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• W1771197839 abstract "Electrical double layer (edl) structure at metal and micro-meso-porous (MMP) carbon electrodes is a key factor determining the power and energy densities of edl capacitors (EDLC), hybrid capacitors (HC), Li-ion and Na-ion capacitors. Due to the economic and ecological reasons the new electrolytes based on Li-free salts and acetonitrile-free solvents, being less expensive and less harmful and based on the more widely distributed elements in nature, are required. The tetraethylammonium and Na ions based salts in aqueous and mixed organic carbonate solutions, and room-temperature ionic liquids (RTIL) have become the focus of a growing interest due to their potential applications in various modern electrochemical energy storage devices. The study and modeling of the single crystal plane and MMP carbon electrode | electrolyte and/or RTIL interface is essential for the development of the EDLC and HC of high specific performances. However, despite of the extensive discussions, our knowledge of the MMP electrode | nonaqueous electrolyte interface is still sketchy. There are theoretical papers written by Kornyshev et al. and Ivanistsev et al. but the verification of these models needs detailed systematic analysis of experimental data, including the results measured at single crystal C(0001) and metal electrodes. In this paper, the electrochemically polished Bi(hkl), cut C(0001) and MMP carbon electrodes in different aqueous and non-aqueous electrolytes and RTIL (containing the same 1-ethyl-3-methylimidazolium cation (EMIm) but various anions: tetrafluoroborate (BF4), tetracyanoborate (TCB), thiocyanate (SCN), and trispentafluoroethyl-trifluorophosphate (FAP)) have been investigated by cyclic voltammetry, chronoamperometry, and impedance spectroscopy. Ex situ STM/AFM, XRD, BET, XPS, FIB-TOF-SIMS and FIBSEM methods have been applied for structural and chemical analysis of the electrodes under study. Experiments have been carried out inside the glove box (H2O and O2 concentrations lower than 0.1 ppm) at 23°C and from 20 to 100°C in the case of Bi(111) and MMP carbon electrode, respectively. DFD calculations have been performed for analysis of the interfacial structure. The cyclic voltammetry, chronocoulometry, and impedance data for the systems studied show that there are no quick faradic processes in the wide electrode potential E region and only at highly negative potentials the exponential increase of cathodic current density has been observed, caused by electroreduction of the complex anions or residual water or O2 at the electrodes. Differently from FAP, BF4, ClO4 and PF6 the specific adsorption of TCB with the partial charge transfer takes place at E > -0.2 V (vs. Ag|AgCl in same RTIL), as at high potential scan rate v ≥ 100 mVs only the very wide and small additional current peaks in j,E-curves have been observed, connected with the specific adsorption of anion with partial charge transfer process. For more detailed analysis, the edl structure of salt + non-aqueous solvent and the RTIL+non-aqueous solvent systems with different salt concentrations has been investigated. The new model developed for diffuse layer by Fawcett et al. has been tested and deviations of our systems from the model under discussion has been explained by the weak specific adsorption of the anions from the electrolyte solution at the surface of the electrodes investigated. Fitting of the calculated impedance spectra to the experimental ones demonstrates that the good concordance can be achieved by the modified equivalent circuit that takes into account both the adsorption and diffusion limitations, and where the Warburg semi-infinite diffusion impedance has been replaced by the finitelength diffusion impedance for open circuit boundary conditions. The high-frequency (i.e. so-called double layer) capacitance, Cdl, depends weakly on the chemical composition of the electrolyte salt and RTIL studied, increasing slightly from FAP to TCB. The lowfrequency (i.e. adsorption) capacitance, Cad, has noticeably higher values than Cdl, and Cad increases in the following order of anions: FAP < BF4 < ClO4 < PF6 < SCN < TCB. A maximum in the Cad vs. potential curves has been observed at potentials more positive than the zero charge potential and Cad strongly depends on the composition of the electrolyte anions and cations. Influence of the chemical nature of the solvent and also anions and cations of a salt and ionic liquid on the power and energy densities of the single cell of EDLC has been demonstrated and analysed. The applicability limits of new Kornyshev et al. model for diffuse layer have been tested inside the so called linear edl region under discussion. Theoretical capacitance vs. electrode potential curves have been calculated, using various theoretical models developed by Kornyshev and co-workers, and compared with the experimental ones. Noticeable influence of the potential drop across the surface layer of the bismuth and MMP carbon electrodes, and dependence of the closest approach of anions to the electrode surface on the edl thickness have been demonstrated in the case of Bi, but especially of MMP carbon electrodes. Systematic analysis of the data shows that the potential drop in thin surface layer of the solid electrode determines the deviation of Bi(hkl) data from that obtained for MMP carbon electrode." @default.
• W1771197839 created "2016-06-24" @default.
• W1771197839 date "2012-01-01" @default.
• W1771197839 modified "2023-09-26" @default.
• W1771197839 title "Influence of Chemical Composition of the Electrolyte and Room-Temperature Ionic Liquids on the Electrical Double Layer Structure and Supercapacitor Characteristics" @default.
• W1771197839 doi "https://doi.org/10.1149/ma2012-02/5/386" @default.
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