Quantifying solvation energies at solid/liquid interfaces using continuum solvation methods

Gray, Corinne; Saravanan, Karthikeyan; Wang, Guofeng; Keith, John A.

doi:10.1080/08927022.2016.1273525

Cited by 72 publications

(56 citation statements)

References 62 publications

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“…Numerous recent experimental works show that solvent and/or electrolyte effects change the activity and selectivity of electrocatalysts for important reactions such as oxygen reduction, hydrogen evolution, CO 2 reduction, and CO reduction . In addition, computational works show that solvation and/or cation coadsorption modify the adsorption energies of reaction intermediates, which may not only lead to changes in reaction pathways but also to considerable differences in the calculated activity of electrocatalysts …”

Section: Computational Detailsmentioning

confidence: 99%

Influence of Van der Waals Interactions on the Solvation Energies of Adsorbates at Pt‐Based Electrocatalysts

et al. 2019

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Solvation can significantly modify the adsorption energy of species at surfaces, thereby influencing the performance of electrocatalysts and liquid‐phase catalysts. Thus, it is important to understand adsorbate solvation at the nanoscale. Here we evaluate the effect of van der Waals (vdW) interactions described by different approaches on the solvation energy of *OH adsorbed on near‐surface alloys (NSAs) of Pt. Our results show that the studied functionals can be divided into two groups, each with rather similar average *OH solvation energies: (1) PBE and PW91; and (2) vdW functionals, RPBE, PBE‐D3 and RPBE‐D3. On average, *OH solvation energies are less negative by ∼0.14 eV in group (2) compared to (1), and the values for a given alloy can be extrapolated from one functional to another within the same group. Depending on the desired level of accuracy, these concrete observations and our tabulated values can be used to rapidly incorporate solvation into models for electrocatalysis and liquid‐phase catalysis.

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Section: Computational Detailsmentioning

confidence: 99%

Influence of Van der Waals Interactions on the Solvation Energies of Adsorbates at Pt‐Based Electrocatalysts

et al. 2019

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“…Alternatively, solvent effects can be incorporated implicitly by describing the solvent as a continuous medium with effective properties. [38,39] In a recent study by Gray et al [39] adsorption energies of H, O and OH adsorbates at a Pt(111) surface were calculated and compared under gas-phase and solvated conditions for periodic slab and surface cluster models. For the adsorption of atomic H and O at the Pt(111) surface, the solvent effect was found to incur small corrections to the calculated adsorption energies.…”

Section: Introductionmentioning

confidence: 99%

Chemisorbed Oxygen at Pt(111): a DFT Study of Structural and Electronic Surface Properties

Malek

Eikerling

2017

Electrocatalysis

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Simulations based on density functional theory are used to study the electronic and electrostatic properties of a Pt (111) surface covered by a layer of chemisorbed atomic oxygen. The impact of the oxygen surface coverage and orientationally ordered interfacial water layers is explored. The oxygen adsorption energy decreases as a function of oxygen coverage due to lateral adsorbate repulsion. The surficial dipole moment density induced by the layer of chemisorbed oxygen causes a positive shift of the work function. In simulations with interfacial water layers, ordering and orientation of water molecules strongly affect the work function. It is found that the surficial dipole moment density and charge density are roughly linearly dependent on the oxygen surface coverage. Moreover, we found that water layers exert only a small impact on the surface charging behavior of the surface.

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“…However, finite clusters can also have complicated spin states that need to be accounted for (e.g., Reference ) while periodic analogs to these systems may not have significant spin polarization. To understand the extent that continuum solvation models can and should be used in applications of surface cluster models, Gray and coworkers computationally modeled adsorbate binding energies under the presence of continuum solvation on both periodic slab and large cluster models . They modeled the Pt(111) surface with a variety of adsorbates: H*, O*, and OH* at different binding sites.…”

Section: Implicit Solvationmentioning

confidence: 99%

Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals

Basdogan

Maldonado

Keith

2019

WIREs Comput Mol Sci

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We provide a critical overview of progress and challenges in computationally modeling multistep reaction mechanisms relevant for catalysis and electrocatalysis.We first discuss how the chemical and materials space of energetically efficient catalysis can be explored with computational chemistry. Since reactions for renewable energy catalysis can involve acid-base chemistry and/or ions under aqueous conditions, we then summarize how solvation can be modeled with quantum chemistry schemes using implicit, mixed implicit/explicit, and fully explicit solvation modeling. We will discuss the insights (and limitations) of these solvation models primarily through the scope of understanding CO 2 reduction reaction mechanisms, but these will also be applicable for future work elucidating other reaction mechanisms of critical importance for human sustainability such as H 2 O oxidation and N 2 reduction. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis K E Y W O R D S cluster-continuum, CO 2 reduction, mixed implicit/explicit, phase diagrams, Pourbaix diagrams, solvation modeling

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Quantifying solvation energies at solid/liquid interfaces using continuum solvation methods

Cited by 72 publications

References 62 publications

Influence of Van der Waals Interactions on the Solvation Energies of Adsorbates at Pt‐Based Electrocatalysts

Influence of Van der Waals Interactions on the Solvation Energies of Adsorbates at Pt‐Based Electrocatalysts

Chemisorbed Oxygen at Pt(111): a DFT Study of Structural and Electronic Surface Properties

Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals

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