On the Operando Structure of Ruthenium Oxides during the Oxygen Evolution Reaction in Acidic Media
Abstract
In the search for rational design strategies for oxygen evolution reaction (OER) catalysts, linking the catalyst structure to activity and stability is key. However, highly active catalysts such as IrOx and RuOx undergo structural changes under OER conditions, and hence, structure–activity–stability relationships need to take into account the operando structure of the catalyst. Under the highly anodic conditions of the oxygen evolution reaction (OER), electrocatalysts are often converted into an active form. Here, we studied this activation for amorphous and crystalline ruthenium oxide using X-ray absorption spectroscopy (XAS) and electrochemical scanning electron microscopy (EC-SEM). We tracked the evolution of surface oxygen species in ruthenium oxides while in parallel mapping the oxidation state of the Ru atoms to draw a complete picture of the oxidation events that lead to the OER active structure. Our data show that a large fraction of the OH groups in the oxide are deprotonated under OER conditions, leading to a highly oxidized active material. The oxidation is centered not only on the Ru atoms but also on the oxygen lattice. This oxygen lattice activation is particularly strong for amorphous RuOx. We propose that this property is key for the high activity and low stability observed formore »
- Authors:
-
[1];
[2];
[3];
[4];
[6];
[1]
- Leiden University (Netherlands)
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Fritz Haber Institute of the Max Planck Society, Berlin (Germany)
- National Synchrotron Radiation Research Center (NSRRC), Hsinchu (Taiwan)
- Tamkang University, Taipei (Taiwan)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1998136
- Report Number(s):
- LA-UR-23-26592
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 11; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; operando XAS; ruthenium oxide; oxygen evolution reaction; electrocatalysis; O K-edge XAS; Ru M-edge XAS; Ru L-edge XAS
Citation Formats
Deka, Nipon, Jones, Travis E., Falling, Lorenz J., Sandoval-Diaz, Luis-Ernesto, Lunkenbein, Thomas, Velasco-Velez, Juan-Jesus, Chan, Ting-Shan, Chuang, Cheng-Hao, Knop-Gericke, Axel, and Mom, Rik V. On the Operando Structure of Ruthenium Oxides during the Oxygen Evolution Reaction in Acidic Media. United States: N. p., 2023.
Web. doi:10.1021/acscatal.3c01607.
Deka, Nipon, Jones, Travis E., Falling, Lorenz J., Sandoval-Diaz, Luis-Ernesto, Lunkenbein, Thomas, Velasco-Velez, Juan-Jesus, Chan, Ting-Shan, Chuang, Cheng-Hao, Knop-Gericke, Axel, & Mom, Rik V. On the Operando Structure of Ruthenium Oxides during the Oxygen Evolution Reaction in Acidic Media. United States. https://doi.org/10.1021/acscatal.3c01607
Deka, Nipon, Jones, Travis E., Falling, Lorenz J., Sandoval-Diaz, Luis-Ernesto, Lunkenbein, Thomas, Velasco-Velez, Juan-Jesus, Chan, Ting-Shan, Chuang, Cheng-Hao, Knop-Gericke, Axel, and Mom, Rik V. Fri .
"On the Operando Structure of Ruthenium Oxides during the Oxygen Evolution Reaction in Acidic Media". United States. https://doi.org/10.1021/acscatal.3c01607. https://www.osti.gov/servlets/purl/1998136.
@article{osti_1998136,
title = {On the Operando Structure of Ruthenium Oxides during the Oxygen Evolution Reaction in Acidic Media},
author = {Deka, Nipon and Jones, Travis E. and Falling, Lorenz J. and Sandoval-Diaz, Luis-Ernesto and Lunkenbein, Thomas and Velasco-Velez, Juan-Jesus and Chan, Ting-Shan and Chuang, Cheng-Hao and Knop-Gericke, Axel and Mom, Rik V.},
abstractNote = {In the search for rational design strategies for oxygen evolution reaction (OER) catalysts, linking the catalyst structure to activity and stability is key. However, highly active catalysts such as IrOx and RuOx undergo structural changes under OER conditions, and hence, structure–activity–stability relationships need to take into account the operando structure of the catalyst. Under the highly anodic conditions of the oxygen evolution reaction (OER), electrocatalysts are often converted into an active form. Here, we studied this activation for amorphous and crystalline ruthenium oxide using X-ray absorption spectroscopy (XAS) and electrochemical scanning electron microscopy (EC-SEM). We tracked the evolution of surface oxygen species in ruthenium oxides while in parallel mapping the oxidation state of the Ru atoms to draw a complete picture of the oxidation events that lead to the OER active structure. Our data show that a large fraction of the OH groups in the oxide are deprotonated under OER conditions, leading to a highly oxidized active material. The oxidation is centered not only on the Ru atoms but also on the oxygen lattice. This oxygen lattice activation is particularly strong for amorphous RuOx. We propose that this property is key for the high activity and low stability observed for amorphous ruthenium oxide.},
doi = {10.1021/acscatal.3c01607},
journal = {ACS Catalysis},
number = 11,
volume = 13,
place = {United States},
year = {Fri May 19 00:00:00 EDT 2023},
month = {Fri May 19 00:00:00 EDT 2023}
}
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