Automatisierte Generierung von Mikrokinetiken für heterogen katalysierte Reaktionen unter Berücksichtigung korrelierter Unsicherheiten**

Kreitz, Bjarne; Lott, Patrick; Studt, Felix; Medford, Andrew J.; Deutschmann, Olaf; Goldsmith, C. Franklin

doi:10.1002/ange.202306514

Automatisierte Generierung von Mikrokinetiken für heterogen katalysierte Reaktionen unter Berücksichtigung korrelierter Unsicherheiten**

Journal Article · Tue Aug 22 00:00:00 EDT 2023 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202306514· OSTI ID:1996313

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School of Engineering Brown University 184 Hope Street Providence RI 02912 USA, Institute for Chemical Technology and Polymer Chemistry Karlsruhe Institute of Technology Engesserstr. 20 76128 Karlsruhe Deutschland
Institute for Chemical Technology and Polymer Chemistry Karlsruhe Institute of Technology Engesserstr. 20 76128 Karlsruhe Deutschland
Institute for Chemical Technology and Polymer Chemistry Karlsruhe Institute of Technology Engesserstr. 20 76128 Karlsruhe Deutschland, Institute of Catalysis Research and Technology Karlsruhe Institute of Technology 76344 Eggenstein-Leopoldshafen Deutschland
School of Chemical and Biomolecular Engineering Atlanta GA 30318 USA
School of Engineering Brown University 184 Hope Street Providence RI 02912 USA

Abstract

Die Studie stellt eine ab initio basierte Methode für die automatische Konstruktion von detaillierten Mikrokinetiken vor, welche korrelierte Unsicherheiten in allen energetischen Parametern und Schätzroutinen berücksichtigt. Hierfür wurden innerhalb des Unsicherheitsraums des BEEF‐vdW Funktionals 2000 Mikrokinetiken für die Oxidationsreaktionen repräsentativer Abgasemissionen von stöchiometrischen Verbrennungsmotoren auf Pt(111) generiert und durch Multiskalenmodellierung mit Experimenten verglichen. Das Ensemble der Simulationsergebnisse unterstreicht die Bedeutung der Berücksichtigung von Unsicherheiten. Innerhalb dieses Ensembles ist es möglich, eine Mikrokinetik zu identifizieren, welche mit den experimentellen Daten übereinstimmt. Diese Mikrokinetik lässt sich auf ein einziges Austausch‐Korrelations‐Funktional zurückführen und legt nahe, dass Pt(111) das aktive Zentrum für die Oxidation leichter Kohlenwasserstoffe sein könnte. Die Studie bietet einen universellen Rahmen für die automatisierte Konstruktion von Reaktionsmechanismen unter Berücksichtigung korrelierter Unsicherheiten und ermöglicht eine DFT‐basierte Optimierung der Mikrokinetik auch für andere heterogen katalysierte Systeme.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0019441

OSTI ID:: 1996313

Alternate ID(s):: OSTI ID: 1996314

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 39 Vol. 135; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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