10:00. Feliu Maseras, Group leader at the Institute of Chemical Research of Catalonia,Tarragona, Spain, will present: Computationally Multimetallics Cooperative Catalysis
Multimetallic catalysis is an emerging field of research further expanding the frontiers of homogeneous catalysis. The simultaneous activation of two substrates by different catalytic entities can be responsible for rate acceleration and modified selectivity, and may ultimately lead to the synthesis of novel compounds. The nature of the metal moieties is the responsible of the activation step, while selectivity mainly derives from non-covalent interactions between substrates and catalysts. The eventual control of both activation and coupling may open the way for the design of novel synthetic routes proceeding in mild conditions. Such control of conditions will be more easily achievable if a detailed mechanistic understanding is available, but this is difficult to acquire from purely experimental methods.
DFT calculations can be very useful in this concern. Theoretical models can provide fundamental insights on the substrate activation by metals as well as on the interactions between the different catalysts. This will allow the deciphering at the atomic level of the preferential pathways leading to different reaction products.
10:45. Maren Podewitz, Assistant professor at the Institute of Materials Chemistry, TU Wien, Vienna, Austria, will present: “Towards predictive and operando computational catalysis - Recent advancements for transition-metal chemistry"
Catalysis is one of the pillars to a more sustainable manufacturing processes by facilitating chemical reactions under mild conditions and reducing the required energy for the transformation. In recent years, experimental efforts have been accompanied by theoretical investigations that provide atomistic insights in bond formation and cleavage as well as in reactivity and selectivity – information that is not or only partially available in experiment. The reliability of such theoretical investigations crucially depends on the accuracy of the chemical model and computational methodology.
However, many current computational studies base their investigations on available X-ray crystal data, considering only one specific conformation and describing only implicit solvation. In contrast, most chemical reactions take place in the liquid phase. Relevant conformations may differ from the X-ray crystal structure and specific solute-solvent interactions might impact reactivity. This may particularly be the case for highly flexible transition-metal catalysts that can adjust their geometries to perturbations by the environment. Yet, these effects are rarely included in computational studies but can make up substantial errors.
In this talk, I present selected examples on how to tackle explicit solute-solvent interactions,
- [1] and generate conformers in explicit solvent
- [2] to improve state of the art computational modelling of reaction mechanisms and transition-metal catalysts.
- [3,4,5] I will show how improved chemical models were essential to predict reactivity and selectivity in these transition metal catalysts.
[1] M. Steiner, T. Holzknecht, M. Schauperl, M. Podewitz* Molecules, 26 (2021), 1793.
[2] 2. R. A. Talmazan and M. Podewitz* J. Chem. Inf. Model. 63 (2023) 5400-5407.
[3] K. Herz, M. Podewitz*, L. Stöhr, D. Wang, W. Frey, K. R. Liedl, S. Sen, M. R. Buchmeiser*. J. Am.
Chem. Soc., 141 (2019), 8264-.
[4] M. Podewitz,* S. Sen, M. R. Buchmeiser, Organometallics, 40 (2021), 2478–2488.
[5] R. A. Talmazan, R. Monroy, F. del Rio-Portilla, I. Castillo, M. Podewitz* ChemCatChem, (2022), 14
(2022), e202200662.