Speaker
Description
Metal clusters in the gas phase exhibit unique properties, such as size dependent reactivities. Those can be studied with mass spectrometry and laser spectroscopy. Along with direct comparison with quantum chemical calculation modelling, metal clusters excellent model systems for investigating chemical reactions and catalytic processes taking place at low-coordinated sites. Previous studies have demonstrated the novelty of reaction model systems. For example, the reactivities of CaMn3O4+ and CaMn4O5+ towards water molecules have been explored as the reaction models for oxygen-evolving complex in photosystem II.1, 2 To gain a comprehensive understanding of reaction mechanisms at the molecular level, it is essential to understand not only the role of active centers but also of the support. Carbonaceous-support metals are of interest in catalysis, hydrogen storage, and related fields. To establish reaction models for such systems, fullerene, serving as gas phase model systems for sp2-bound carbon materials, can be used. The reactivities of metal-fullerene complexes toward small molecules such as H2, H2O, CO2, were systematically investigated.3, 4 These studies have revealed that C60 can promote reaction processes such as water splitting and CO2 reduction. Furthermore, infrared multiple photon dissociation (IRMPD) spectroscopy was employed to examine the vibrational spectra of these complexes. The structures of fullerene-metal complexes and binding motifs of the adsorbates can be identified. Possible reaction pathways were elucidated through theoretical calculations, offering atomic-level insights into the reaction mechanisms.3–6
References
[1] S. Mauthe et al. Angew. Chem. Int. Ed. 131, 8592–8597 (2019).
[2] Y. Zhang et al. Chem. Commun., 55, 14327–14330 (2019).
[3] J. Vanbuel et al. ChemPhysChem 21, 1012–1018 (2020).
[4] G. Hou et al. Angew. Chem. Int. Ed. 60, 27095–27101 (2021).
[5] E. German et al. Carbon 197, 535–543 (2022).
[6] J. Xu et al. J. Am. Chem. Soc. 145, 22243−22251 (2023).
