2018
DOI: 10.1063/1.5047829
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Grand-canonical approach to density functional theory of electrocatalytic systems: Thermodynamics of solid-liquid interfaces at constant ion and electrode potentials

Abstract: Properties of solid-liquid interfaces are of immense importance for electrocatalytic and electrochemical systems but modeling such interfaces at the atomic level presents a serious challenge and approaches beyond standard methodologies are needed. An atomistic computational scheme needs treat at least part of the system quantum mechanically to describe adsorption and reactions while the entire system is in thermal equilibrium. The experimentally relevant macroscopic control variables are temperature, electrode… Show more

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Cited by 180 publications
(221 citation statements)
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“…This 322 behavior is possibly connected to the observa-323 tion that standard Poisson-Boltzmann models 324 do not necessarily enforce strict charge neutral-325 ity. 54 We therefore performed single-point cal-326 culations using the JDFTx code which imple-327 ments a truncated Coulomb scheme to fully de-328 couple periodically repeated slabs. 55 As shown 329 in Table 1, the JDFTx activation energies in-330 deed agree well with the VASPsol results ex-331 trapolated to L z = ∞.…”
Section: Methodsmentioning
confidence: 99%
“…This 322 behavior is possibly connected to the observa-323 tion that standard Poisson-Boltzmann models 324 do not necessarily enforce strict charge neutral-325 ity. 54 We therefore performed single-point cal-326 culations using the JDFTx code which imple-327 ments a truncated Coulomb scheme to fully de-328 couple periodically repeated slabs. 55 As shown 329 in Table 1, the JDFTx activation energies in-330 deed agree well with the VASPsol results ex-331 trapolated to L z = ∞.…”
Section: Methodsmentioning
confidence: 99%
“…In computational electrocatalysis adsorbate‐solvent and adsorbate‐electrolyte interactions at the interface can be evaluated implicitly (where the solvent is modelled as a continuum with certain dielectric constant), explicitly, or through combinations of the two . Furthermore, efforts have been devoted to determine the minimal number of explicit water molecules needed to stabilize a given adsorbate .…”
Section: Computational Detailsmentioning
confidence: 99%
“…Section 2.3). Therefore, furtherm odel development in ab initio electrochemistry is called for that facilitates the incorporation of the appliede lectrode potentiald irectly into the underlying calculations, such as in ar ecent contribution of Melander et al, [124] in whichagrand canonical approach was used to investigatee lectrocatalyticsystems at constant ionand electrode potentials. The application of MD simulations [125,126] is required for ap roper sampling of solventc onfigurations, which can be linked to the applied electrode potential.…”
Section: Discussionmentioning
confidence: 99%