and proven feasibility of the DRC-FPO concept opens a paradigm-shift in the operation of catalysts. It generates ground-breaking ways to create defined active surface sites and avoid catalyst deactivation. This novel approach tackles current limitations of heterogeneous catalysis.
After 30 month of the 5 Year project we have successfully established synthesis procedures yielding in highly phase pure mixed metal oxides in a wide range of chemical compositions that allows us to tailor the materials redox properties as intended. The newly generated phase pure synthesis protocolls enables us now to tailor catalysts that enables the DRC-FPO approach. In addition, a flexible reactor system was designed, constructed and comissioned in order to start now the catalytic investigations on the activity in our test reactions.
In our first results we see that the dynamic approach in combination with dynamic catalysts can be advantageous over steady state operation.
In our first results we see that the dynamic approach in combination with dynamic catalysts can be advantageous over steady state operation.
With the established new sysnthesis route we are practically able to generate phase pure spinels and perovskites in any elemental combination as desribed in the proposal. It is hence a big milestone as it allows us to draw direct conclusions about the actions taking place during catalyis and which phase is essential for high catalytic activity. First catalytic results show the advantageous effect of dynamic operation. In future work we will analyze in more detail the effects of dynamic operation on the reactivity and the structure of the catalysts.