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Title: Orientation-Dependent Oxygen Evolution on RuO 2 without Lattice Exchange

Abstract

RuO2 catalysts exhibit record activities towards the oxygen evolution reaction (OER), which is crucial to enable efficient and sustainable energy storage. Here we examine the RuO2 OER kinetics on rutile (110), (100), (101), and (111) orientations, finding (100) the most active. We assess the potential involvement of lattice oxygen in the OER mechanism with online 3 electrochemical mass spectrometry, which showed no evidence of oxygen exchange on these oriented facets in acidic or basic electrolytes. Similar results were obtained for polyoriented RuO2 films and particles, in contrast to previous work, suggesting lattice oxygen is not exchanged in catalyzing OER on crystalline RuO2 surfaces. This hypothesis is supported by the correlation of activity with the number of active Ru-sites calculated by DFT, where more active facets bind oxygen more weakly. This new understanding of the active sites provides a design strategy to enhance the OER activity of RuO2 nanoparticles by facet engineering.

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1364004
Report Number(s):
PNNL-SA-126477
Journal ID: ISSN 2380-8195
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Energy Letters; Journal Volume: 2; Journal Issue: 4
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Stoerzinger, Kelsey A., Diaz-Morales, Oscar, Kolb, Manuel, Rao, Reshma R., Frydendal, Rasmus, Qiao, Liang, Wang, Xiao Renshaw, Halck, Niels Bendtsen, Rossmeisl, Jan, Hansen, Heine A., Vegge, Tejs, Stephens, Ifan E. L., Koper, Marc T. M., and Shao-Horn, Yang. Orientation-Dependent Oxygen Evolution on RuO 2 without Lattice Exchange. United States: N. p., 2017. Web. doi:10.1021/acsenergylett.7b00135.
Stoerzinger, Kelsey A., Diaz-Morales, Oscar, Kolb, Manuel, Rao, Reshma R., Frydendal, Rasmus, Qiao, Liang, Wang, Xiao Renshaw, Halck, Niels Bendtsen, Rossmeisl, Jan, Hansen, Heine A., Vegge, Tejs, Stephens, Ifan E. L., Koper, Marc T. M., & Shao-Horn, Yang. Orientation-Dependent Oxygen Evolution on RuO 2 without Lattice Exchange. United States. doi:10.1021/acsenergylett.7b00135.
Stoerzinger, Kelsey A., Diaz-Morales, Oscar, Kolb, Manuel, Rao, Reshma R., Frydendal, Rasmus, Qiao, Liang, Wang, Xiao Renshaw, Halck, Niels Bendtsen, Rossmeisl, Jan, Hansen, Heine A., Vegge, Tejs, Stephens, Ifan E. L., Koper, Marc T. M., and Shao-Horn, Yang. Wed . "Orientation-Dependent Oxygen Evolution on RuO 2 without Lattice Exchange". United States. doi:10.1021/acsenergylett.7b00135.
@article{osti_1364004,
title = {Orientation-Dependent Oxygen Evolution on RuO 2 without Lattice Exchange},
author = {Stoerzinger, Kelsey A. and Diaz-Morales, Oscar and Kolb, Manuel and Rao, Reshma R. and Frydendal, Rasmus and Qiao, Liang and Wang, Xiao Renshaw and Halck, Niels Bendtsen and Rossmeisl, Jan and Hansen, Heine A. and Vegge, Tejs and Stephens, Ifan E. L. and Koper, Marc T. M. and Shao-Horn, Yang},
abstractNote = {RuO2 catalysts exhibit record activities towards the oxygen evolution reaction (OER), which is crucial to enable efficient and sustainable energy storage. Here we examine the RuO2 OER kinetics on rutile (110), (100), (101), and (111) orientations, finding (100) the most active. We assess the potential involvement of lattice oxygen in the OER mechanism with online 3 electrochemical mass spectrometry, which showed no evidence of oxygen exchange on these oriented facets in acidic or basic electrolytes. Similar results were obtained for polyoriented RuO2 films and particles, in contrast to previous work, suggesting lattice oxygen is not exchanged in catalyzing OER on crystalline RuO2 surfaces. This hypothesis is supported by the correlation of activity with the number of active Ru-sites calculated by DFT, where more active facets bind oxygen more weakly. This new understanding of the active sites provides a design strategy to enhance the OER activity of RuO2 nanoparticles by facet engineering.},
doi = {10.1021/acsenergylett.7b00135},
journal = {ACS Energy Letters},
number = 4,
volume = 2,
place = {United States},
year = {Wed Mar 15 00:00:00 EDT 2017},
month = {Wed Mar 15 00:00:00 EDT 2017}
}