Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation
Fe oxides and (oxy)hydroxides are promising cost-effective catalysts for scalable water electrolysis. For an improvement in the understanding of the structural factors required by the most active Fe sites, the role of geometric tilting in determining the activity of the FeO6 octahedron for water oxi...
| Main Authors: | , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2020
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| Online Access: | https://hdl.handle.net/10356/144859 |
| _version_ | 1811693085789257728 |
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| author | Li, Haiyan Chen, Yubo Xi, Shibo Wang, Jingxian Sun, Shengnan Sun, Yuanmiao Du, Yonghua Xu, Zhichuan Jason |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Li, Haiyan Chen, Yubo Xi, Shibo Wang, Jingxian Sun, Shengnan Sun, Yuanmiao Du, Yonghua Xu, Zhichuan Jason |
| author_sort | Li, Haiyan |
| collection | NTU |
| description | Fe oxides and (oxy)hydroxides are promising cost-effective catalysts for scalable water electrolysis. For an improvement in the understanding of the structural factors required by the most active Fe sites, the role of geometric tilting in determining the activity of the FeO6 octahedron for water oxidation was investigated. The catalytic performance of the FeO6 octahedron in a series of crystalline structures, i.e., perovskites AFeO3, spinel ZnFe2O4, and β-FeOOH, was found to be negatively correlated with their octahedral tilting degree. This correlation was rationalized through the Fe–O covalency, which is reflected by the O 2p band center as well as the charge-transfer energy obtained from ab initio calculations. Thus, it was disclosed that FeO6 octahedral tilting alters the activity for water oxidation through changing the covalency degree of Fe–O bonds. |
| first_indexed | 2024-10-01T06:46:05Z |
| format | Journal Article |
| id | ntu-10356/144859 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:46:05Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-10356/1448592021-11-27T20:11:10Z Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation Li, Haiyan Chen, Yubo Xi, Shibo Wang, Jingxian Sun, Shengnan Sun, Yuanmiao Du, Yonghua Xu, Zhichuan Jason School of Materials Science and Engineering Interdisciplinary Graduate School (IGS) Solar Fuels Laboratory Energy Research Institute @ NTU (ERI@N) Engineering::Materials Perovskites Oxygen Vacancies Fe oxides and (oxy)hydroxides are promising cost-effective catalysts for scalable water electrolysis. For an improvement in the understanding of the structural factors required by the most active Fe sites, the role of geometric tilting in determining the activity of the FeO6 octahedron for water oxidation was investigated. The catalytic performance of the FeO6 octahedron in a series of crystalline structures, i.e., perovskites AFeO3, spinel ZnFe2O4, and β-FeOOH, was found to be negatively correlated with their octahedral tilting degree. This correlation was rationalized through the Fe–O covalency, which is reflected by the O 2p band center as well as the charge-transfer energy obtained from ab initio calculations. Thus, it was disclosed that FeO6 octahedral tilting alters the activity for water oxidation through changing the covalency degree of Fe–O bonds. Ministry of Education (MOE) National Research Foundation (NRF) Accepted version This work was supported by the Singapore Ministry of Education Tier 2 Grant (MOE2017-T2-1-009), Tier 1 Grant (RG3/17(S)), and the Singapore National Research Foundation under its Campus for Research Excellence and Technological Enterprise (CREATE) programme. 2020-11-30T08:53:07Z 2020-11-30T08:53:07Z 2018 Journal Article Li, H., Chen, Y., Xi, S., Wang, J., Sun, S., Sun, Y., Du, Y. & Xu, Z. J. (2018). Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation. Chemistry of Materials, 30(13), 4313-4320. https://dx.doi.org/10.1021/acs.chemmater.8b01321 0897-4756 https://hdl.handle.net/10356/144859 10.1021/acs.chemmater.8b01321 13 30 4313 4320 en MOE2017-T2-1-009 RG3/17(S) Chemistry of Materials This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.chemmater.8b01321. application/pdf |
| spellingShingle | Engineering::Materials Perovskites Oxygen Vacancies Li, Haiyan Chen, Yubo Xi, Shibo Wang, Jingxian Sun, Shengnan Sun, Yuanmiao Du, Yonghua Xu, Zhichuan Jason Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation |
| title | Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation |
| title_full | Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation |
| title_fullStr | Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation |
| title_full_unstemmed | Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation |
| title_short | Degree of geometric tilting determines the activity of FeO₆ octahedra for water oxidation |
| title_sort | degree of geometric tilting determines the activity of feo₆ octahedra for water oxidation |
| topic | Engineering::Materials Perovskites Oxygen Vacancies |
| url | https://hdl.handle.net/10356/144859 |
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