SKM 2021 – scientific programme
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CPP: Fachverband Chemische Physik und Polymerphysik
CPP 3: Polymer Physics
CPP 3.8: Talk
Monday, September 27, 2021, 16:00–16:15, H3
Free energy considerations in confined heterocatalysis in a supported ionic liquid phase — •Takeshi Kobayashi1, Hamzeh Kraus2, Felix Ziegler3, Michael Buchmeiser3, Niels Hansen2, and Maria Fyta1 — 1Institute for Computational Physics, University of Stuttgart — 2Institute of Thermodynamics and Thermal Process Engineering, University of Stuttgart — 3Institute of Polymer Chemistry, University of Stuttgart
The high potential of performing heterocatalysis in a confined mesoporous media within a supported ionic liquid phase (SILP) is studied using Molecular Dynamics (MD) simulations. Specifically, we investigate the possibility of immobilizing catalytic molecules in confined media in a biphasic solution consisting of an ionic liquid (IL) and heptane as the second phase within a pore with a lateral size of about 5 nm. Divalent cationic Ru-alkylidene N-heterocyclic carbene catalysts are placed in the solution. We were able to monitor the immobilization of the catalysts within the IL for achieving higher turnover rates in the catalytic reactions. We further analyze the accumulation and diffusion of the molecules within the pore, the influence of steric and IL-specific effects, the structuring of a solvent environment, and their synergistic interactions with the catalytic molecules. The free energy calculations reveal that the catalytic reaction must occur at the interface between the heptane and the IL. Our investigations are supported by experimental evidence and provide a deeper understanding of the inherent details that control a rational design of a linker-free catalyst immobilization in nanometer-sized templates for catalytic applications.