PNNL

Abstract

In situ time-of-flight secondary ion mass spectrometry (ToF-SIMS) coupled with a vacuum compatible microfluidic reactor, System for Analysis at Liquid Vacuum Interface (SALVI), has enabled the first spatial mapping of the switchable ionic liquids (SWILs) derived from 1,8-diazabicycloundec-7-ene (DBU) and 1-hexanol. As predicted by molecular dynamic simulations, our molecular imaging results confirmed a dynamic heterogeneous molecular structure with ionic regions (high CO2 concentration) coexisting with non-ionic regions (no CO2) where stoichiometry would indicate otherwise. Chemical speciation was also found to be more complex than initially thought, with spectral principal component analysis identifying dimers that ultimately highlight a highly complex molecular structure unique to SWILs. The spatial chemical mapping enabled by ToF-SIMS and SALVI advances the understanding of how the heterogeneous molecular structure impacts the dynamic physical and thermodynamic properties or SWILs.