Charging Ultrananoporous Electrodes with Size-Asymmetric Ions Assisted by Apolar Solvent

Rochester, Christopher; Kondrat, Svyatoslav; Pruessner, Gunnar; Kornyshev, Alexei A.

doi:10.1021/acs.jpcc.5b12730

Cited by 39 publications

(80 citation statements)

References 47 publications

(112 reference statements)

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“…As the adhesion energy of impurity molecules with the electrode surface increases, the capacitance-potential curves can change from the bell shape to the two-hump camel shape, with the peak shifting toward a higher charging potential. Qualitatively the impurity effect on the charging behavior is similar to the solvent effect as studied by Rochester and coworkers [81]. Whereas the amount of impurity and solvent in the bulk is considerably different, the concentration effect can be compensated by the change in the transfer energy to yield a same charging behavior.…”

Section: Impurity or Additivesupporting

confidence: 71%

Classical Density Functional Theory Insights for Supercapacitors

Lian¹,

Liu²

2018

Supercapacitors - Theoretical and Practical Solutions

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The most urgent issue for supercapacitor is to improve their energy density so that they can better compete with batteries. To design materials and interfaces for supercapacitor with higher energy density requires a deeper understanding of the factors and contributions affecting the total capacitance. In our recent works, the classical density functional theory (CDFT) was developed and applied to study the electrode/electrolyte interface behaviors, to understand capacitive energy storage. For porous electrode materials, we studied the pore size effect, curvature effect, and the surface modification of porous materials on the capacitance. Thought CDFT, we have found that the curvature effects on convex and concave EDLs are drastically different and that materials with extensive convex surfaces will lead to maximized capacitance; CDFT also predicts oscillatory variation of capacitance with pore size, but the oscillatory behavior is magnified as the curvature increases; an increase in the ionophobicity of the nanopores leads to a higher capacity for energy storage, and a pore-like impurity can enter the pore, makes the pore ionophobic and storage more energy. We also find the mixture effect, which makes more counterions pack on and more co-ions leave from the electrode surface, leads to an increase of the counterion density within the EDL and thus alargercapacitance.

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Section: Impurity or Additivesupporting

confidence: 71%

Classical Density Functional Theory Insights for Supercapacitors

Lian¹,

Liu²

2018

Supercapacitors - Theoretical and Practical Solutions

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“…Such quasi-1D systems have been studied by mapping them on the corresponding models of statistical mechanics [23][24][25][26][27][28][29][30][31]. The simplest appropriate model is a classical two-state anti-ferromagnetic Ising model with nearest neighbor interactions in external field [28].…”

Section: Introductionmentioning

confidence: 99%

Superionic liquids in conducting nanoslits: A variety of phase transitions and ensuing charging behavior

Dudka

Kondrat

Bénichou

et al. 2019

The Journal of Chemical Physics

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South Kensington Campus, London SW7 2AZ, United Kingdom ‡ 7 Interdisciplinary Scientific Center J-V Poncelet, UMI CNRS 2615, 11 Bol. Vlassievsky per., Moscow, Russia §We develop a theory of charge storage in ultra-narrow slit-like pores of nanostructured electrodes. Our analysis is based on the Blume-Capel model in external field, which we solve analytically on a Bethe lattice. The obtained solutions allow us to explore the complete phase diagram of confined ionic liquids in terms of the key parameters characterising the system, such as pore ionophilicity, interionic interaction energy and voltage. The phase diagram includes the lines of first and second-order, direct and re-entrant, phase transitions, which are manifested by singularities in the corresponding capacitance-voltage plots. To test our predictions experimentally requires mono-disperse, conducting, ultra-narrow slit pores, permitting only one layer of ions, and thick pore walls, preventing interionic interactions across the pore walls. However, some qualitative features, which distinguish the behavior of ionophilic and arXiv:1909.13089v1 [cond-mat.soft] 28 Sep 2019 ionophobic pores, and its underlying physics, may emerge in future experimental studies of more complex electrode structures.

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“…There is an escalating interest in understanding capacitive phenomena in narrowly confined ionic systems [1][2][3][4]. Obviously, the topic is of foremost fundamental importance in electrochemistry.…”

Section: Introductionmentioning

confidence: 99%

Impedance Resonance in Narrow Confinement

2018

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The article explores the ion flux response of a capacitor configuration to an alternating voltage. The model system comprises a symmetric binary electrolyte confined between plan-parallel capacitor plates. The AC response is investigated for the sparsely studied albeit practically important case of a large amplitude voltage applied across a narrow device, with the distance between the two plates amounting to a few ion diameters. Dynamic density functional theory is employed to solve for the spatiotemporal ion density distribution as well as the transient ion flux and complex impedance of the system. The analysis of these properties reveals a hitherto hidden impedance resonance. A single ion analogue of the capacitor, which is equivalent to neglecting all interactions between the ions, is employed for a physical interpretation of this phenomenon. It explains the resonance as a consequence of field-induced ion condensation at the capacitor plates and coherent motion of condensed ions in response to the field variation.

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Charging Ultrananoporous Electrodes with Size-Asymmetric Ions Assisted by Apolar Solvent

Cited by 39 publications

References 47 publications

Classical Density Functional Theory Insights for Supercapacitors

Classical Density Functional Theory Insights for Supercapacitors

Superionic liquids in conducting nanoslits: A variety of phase transitions and ensuing charging behavior

Impedance Resonance in Narrow Confinement

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