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Ionic liquids offer unique bulk and interfacial characteristics as battery electrolytes. Our continuum approach naturally describes the electrolyte on a macroscale. An integral formulation for the molecular repulsion,which can be…

Chemical Physics · Physics 2022-11-30 Max Schammer , Arnulf Latz , Birger Horstmann

This work investigates two physics-based models that simulate the non-linear partial differential algebraic equations describing an electric double layer supercapacitor. In one model the linear dependence between electrolyte concentration…

Systems and Control · Computer Science 2014-12-09 Ross Drummond , David A. Howey , Stephen R. Duncan

We generalize linearized Gouy-Chapman-Stern theory of electric double layer for nanostructured and morphologically disordered electrodes. Equation for capacitance is obtained using linear Gouy-Chapman (GC) or Debye-$\rm{\ddot{u}}$ckel…

Materials Science · Physics 2015-06-04 Rama Kant , Birla S. Maibam

We study the electric double layer by combining the effects of ion finite size and dielectric decrement. At high surface potential, both mechanisms can cause saturation of the counter-ion concentration near a charged surface. The modified…

Soft Condensed Matter · Physics 2015-03-31 Yasuya Nakayama , David Andelman

An electric double layer capacitor (EDLC) stores energy by modulating the spatial distribution of ions in the electrolytic solution that it contains. We determine the mean-field time scales for planar EDLC relaxation to equilibrium, after a…

The work reviews on a general level various modified Poisson-Boltzmann equations and demonstrates their use on the specific system of charged particles at an interface. This system is special, first, because it exhibits the long-range…

Soft Condensed Matter · Physics 2012-11-14 Derek Frydel , Martin Oettel

A classical coulombic correlation functional in one-loop (1L) and local-density-approximation (LDA) is derived for electrolyte solutions, starting from a first-principles many-body partition function. The 1L-LDA functional captures…

Chemical Physics · Physics 2026-02-17 Nils Bruch , Tobias Binninger , Jun Huang , Michael Eikerling

Atomistic simulations of electrochemical interfaces remain challenging due to the long time scales required to adequately sample the structure of the electric double layer. The emergence of efficient, short-range machine learning…

Mean-field theories claim that the capacitance of the double-layer formed at a metal/ionic conductor interface cannot be larger than that of the Helmholtz capacitor, whose width is equal to the radius of an ion. However, in some experiments…

Soft Condensed Matter · Physics 2015-03-17 M. S. Loth , Brian Skinner , B. I. Shklovskii

We present a simulation method to study electrolyte solutions in a dielectric slab geometry using a modified 3D Ewald summation. The method is fast and easy to implement, allowing us to rapidly resum an infinite series of image charges. In…

Soft Condensed Matter · Physics 2015-08-12 Alexandre P. dos Santos , Yan Levin

Three driving forces control the energy level alignment between transition-metal oxides and organic materials: the chemical interaction between the two materials, the organic electronegativity and the possible space charge layer formed in…

Polymer electrolytes are intensely investigated for use as solid electrolytes in next generation lithium-ion and lithium-metal batteries. However, little is known about the structural and dynamical properties of polymer electrolytes close…

Soft Condensed Matter · Physics 2021-12-02 Andreas Thum , Diddo Diddens , Andreas Heuer

We report on the systematic investigation of the role of surface nanoscale roughness and morphology on the charging behaviour of nanostructured titania (TiO2) surfaces in aqueous solutions. IsoElectric Points (IEPs) of surfaces have been…

Mesoscale and Nanoscale Physics · Physics 2017-06-21 F. Borghi , V. Vyas , A. Podestà , P. Milani

Molecular dynamics simulations at a constant electric potential are an essential tool to study electrochemical processes, providing microscopic information on the structural, thermodynamic, and dynamical properties. Despite the numerous…

Constant-potential molecular dynamics (MD) simulations are indispensable for understanding the capacitance, structure, and dynamics of electrical double layers (EDLs) at the atomistic level. However, the classical constant-potential method,…

Ab initio modeling of electrochemical systems is becoming a key tool for understanding and predicting electrochemical behavior. Development and careful benchmarking of computational electrochemical methods are essential to ensure their…

Chemical Physics · Physics 2017-03-01 Ravishankar Sundararaman , Kathleen Schwarz

Electrolyte decomposition reactions on Li-ion battery electrodes contribute to the formation of solid electrolyte interphase (SEI) layers. These SEI layers are one of the known causes for the loss in battery voltage and capacity over…

Classical theory of the electric double layer is based on the fundamental assumption of a dilute solution of point ions. There are a number of situations such as high applied voltages, high concentration of electrolytes, systems with…

Fluid Dynamics · Physics 2015-06-11 Brian D. Storey , Martin Z. Bazant

Whether or not specific ion effects determine the charge storage properties of aqueous graphene and graphite-based supercapacitors remains a highly debated topic. In this work we present a multiscale quantum mechanics classical molecular…

Materials Science · Physics 2022-11-10 Joshua D. Elliott , Mara Chiricotto , Alessandro Troisi , Paola Carbone

Understanding the response of the surface of metallic solids to external electric field sources is crucial to characterize electrode-electrolyte interfaces. Continuum electrostatics offer a simple description of the induced charge density…

Chemical Physics · Physics 2021-12-14 Giovanni Pireddu , Laura Scalfi , Benjamin Rotenberg