On the key role of electrolyte–electrode van der Waals interactions in the simulation of ionic liquids-based supercapacitors

Influence of surface nanostructure-induced innermost ion structuring on capacitance of carbon/ionic liquid double layers

“…[9][10][11][12][13][14][15][16][17][18][19][20][21][22][23] The differential capacitance profiles reflect the structure and properties of the IL double layers at each applied potential. In combination with electrochemical measurements, complementary experimental techniques including atomic force microscopy (AFM), [24][25][26][27] X-ray reflectometry (XR), 28 surface force apparatus (SFA), 29,30 surface-enhanced Raman spectroscopy (SERS), 21 sum frequency generation (SFG), 31,32 and molecular dynamics (MD) simulations [33][34][35][36][37][38][39][40][41][42][43][44][45][46][47][48][49][50][51] have revealed a wealth of microscopic insight into the EDL structure and differential capacitance of ILs at the electrode interface.…”

“…Theoretical [87][88][89][90] and computational work [33][34][35][36][37][38][39][40][41][42][43][44][45][46][47][48][49][50][51] has helped predict and provide insight into the structure, ion correlation, and properties of EDLs. 54,91 We note that more recent analytical theories/models that incorporate ion-ion correlations and nonelectrostatic interactions have been shown to provide more accurate descriptions of EDLs and reproduce capacitance profiles in qualitatively better agreement with experimental capacitance data.…”

Differential Capacitance of Ionic Liquid Confined between Metallic Interfaces

“…The last two decades have seen a strong development of research in ionic liquids (IL) due to their application as the electrolyte in electrochemical capacitors, or supercapacitors. − A crucial step to advance such applications is the understanding of the structure of the electric double layer (EDL) at the electrolyte/electrode interface. , Experimentally, information on the EDL structure can be indirectly obtained by measuring the differential capacitance, namely, the capacitance as a function of the applied voltage. A few features of the differential capacitance of ILs are well established, e.g., its asymmetry as consequence of the asymmetry in the constituent ions.…”

Coordination Behavior of a Confined Ionic Liquid in Carbon Nanotubes from Molecular Dynamics Simulations

“…At the molecular level, these property changes result from liquid− electrode interactions and an imposed change in liquid−liquid interactions near the surface. 5,6 Water, 8−10 water-based electrolytes, 11−13 ionic liquids (ILs), 6,14−21 and other electrolytes 22−24 are often studied in combination with solids such as carbon materials, 2,9,15,16,22,23,25,26 transition-metal oxides, 11 metal−organic frameworks, 20,27,28 or metal surfaces. 12,29 ILs have several favorable properties as electrolyte materials, such as low volatility, a wide electrochemical window, and high thermal and chemical stability.…”

“…Liquids at surfaces and in confined spaces behave significantly differently from their bulk phase, with the resulting physical properties being highly dependent on the type of liquid and solid. − This is particularly important for energy devices where the liquid is in contact with an electrode. At the molecular level, these property changes result from liquid–electrode interactions and an imposed change in liquid–liquid interactions near the surface. , Water, − water-based electrolytes, − ionic liquids (ILs), ,− and other electrolytes − are often studied in combination with solids such as carbon materials, ,,,,,,, transition-metal oxides, metal–organic frameworks, ,, or metal surfaces. , ILs have several favorable properties as electrolyte materials, such as low volatility, a wide electrochemical window, and high thermal and chemical stability. However, the viscosities of most ILs are high at room temperature, accompanied by a slow diffusion of ions, and thus neat ILs usually have a relatively low ionic conductivity at ambient conditions .…”