Capacitive deionization (CDI) is an emerging technology for the energy-efficient removal of dissolved ions from aqueous solutions. Expanding this technology to non-aqueous media, we present an experimental characterization of a pair of porous carbon electrodes towards electrosorption of dissolved ions in propylene carbonate. We demonstrate that application of CDI technology for treatment of an organic solution with an electrochemical stability window beyond 1.2 V allows for a higher salt removal capacity and higher charge efficiency as compared to CDI applied for treatment of aqueous electrolytes. Further, we show that using conductivity measurements of the stream emerging from the CDI cell combined with an equilibrium electric double-layer structure model, we can gain insights into charge compensation mechanisms and ion distribution in carbon nanopores.Electrosorption is a process whereby ionic electrolyte species are electrostatically conned near to charged solid-liquid interfaces, enabling fast energy storage and recovery via electric double-layer capacitors (or supercapacitors)1 and water desalination via capacitive deionization (CDI).2 In such applications, a pair of porous carbon electrodes (or stacks thereof) is charged, and ions are electrosorbed onto the pore surfaces, residing in electric double-layers (EDLs). One important difference between supercapacitors and CDI is the operation at very different ionic strength: CDI is employed at low concentrations, typically in the range of 100 mM or lower, while supercapacitors operate at 1 M or higher (depending on the electrolyte system).3 Also, while the eld of CDI has been focused almost entirely on the study and application of water desalination (ion removal from aqueous electrolytes), 4 supercapacitors can store energy with aqueous electrolytes, organic electrolytes, and solvent-free systems based on ionic liquids.While it is well known that CDI can separate a feed water stream into potable water and a separate brine stream, recently, CDI has been investigated as a promising tool for other separations in aqueous solutions, including between ionic species with different valencies, 5 and in separations for microuidic sample purication.6 A key property of CDI is the potential for energy efficient separation when using relatively dilute electrolyte solutions (i.e., where the molecules of water outnumber by roughly three or more orders of magnitude the number of ions). 7 Despite CDI's many benets, a fundamental limitation to the usable cell voltage range is the narrow electrochemical stability window of water.4 As a consequence, the maximum voltage in typical CDI systems does not exceed 1.2 to 1.4 V.4,8 At electric potentials above this level, water decomposition occurs at the electrodes via water electrolysis, which acts as a parasitic energy loss and a source of unwanted gas generation. Thus, the maximum NaCl adsorption capacity for CDI systems based on capacitive electrodes remains limited to roughly 20 mg NaCl g carbon À1 , when normalized by the mass ...