Patrick Gono^1*, Francesco Amborsio^1*, Alfredo Pasquarello^1*

1 Chair of Atomic Scale Simulation (CSEA), Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

* Corresponding authors emails: patrick.gono@epfl.ch, francesco.ambrosio@epfl.ch, alfredo.pasquarello@epfl.ch

DOI10.24435/materialscloud:2019.0038/v2 [version v2]

Publication date: Aug 02, 2019

How to cite this record

Patrick Gono, Francesco Amborsio, Alfredo Pasquarello, Effect of the Solvent on the Oxygen Evolution Reaction at the TiO2-Water Interface, Materials Cloud Archive 2019.0038/v2 (2019), https://doi.org/10.24435/materialscloud:2019.0038/v2

Description

We investigate the solvation effect of water on the overpotentials of the oxygen evolution reaction on rutile TiO2 by applying the thermodynamic integration method on atomistic model interfaces with and without the water molecules. We compare the results at the vacuum interface with the commonly used computational hydrogen electrode method, finding overall good agreement. The effect of the solvent is found to be twofold. First, the explicit treatment of the solvent can lead to equilibrium configurations differing from the relaxed structures without solvent. Second, the overpotentials can be affected by up to 0.5 eV. The energetics are subject to electrostatic effects at the interface rather than to modifications in the hydrogen bond network. These results provide a promising perspective for treating the solvent with implicit models.

Materials Cloud sections using this data

Files

File name	Size	Description
vacuum_.zip MD5md5:0a7f3823cb2b0767c6e3a8a7e3d5dc48	26.1 MiB	Ab-initio molecular dynamics trajectory of the clean TiO2-vacuum interface
vacuum_H2O.zip MD5md5:6f1e9b0232ab9828f948bab532847733	20.2 MiB	Ab-initio molecular dynamics trajectory of the TiO2-vacuum interface with H2O adsorbed
vacuum_H2O2.zip MD5md5:9c2742529160bf0bb67dd11249a4f781	16.0 MiB	Ab-initio molecular dynamics trajectory of the TiO2-vacuum interface with H2O2 adsorbed
solvent_O2.zip MD5md5:0eb5d9b4e0dd23c521da8b32d19f9e7b	59.7 MiB	Ab-initio molecular dynamics trajectory of the TiO2-water interface with O2 adsorbed
solvent_H2O2.zip MD5md5:166df82d0928ba415edbe344218db9a3	59.9 MiB	Ab-initio molecular dynamics trajectory of the TiO2-water interface with H2O2 adsorbed
vacuum_O2.zip MD5md5:384bd6ed058b516d48568dcd76051231	32.6 MiB	Ab-initio molecular dynamics trajectory of the TiO2-vacuum interface with O2 adsorbed
solvent_O.zip MD5md5:4d89cd874ef4375f7f5785a86da694a2	60.0 MiB	Ab-initio molecular dynamics trajectory of the TiO2-water interface with O adsorbed
CHE_structures.zip MD5md5:15321c5b3d0972ac9b12cc017e2b8e72	37.6 KiB	Relaxed structures of the vacuum interface with all relevant adsorbates used in the computational hydrogen electrode calculations
solvent_OOH.zip MD5md5:370182a7604b264946b4b0559f716d59	59.8 MiB	Ab-initio molecular dynamics trajectory of the TiO2-water interface with OOH adsorbed
H2O_OH_0.5.inp MD5md5:d262e807480669197070aaebe2d69ebc	1.6 KiB	CP2K 4.1 input file for a mixed-Hamiltonian dynamics
vacuum_O.zip MD5md5:51688e240823fb2bff3f9392567c53fc	7.7 MiB	Ab-initio molecular dynamics trajectory of the TiO2-vacuum interface with O adsorbed
input.inc MD5md5:046008bdb508d1d03a4ff6be2c4cc418	2.6 KiB	part of the CP2K 4.1 input file, to be included in the file H2O_OH_0.5.inp
solvent_H2O.zip MD5md5:c663f69e8f7c1ac52c191954a382f46e	29.0 MiB	Ab-initio molecular dynamics trajectory of the TiO2-water interface with H2O adsorbed
solvent_OH.zip MD5md5:0370af0e79dc8974c8abc260f7393398	60.1 MiB	Ab-initio molecular dynamics trajectory of the TiO2-water interface with OH adsorbed
vacuum_OOH.zip MD5md5:0568827902c4f98da5b33d02440d9062	11.0 MiB	Ab-initio molecular dynamics trajectory of the TiO2-vacuum interface with OOH adsorbed
vacuum_OH.zip MD5md5:161d07f951bcd7430c33e511b1ef15dd	25.0 MiB	Ab-initio molecular dynamics trajectory of the TiO2-vacuum interface with OH adsorbed

License

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Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Keywords

MARVEL/DD3 water explicit solvent solvation effect oxygen evolution reaction TiO2 rutile