Challenges in Modeling Electrochemical Reaction Energetics with Polarizable Continuum Models

Gauthier, Joseph A.; Ringe, Stefan; Dickens, Colin F.; Garza, Alejandro J.; Bell, Alexis T.; Head-Gordon, Martin; Nørskov, Jens K.; Chan, Karen

doi:10.1021/acscatal.8b02793

Title: Challenges in Modeling Electrochemical Reaction Energetics with Polarizable Continuum Models

Journal Article · 27 November 2018 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.8b02793 · OSTI ID:1507029

^[1]; Ringe, Stefan ^[2];

^[1]; Garza, Alejandro J. ^[3];

^[4];

^[4]; Nørskov, Jens K. ^[1];

^[5]

Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

A major challenge in the modeling of electrochemical phenomena is the accurate description of the interface between an electrolyte and a charged conductor. Polarizable continuum models (PCM) have been gaining popularity because they offer a computationally inexpensive method of modeling the electrolyte. In this Perspective, we discuss challenges from using one such model which treats the ions using a linearized Poisson–Boltzmann (LPB) distribution. From a physical perspective, this model places charge unphysically close to the surface and adsorbates, and it includes excessively steep ramping of the dielectric constant from the surface to the bulk solvent. Both of these issues can be somewhat mitigated by adjusting parameters built into the model, but in doing so, the resultant capacitance deviates from experimental values. Likewise, hybrid explicit-implicit approaches to the solvent may offer a more realistic description of hydrogen bonding and solvation to reaction intermediates, but the corresponding capacitances also deviate from experimental values. These deviations highlight the need for a careful adjustment of parameters in order to reproduce not only solvation energies but also other physical properties of solid–liquid interfaces. Continuum approaches alone also necessarily do not capture local variations in the electric field from cations at the interface, which can affect the energetics of intermediates with substantial dipoles or polarizability. Finally, since the double-layer charge can be varied continuously, LPB/PCM models provide a way to determine electrochemical barriers at constant potential. However, double-layer charging and the atomic motion associated with reaction events occur on significantly different timescales. As a result, we suggest that more detailed approaches, such as the modified Poisson–Boltzmann model and/or the addition of a Stern layer, may be able to mitigate some but not all of the challenges discussed.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 1507029

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 2 Vol. 9; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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