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MO: Fachverband Molekülphysik

MO 29: Cluster and Nanoparticles II (joint session MO/A)

MO 29.2: Talk

Friday, March 14, 2025, 11:30–11:45, HS XV

Dynamics of CO₂ activation by transition metal ions — •Marcel Meta, Maximilian E. Huber, Martin Wedele, and Marcel Meta — RPTU Kaiserslautern-Landau und Forschungszentrum OPTIMAS, Fachbereich Chemie, Kaiserslautern, Germany

Here, we present a joint experimental and theoretical study of the dynamics of ion-molecule reactions. We focus on the oxygen atom transfer (OAT) reaction between transition metal ions and carbon dioxide M ⁺ + CO ₂ → MO ⁺ + CO (M ⁺ =Ta ⁺ ,Nb ⁺ ,Zr ⁺ ) [1,2]. Indirect dynamics were observed for all reactions, despite the fact that the thermal rates are close to the collision rate and the reaction is exothermic in all cases. The investigated reactions have a multi-state character and require an inter-system crossing (ISC) for their occurrence. These findings indicate the presence of a bottleneck along the reaction. The nature of the bottleneck (submerged transition state versus ISC) was investigated in a collaborative effort.
In order to achieve this, angle and energy differential cross-sections were measured using 3D velocity map imaging at different collision energies. Thermal rate constants were obtained using selected ion flow tube (SIFT). These experimental findings were supplemented by high-level theory and trajectory simulations [3]. In addition, this approach allows us to make precise assertions regarding the distribution of energy. [1] M. E. Huber et al. 8670, 26, Phys. Chem. Chem. Phys. (2024). [2] M. Meta et al., 5524, 14, J. Phys. Chem. Lett (2023). [3] Y. Liu et al. J. Am Chem. Soc., 14182, 146 (2024).

Keywords: VMI; Collision; Ion-Molecule-Reaction; Dynamics