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MM: Fachverband Metall- und Materialphysik

MM 27: Data Driven Material Science: Big Data and Workflows IV

MM 27.3: Talk

Tuesday, March 19, 2024, 14:00–14:15, C 243

Synergistic catalytic sites in high-entropy metal hydroxide organic framework — Arkendu Roy, •Sourabh Kumar, Ana Guilherme Buzanich, Tilmann Hickel, Franziska Emmerling, and Biswajit Bhattachary — BAM, Bundesanstalt für Materialforschung und -prüfung, Richard-Willstätter-Str. 11, 12489 Berlin

Leveraging data-driven computational techniques accelerates catalytic process analysis and prediction, enabling materials discovery and chemical reaction optimization. Among such materials, high-entropy metal hydroxide organic frameworks (HE-MHOFs), with intricate structures surpassing conventional MOFs, are of special interest. In HE-MHOFs, high-entropy hydroxide layers are connected by ligands to form a superlattice, introducing structural disorder and diversity. Using the state-of-art ab initio calculations, the HE-MHOFs have been designed based on the stability of unary MHMOFs by constructing their ab initio Pourbaix diagram, followed by their synthesis using a conventional solvothermal process. The incorporation of different transition metals (TMs) alters the electronic structure, influencing adsorbate binding energy and catalytic activation potential. The SQS approach is used to deconvolute the atomic patterns and sample out the most favourable surfaces for OER investigations. Then the complexities in the proton-coupled electron transfer OER reaction mechanism are addressed by constructing a potential energy surface for each redox-active TM and comparing it to parent unary MOFs. A confirmation through in-situ XPS and EDX mapping complements our computational approach.

Keywords: ab initio; metal-organic frameworks; oxygen evolution reaction; Pourbaix diagram