Speakers
Description
One of the most important aspects of rational catalyst design is controlling the environment of active sites. In electrocatalysis, the use of organic ligands has emerged as a promising strategy to tune the activity and selectivity of the catalyst. In particular, Arduengo-type N-heterocyclic carbenes (NHCs) and the closely related N-heterocyclic olefins (NHO) have emerged as promising ligands able to strongly bind to metal atoms, in many cases with higher stability than other ligands, such as thiols. Furthermore, NHCs have been successfully used in CO2RR to increase the selectivity of the catalyst towards desired products [1].
Understanding how these organic ligands interact with the catalyst is of paramount importance to further improve catalytic functionalities and stability. To shed light on this question, we combined different surface sensitive techniques to study the adsorption configuration, molecular arrangement and charge transfer of model NHCs and NHOs on Cu(111) [2,3]. Our results highlight the importance of the anchor and N-substituent groups to create tailor-made organic layers and to tune the surface properties. In addition, with the activation of CO2 molecules for CO2RR in mind [4], novel NHC-based assemblies containing nitrile groups were investigated. We found that the thermal stability of nitrile-containing NHCs on Cu(111) is higher than on Ag(111), which can be explained by the formation of molecular networks on Cu(111).
- Cao, Z. et al. Angew.Chem.Int.Ed. 57, 4981 (2018)
- Navarro, J. J. et al. Angew.Chem.Int.Ed. 2022, 61, e202202127 (2022)
- Landwehr, F. et al. Adv.Mater.Interfaces 2024, 2400378 (2024)
- Mukhopadhyay, S. et al. Nat.Commun. 15, 3397 (2024)
