Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution
While the surface atomic structure of RuO2 has been well studied in ultra high vacuum, much less is known about the interaction between water and RuO2 in aqueous solution. In this work, in situ surface X-ray scattering measurements combined with density functional theory (DFT) were used to determine...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
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Royal Society of Chemistry (RSC)
2020
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| Online Access: | https://hdl.handle.net/1721.1/126174 |
| _version_ | 1826205494152265728 |
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| author | Rao, Reshma R. Stoerzinger, Kelsey Ann Giordano, Livia Shao-Horn, Yang |
| author2 | Massachusetts Institute of Technology. Department of Mechanical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Mechanical Engineering Rao, Reshma R. Stoerzinger, Kelsey Ann Giordano, Livia Shao-Horn, Yang |
| author_sort | Rao, Reshma R. |
| collection | MIT |
| description | While the surface atomic structure of RuO2 has been well studied in ultra high vacuum, much less is known about the interaction between water and RuO2 in aqueous solution. In this work, in situ surface X-ray scattering measurements combined with density functional theory (DFT) were used to determine the surface structural changes on single-crystal RuO2(110) as a function of potential in acidic electrolyte. The redox peaks at 0.7, 1.1 and 1.4 V vs. reversible hydrogen electrode (RHE) could be attributed to surface transitions associated with the successive deprotonation of -H2O on the coordinatively unsaturated Ru sites (CUS) and hydrogen adsorbed to the bridging oxygen sites. At potentials relevant to the oxygen evolution reaction (OER), an -OO species on the Ru CUS sites was detected, which was stabilized by a neighboring -OH group on the Ru CUS or bridge site. Combining potential-dependent surface structures with their energetics from DFT led to a new OER pathway, where the deprotonation of the -OH group used to stabilize -OO was found to be rate-limiting. |
| first_indexed | 2024-09-23T13:14:20Z |
| format | Article |
| id | mit-1721.1/126174 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T13:14:20Z |
| publishDate | 2020 |
| publisher | Royal Society of Chemistry (RSC) |
| record_format | dspace |
| spelling | mit-1721.1/1261742022-09-28T12:51:53Z Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution Rao, Reshma R. Stoerzinger, Kelsey Ann Giordano, Livia Shao-Horn, Yang Massachusetts Institute of Technology. Department of Mechanical Engineering Massachusetts Institute of Technology. Department of Materials Science and Engineering Massachusetts Institute of Technology. Research Laboratory of Electronics While the surface atomic structure of RuO2 has been well studied in ultra high vacuum, much less is known about the interaction between water and RuO2 in aqueous solution. In this work, in situ surface X-ray scattering measurements combined with density functional theory (DFT) were used to determine the surface structural changes on single-crystal RuO2(110) as a function of potential in acidic electrolyte. The redox peaks at 0.7, 1.1 and 1.4 V vs. reversible hydrogen electrode (RHE) could be attributed to surface transitions associated with the successive deprotonation of -H2O on the coordinatively unsaturated Ru sites (CUS) and hydrogen adsorbed to the bridging oxygen sites. At potentials relevant to the oxygen evolution reaction (OER), an -OO species on the Ru CUS sites was detected, which was stabilized by a neighboring -OH group on the Ru CUS or bridge site. Combining potential-dependent surface structures with their energetics from DFT led to a new OER pathway, where the deprotonation of the -OH group used to stabilize -OO was found to be rate-limiting. Skoltech-MIT Center for Electrochemical Energy (Agreement 02/MI/MIT/CP/11/07633/GEN/G/00) National Science Foundation (U.S.) (Grant ACI-1548562) 2020-07-14T14:58:26Z 2020-07-14T14:58:26Z 2017-08 2019-11-25T18:08:27Z Article http://purl.org/eprint/type/JournalArticle 1754-5706 1754-5692 https://hdl.handle.net/1721.1/126174 Rao, Reshma R. et al. “Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution.” Energy & environmental science, vol. 10, no. 12, 2017, pp. 2626-2637 © 2017 The Author(s) en 10.1039/C7EE02307C Energy & environmental science Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf Royal Society of Chemistry (RSC) other univ website |
| spellingShingle | Rao, Reshma R. Stoerzinger, Kelsey Ann Giordano, Livia Shao-Horn, Yang Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution |
| title | Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution |
| title_full | Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution |
| title_fullStr | Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution |
| title_full_unstemmed | Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution |
| title_short | Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution |
| title_sort | towards identifying the active sites on ruo 2 110 in catalyzing oxygen evolution |
| url | https://hdl.handle.net/1721.1/126174 |
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