Manipulating cation Lewis acidity to create functional ionic liquid based systems

This work focuses on designing new Lewis acidic (LA) cationic species for functional ionic‑liquid (IL) systems, with applications in intrinsically frustrated Lewis pairs (FLPs) for catalysis and in charge‑transfer (CT) materials.<br>Chapter 2 introduces a proof‑of‑concept intrinsic IL FLP formed from 2,6‑lutidine as the Lewis base (LB) and N‑methylacridinium bis(trifluoromethylsulfonyl)imide ([Me‑Ac][NTf₂]) as the LA cation.

Comprehensive physical–chemical characterisation, including phase‑diagram analysis of mixtures and their hydrogen‑activation products, establishes the fundamental behaviour of this FLP system. Chapter 3 presents neutron‑scattering studies of H/D‑isotopomeric 2,6‑lutidine/[Me‑Ac][NTf₂] mixtures to probe acid–base association and solvation structure. These measurements provide direct evidence for FLP encounter‑complex formation and offer insight into hydrogen‑activation pathways and proton/hydride transfer in IL environments.