Studying carbon dioxide-reduction by Fe-Ni Sulfides with modern electronic structure methods: A case of multistate reactivity?

• Applicant: Professor Dr. Michael Roemelt
• Subject Area: Theoretical Chemistry: Molecules, Materials, Surfaces
• Term: from 2021 to 2025
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 471174587

• Final Report Year: 2025

Final Report Abstract

The main objective of this project was to study the experimentally observed electroreduction of CO2 to CO on pentlandite Fe4.5 Ni4.5 S8 surfaces by means of different theoretical approaches to obtain an atomistic and detailed picture of the reaction mechanism and the electronic factors governing the reactivity. After careful benchmarking of the methodology a series of periodic density functional theory calculations yielded insight into aforementioned reaction including preferred coordination surfaces, binding modes and reaction pathways. Additional multireference calculations of embedded cluster models provide a different perspective on the local electronic structure at the binding site for important intermediates of the reaction.