Abstract
Atomically flat, single-crystal solid–liquid interfaces attract considerable interest through their electrochemical relevance and well-defined structure facilitating controlled atomistic characteri...
Highlights
Single-crystal platinum surfaces constitute attractive models for fundamental studies of electrochemical interfaces following their well-defined structure and experimental relevance as excellent electrocatalysts for reactions such as hydrogen evolution and oxidation (HER, HOR).[1]
Experimental measurements alone struggle with unambiguously elucidating key atomistic details that determine the electrochemical response of solid−liquid interfaces encouraging progress in applying methods such as X-ray absorption, sum frequency generation, and in situ Raman spectroscopies has been made.[2−4] For a complementary picture, experiments are frequently augmented with density functional theory (DFT) simulations with interpretive and, ideally, predictive power, facilitating the rational theory-driven development of electrode materials.[5]
Extensive DFTMD simulations were performed to characterize the influence of surface coverage on the dynamic adlayer−water structure and interfacial electrostatics of hydrogenated single-crystal platinum electrodes
Summary
Single-crystal platinum surfaces constitute attractive models for fundamental studies of electrochemical interfaces following their well-defined structure and experimental relevance as excellent electrocatalysts for reactions such as hydrogen evolution and oxidation (HER, HOR).[1]. Low-index platinum is one of the most thoroughly characterized electrode materials,[1] and the large body of available experimental reference data[26,27,31−35] enable careful benchmarking of the computational results in order to pinpoint the necessary level of theory for obtaining physically meaningful predictions To address this challenge, we report extensive DFTMD simulations of explicitly solvated, hydrogenated Pt(111) interfaces including the coverages 0, 1/3, 2/3, and 1 ML with particular focus on the interfacial structure, dynamics, and electrostatics. Comparing the sampled dynamic coverage vs potential data with experimental measurements and statically derived Frumkin adsorption isotherms enables a direct assessment of the accuracy of the CHE formalism, frequently employed in fast, descriptor-oriented electrocatalyst screening Regarding the latter, special emphasis is placed on the exchangecorrelation functional dependence, which is benchmarked at both generalized gradient approximation (GGA) and hybrid Hartree−Fock−DFT levels
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