Berlin 2024 – wissenschaftliches Programm

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CPP: Fachverband Chemische Physik und Polymerphysik

CPP 23: Modeling and Simulation of Soft Matter III

CPP 23.7: Vortrag

Mittwoch, 20. März 2024, 11:00–11:15, H 0107

Encapsulation Of Pt-based Clusters In ZIF-8: Insights From First Principles Simulations — •poonam p¹, kathrin l. kollmannsberger³, waldemar kaiser², julien warnan³, roland a. fischer³, and alessio gagliardi¹ — ¹Chair of Simulation of Nanosystems for Energy Conversion, Technical University of Munich, Garching bei Munich, Germany — ²Chair of Theory of Functional Energy Materials, Technical University of Munich, Garching bei Munich, Germany — ³Department of Chemistry, TUM School of Natural Sciences, Technical University of Munich

The reactivity of Pt-based catalysts dramatically depends on their size and detailed atomic structure. Recently, atom-precise nanoparticles have been generated from molecular ligand-stabilized clusters via encapsulation within MOFs. Our work aims to rationalize the underlying encapsulation mechanism of the ligand-stabilized Pt-based clusters using first-principles simulations. Using Density Functional Theory calculations, we determine the interaction of ZIF-8 precursors with the CO ligands of the Pt-clusters and reveal chemically distinct sites of all the considered clusters, which favor the attraction of Zn2+ ions in solution. AIMD simulations of Pt-based clusters in an explicit methanol solvent model shed light on the competition between the attraction of Zn2+ and the Pt-clusters and the desorption of Zn2+ by solvation with methanol molecules, revealing the importance of bridging CO ligands to create a Zn-rich environment around the Pt-cluster and to guarantee the successful encapsulation.

Keywords: Nanocluster; MOFs; Self-assembly; Computational Materials Sciences; DFT and AIMD