Dedicated to Professor Andre E. Merbach on the occasion of his 65th birthdayThe two known Me-and allyl-substituted 1H-imidazol-3-ium bromides 1 and 2, respectively, were converted to the corresponding BF À 4 and BPh À 4 salts 3 ± 6 (Scheme 1). Compounds 3 and 4 were liquids at ambient temperature. Reaction of 1 or 2 with [PdCl 2 ] afforded the corresponding 2 : 1 imidazolium/metal complexes 7 and 8. The latter complex, melting at 588, can be regarded as a true ionic liquid. Attempts to polymerise 7 by radical promotion (AIBN) were unsuccessful, but resulted in the centrosymmetric 2 : 1 complex 9. The allyl group of 1 could be arylated (giving rise to 10) or hydrogenated (at 100 bar H 2 pressure). The solidstate structures of compounds 5 ± 7 and 9 were solved by means of single-crystal X-ray analyses (Figs. 1 ± 4).Introduction. ± Room-temperature ionic liquids have received considerable attention as alternative solvents for a wide range of applications, in particular as reaction media for homogeneous, heterogeneous, and enzymatic catalysis [1]. Ionic liquids that incorporate functional groups are becoming more and more important, since imparting specific chemical properties to the ionic liquid could lead to highly specific roles in synthesis and catalysis unparalleled by more-generic systems. It is interesting to note that the first liquid alkene-or allyl-substituted 1 ) imidazolium salts were reported as early as 1971 [24]. However, at that time, the