Ionic liquid-modified porous materials for gas separation and heterogeneous catalysis

This work examines important physicochemical and thermophysical properties of ultrathin ionic liquid (IL) layers under confinement into the pore structure of siliceous supports and brings significant advances toward understanding the effects of these properties on the gas separation and catalytic performance of the developed supported ionic liquid phase (SILP) and solid catalysts with ionic liquid layers (SCILL). SILPs were developed by making use of functionalized and nonfunctionalized ILs, such as 1-(silylpropyl)-3-methyl-imidazolium hexafluorophosphate and 1-butyl-3-methyl-imidazolium hexafluorophosphate ILs, whereas the SCILL was prepared by effectively dispersing gold nanoparticles (AuNPs) onto the IL layers inside the open pores of the SILP. The information derived from the gas absorption/diffusivity and heterogeneous catalysis experiments was exemplified in relation to the liquid crystalline ordering and orientation of the IL molecules, investigated by X-ray diffraction (XRD) and modulated differential scanning calorimetry (MDSC). The extent of pore blocking was elucidated with small angle neutron scattering (SANS) and was proven to be a decisive factor for the gas separation efficiency of the SILPs. CO ₂/CO separation values above 50 were obtained in cases where liquid crystalline ordering of the IL layers and extended pore blocking had occurred. The presence of the IL layer in the developed SCILL assisted the formation of ultrasmall (2-3 nm) and well-stabilized AuNPs. The low-temperature CO oxidation efficiency was 22%. The catalytic experiments showed an additional functionality of the IL, acting as an "in-situ trap" that abstracts the product (CO ₂) from the reaction site and improves yield.