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Oxygen evolution reaction: Bifunctional mechanism breaking the linear scaling relationship

Patrick Gono1*, Alfredo Pasquarello1*

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

* Corresponding authors emails: patrick.gono@epfl.ch, alfredo.pasquarello@epfl.ch
DOI10.24435/materialscloud:2020.0038/v1 [version v1]

Publication date: Apr 18, 2020

How to cite this record

Patrick Gono, Alfredo Pasquarello, Oxygen evolution reaction: Bifunctional mechanism breaking the linear scaling relationship, Materials Cloud Archive 2020.0038/v1 (2020), doi: 10.24435/materialscloud:2020.0038/v1.

Description

The bifunctional mechanism for the oxygen evolution reaction (OER) involving two distinct reaction sites is studied through the computational hydrogen electrode method for a set of catalyst materials including rutile TiO2(110), anatase TiO2(101), SnO2(110), RuO2(110), IrO2(110), Ni2P(0001), and BiVO4(001). The calculations are performed both at the semilocal level and at the hybrid functional level. Moreover, anodic conditions are modeled and their effect on the OER free energy steps is evaluated. The free energies of the reaction steps indicate that for specific combinations of catalysts, the limitations due to the linear scaling relationship can be overcome, leading to smaller overpotentials for the overall OER. At the same time, a detailed analysis of the results reveals a strong dependence on the adopted functional. For both functionals, it is shown that the energy level of the highest occupied electronic state can serve as a descriptor to guide the search for the optimal catalyst acting as a hydrogen acceptor. These results support the bifunctional mechanism as a means to break the linear scaling relationship and to further reduce the overpotential of the OER.

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Files

File name Size Description
Structures_Hybrids.tar.gz
MD5md5:9d5643caa8aff2afc3aa68acc00b2423
151.3 KiB Relaxed geometries (in .xyz format) for all structures obtained using hybrid functionals.
Structures_RPBE.tar.gz
MD5md5:663853bba8d00fe2b572df7e0221eb56
150.0 KiB Relaxed geometries (in .xyz format) for all structures obtained using the semilocal RPBE functional.
TiO2_PBE0.inp
MD5md5:16af8bb2c03040f30ff1e4254db63fc7
2.7 KiB Sample CP2K input file corresponding to a calculation with the hybrid PBE0 functional.
TiO2_RPBE.inp
MD5md5:01a10b6422e3e9dd27305babe526e7ef
1.9 KiB Sample CP2K input file corresponding to a calculation with the RPBE functional.
README.txt
MD5md5:26586a0b486feb364f6b4b891a1fa5b1
944 Bytes README file containing a description of all files in this record.

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Journal reference (Paper which the data is associated with)
P. Gono, A. Pasquarello, J. Chem. Phys. 152, 104712 (2020) doi:10.1063/1.5143235
Preprint (Publicly available preprint version of the relevant publication)
P. Gono, A. Pasquarello, J. Chem. Phys. 152, 104712 (2020)

Keywords

EPFL OER overpotential bifunctional oxygen evolution reaction free energy interface linear scaling MARVEL/DD3

Version history:

2020.0038/v1 (version v1) [This version] Apr 18, 2020 DOI10.24435/materialscloud:2020.0038/v1