Imidazolium Decyl Sulfate: A Very Promising Selfmade Ionic Hydrogel

This is the Accepted Manuscript version of the article. It has been through the peer review process at the Royal Society of Chemistry and has been accepted for publication in the journal "Materials Chemistry Frontiers".[Abstract] In this paper, we show, for the first time, the synthesis, structural characterization, phase diagram and physical properties of the ionic liquid, 1-ethyl-3-methyl imidazolium decyl sulfate [EMIm][DSO4]. At 25 °C it is either a crystalline solid or a liquid depending on the thermal history as its melting point is about 33 °C and its point of solidification is about 22 °C. The interest of this new IL lies in its ability to become a rigid hydrogel when mixed with water. As observed in many ILs, the as-prepared IL is hygroscopic and it adsorbs about 14 wt% of water at usual laboratory conditions and up to 27 wt% in a 100% saturated atmosphere. Due to the H-bonds between water and the amphiphilic [DSO4] anions, a lyotropic HIliquid crystalline phase is formed in the hydrated state, which can be observed in micrographs recorded using white polarized light. The moisture adsorption is a completely reversible process; thus, the rigid-gel sample loses all adsorbed water when it is left in a dry atmosphere for a few hours, transitioning to the liquid state. Phase diagrams of the temperature-water concentration is presented and compared with that of the parent compound [EMIm] octyl sulfate, [OSO4]. X-ray diffraction revels that below 15 °C the hydrated compound crystallizes into aP2/mmonoclinic structure. The structure of the new compound was confirmed by NMR, FTIR and mass spectroscopy (MS). In addition, the temperature behavior of ionic conductivity was experimentally measured and analyzed for the pure compound and for two samples hydrated with 10 wt% and 39 wt% of water. Viscosity and density were also measuredvs.temperature for the pure sample. The as-prepared IL shows great potential for numerous practical applications.This work was financed by MINECO from the Spanish Government (Grants No. MAT2014-57943-C3-1-P, MAT2014-57943-C3-2-P, MAT2014-57943-C3-3-P and DPI2012-38841-C02-02), by the European Union (COST Action CM 1206) and by the Galician Network on Ionic Liquids, REGALIs (CN 2014/015). Research projects have been co-financed by the European Regional Development Fund (FEDER