We report here electrochemical capacitors using an aqueous electrolyte based on the concept of "water-in-salt" with the aim to improve the energy density by increasing the voltage of the cell. A "water-in-salt" consists of a highly concentrated aqueous LiTFSI solution in which both volume and mass of LiTFSI are greater than those of water. With activated carbon supercapacitor electrodes (PICA) and 31 m "water-in-salt" electrolytes (m stands for molality), we were able to reach a cell voltage of 2.4 V whereas it is difficult to exceed 1.6 V in conventional aqueous devices because of water splitting. Moreover, it was observed that the specific capacitance of the cell is improved using "water-in-salt" electrolytes. In these conditions, an energy density of 30 Wh kg −1 was obtained which is at least three times greater than for conventional aqueous devices and in the same order of magnitude than for redox enhanced capacitors. Interestingly, fair stability, over 2000 cycles, was obtained for the 7 m electrolyte. Up to 90 sec chargingdischarging rate, this latter electrolyte offers the best compromise between voltage, power and energy densities and stability. This study demonstrates the feasibility of water-in-salt as an electrolyte for supercapacitors and points out the most suited compositions for these electrolytes.

Water-in-salts are a new family of electrolytes that may allow the development of aqueous Li-ion batteries. They have a structure which is reminiscent of the one of ionic 1 liquids, and they are characterized by a large concentration of ionic species. In this work we study their transport properties and how they evolve with concentration by using molecular dynamics simulations. We first focus on the choice of the force field. By comparing the simulated viscosities and self diffusion coefficients with experimental measurements, we select a set of parameters that reproduces well the transport properties. We then use the selected force field to study in detail the variations of the self and collective diffusivities of all the species as well as the transport number of the lithium ion. We show that correlation between ions and water play an important role over the whole concentration range. In the water-in-salt regime, the anions form a percolating network which reduces the cation-anion correlations and leads to rather large values for the transport number compared to other standard electrolytes.