Towards a Conceptual Transfer of Gas-Phase Ion-Chemistry into the Condensed Phase

• Applicant: Dr. Burkhard Butschke
• Subject Area: Inorganic Molecular Chemistry - Synthesis and Characterisation
• Term: since 2017
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 372823605

The aim of the research project is the conceptual transfer of gas-phase ion-chemistry into the condensed phase. Due to the very different conditions in both environments, such a transfer is not trivial and has not been studied sufficiently so far. Conversely, mass-spectrometric methods are increasingly used to study processes in solution. Therefore, it is crucial to gain a deeper understanding of the relationship of chemical reactivity in both phases. A goal derived from these efforts is to make practical use of the results gained in gas-phase experiments. The focus is on the activation of small molecules, bond-forming reactions, and oxygen-atom transfer. The ultimate goal is the development of gas phase-inspired catalytic transformations. Towards this goal, we use model systems, the reactivity of which we investigate both in gas-phase experiments and in solution. These experiments enable the determination of the influence of solvent molecules, counterions, and additional ligation on intrinsic-reactivity patterns. One of the targeted model systems involves heterobimetallic coinage-metal platinum-complexes. The bare diatomic cations mediate dehydrogenative C–N-bond coupling of methane and ammonia in gas-phase experiments. Another direction constitutes the investigation of ligand-exchange processes. In the second funding period, the focus is on investigations of metal-oxo complexes. This direction is inspired by the rich gas-phase chemistry of diatomic transition-metal oxo cations. In the framework of our gas-phase mimetic approach, we want to generate appropriately coordinated systems both mass-spectrometrically and in solution. We will study the reactivity of these systems as a function of the coordination environment.

• DFG Programme: Research Grants