Abstract
• Crystal polymorphs and multiple pathways of fluorinated ionic liquid under high pressure. • Reentrant phase behavior with the layered structures. • Hybrid layered structure of [PFBS] − intermediate and gauche c onformers. 1-Hexyl-3-methylimidazolium perfluorobutanesulfonate ([C 6 mim][PFBS]), a fluorinated ionic liquid (fIL), exhibited complicated phase behaviors under high pressure (HP). The asymmetric [PFBS] − anion possesses conformational degrees of freedom. Using X-ray diffraction, HP crystal structures were determined upon compression and decompression. 00ℓ Bragg reflections at the small scattering angle representing the layered structures appeared reentrantly. The reentrant phase behavior is described by layering of [PFBS] − ( layering I) below 3.7 GPa ( P 1 ) and the hybrid layered structure of [PFBS] − ( layering II) above 7.6 GPa. The layering II caused irreversible crystal polymorph in the pressure cycle. Below P 1 , HP-phase transition changed to reversible crystal polymorph. The complicated HP-crystal polymorphs and multiple pathways were derived from the conformation-driven molecular packing states.
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