Speaker
Description
We rely on hybrid QM:QM methods that combine high-level MP2 on cluster models with low-level DFT+D2 on periodic models to obtain accurate potential energy surfaces (PESs) for even extended and complex periodic systems. The hybrid MP2:(DFT+D2) PESs are counterpoise corrected (CPC) for the basis set superposition error (BSSE) and extrapolated to the complete basis set (CBS) limit. A posteriori, CCSD(T) coupled-cluster correlation effects are estimated as CCSD(T)-MP2 energy differences. The multi-level hybrid MP2/CPC-CBS:(DFT+D2) + ΔCCSD(T) PESs are designed by using the new MonaLisa program [1].
Within this computational strategy we reached chemical accuracy limits (± 4 kJ/mol on the electronic energy) and extended the benchmark data available for periodic systems to experimentally well-known processes from the field of heterogeneous catalysis: (i) adsorption of light alkane molecules in the H-chabazite zeolite [2], (ii) adsorption of methane and ethane monolayers on the MgO(001) surface [3] and (iii) methylation reactions via methanol of light alkene molecules in the H-ZSM-5 zeolite [4].
References
[1] F. A. Bischoff, M. Alessio, M. John, M. Rybicki and J. Sauer, Multi-Level Energy Landscapes: The MonaLisa Program, available from: https://www.chemie.hu-berlin.de/de/forschung/quantenchemie/monalisa/, Humboldt-University: Berlin, 2017.
[2] G. Piccini, M. Alessio, J. Sauer, Y. Liu, R. Kolvenbach, A. Jentys and J. A. Lercher, J. Phys. Chem. C 2015, 119, 6128.
[3] M. Alessio and J. Sauer, Phys. Chem. Chem. Phys. 2018, accepted.
[4] G. Piccini, M. Alessio and J. Sauer, Angew. Chem. Int. Ed. 2016, 54, 5235.
