Role of Dissolution Intermediates in Promoting Oxygen Evolution Reaction at RuO2(110) Surface
Abstract
RuO2 is one of the most active electrocatalysts toward oxygen evolution reaction (OER), but it suffers from rapid dissolution in electrochemical environments. It is also established experimentally that corrosion of metal oxides can, in fact, promote catalytic activity for OER owing to the formation of a surface hydrous amorphous layer. Furthermore, the mechanistic interplay between corrosion and OER across metal-oxide catalysts and to what degree these two processes are correlated are still debated. Herein, we employ ab initio molecular dynamics-based blue moon ensemble approach in combination with OER thermodynamic analysis to reveal a clear mechanistic coupling between Ru dissolution and OER at the RuO2(110)/water interface. Specifically, we demonstrate that (i) dynamic transitions between metastable dissolution intermediates greatly affect catalytic activity toward OER, (ii) dissolution and OER processes share common intermediates with OER promoting Ru detachment from the surface, (iii) the lattice oxygen can be involved in the OER, and (iv) the coupling between different OER intermediates formed at the same Ru site of the metastable dissolution state can lower the theoretical overpotential of OER down to 0.2 eV. Collectively, our findings illustrate the critical role of highly reactive metastable dissolution intermediates in facilitating OER and underscore the need for themore »
- Authors:
-
[1];
[2]
- Univ. of Nebraska, Lincoln, NE (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Univ. of Nebraska, Lincoln, NE (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); American Chemical Society, Petroleum Research Fund
- OSTI Identifier:
- 1577508
- Grant/Contract Number:
- AC02-05CH11231; ACS PRF 58410-DNI5
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 123; Journal Issue: 36; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; science & technology; other topics; materials science; radiology; oxygen; thermodynamics; dissolution; chemical reactions
Citation Formats
Klyukin, Konstantin, Zagalskaya, Alexandra, and Alexandrov, Vitaly. Role of Dissolution Intermediates in Promoting Oxygen Evolution Reaction at RuO2(110) Surface. United States: N. p., 2019.
Web. doi:10.1021/acs.jpcc.9b03418.
Klyukin, Konstantin, Zagalskaya, Alexandra, & Alexandrov, Vitaly. Role of Dissolution Intermediates in Promoting Oxygen Evolution Reaction at RuO2(110) Surface. United States. https://doi.org/10.1021/acs.jpcc.9b03418
Klyukin, Konstantin, Zagalskaya, Alexandra, and Alexandrov, Vitaly. Fri .
"Role of Dissolution Intermediates in Promoting Oxygen Evolution Reaction at RuO2(110) Surface". United States. https://doi.org/10.1021/acs.jpcc.9b03418. https://www.osti.gov/servlets/purl/1577508.
@article{osti_1577508,
title = {Role of Dissolution Intermediates in Promoting Oxygen Evolution Reaction at RuO2(110) Surface},
author = {Klyukin, Konstantin and Zagalskaya, Alexandra and Alexandrov, Vitaly},
abstractNote = {RuO2 is one of the most active electrocatalysts toward oxygen evolution reaction (OER), but it suffers from rapid dissolution in electrochemical environments. It is also established experimentally that corrosion of metal oxides can, in fact, promote catalytic activity for OER owing to the formation of a surface hydrous amorphous layer. Furthermore, the mechanistic interplay between corrosion and OER across metal-oxide catalysts and to what degree these two processes are correlated are still debated. Herein, we employ ab initio molecular dynamics-based blue moon ensemble approach in combination with OER thermodynamic analysis to reveal a clear mechanistic coupling between Ru dissolution and OER at the RuO2(110)/water interface. Specifically, we demonstrate that (i) dynamic transitions between metastable dissolution intermediates greatly affect catalytic activity toward OER, (ii) dissolution and OER processes share common intermediates with OER promoting Ru detachment from the surface, (iii) the lattice oxygen can be involved in the OER, and (iv) the coupling between different OER intermediates formed at the same Ru site of the metastable dissolution state can lower the theoretical overpotential of OER down to 0.2 eV. Collectively, our findings illustrate the critical role of highly reactive metastable dissolution intermediates in facilitating OER and underscore the need for the incorporation of interfacial reaction dynamics to resolve apparent conflicts between theoretically predicted and experimentally measured OER overpotentials.},
doi = {10.1021/acs.jpcc.9b03418},
journal = {Journal of Physical Chemistry. C},
number = 36,
volume = 123,
place = {United States},
year = {Fri Jun 07 00:00:00 EDT 2019},
month = {Fri Jun 07 00:00:00 EDT 2019}
}
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