Atomistic Understanding of CO2 Reduction using Molecular Catalysts

• Applicant: Dr. Philipp Schienbein
• Subject Area: Theoretical Chemistry: Electronic Structure, Dynamics, Simulation
• Term: since 2025
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 563085417

Electrochemical CO2 reduction offers a promising pathway toward a sustainable, carbon neutral industry by converting CO2 into high-value feedstocks. Despite significant research efforts, no catalyst has yet been identified that efficiently facilitates this reaction. A key chal lenge lies in the lack of a detailed microscopic understanding of the reaction mechanism and the intermediate states involved. The main objective of this project is to develop a comprehensive atomistic understanding of CO2 reduction at molecular catalysts. Experimental studies have revealed a delicate synergy between the catalyst molecule and the solvent, which uncovered that the solvent is not an inert reaction medium, but actively influences the reaction parameters. Consequently, it is essential for theoretical models to explicitly incorporate solvent molecules and account for their thermal fluctuations in the liquid state. In this project, we will investigate a highly relevant catalytic system – one of the leading candidates for electrochemical CO2 reduction – using atomistic machine learning molecular dynamics simulations for the first time. Vibrational spectra will be calculated from these simulations and compared with previously reported experimental data to validate the predictive accuracy of the simulations. By correlating calculated microscopic structural, dynamical, thermodynamic, and kinetic properties with reported macroscopic experimental observations, we aim to identify trends and establish structure-function relationships. These insights will be crucial not only for systematically improving catalytic performance, but also for optimizing complementary aspects, such as substituting hazardous solvents with safer, environmentally friendly alternatives.

• DFG Programme: Research Grants