Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation
The development of efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) is critical for improving the efficiency of water electrolysis. Here, we report a strategy using Fe substitution to enable the inactive spinel CoAl2O4 to become highly active and superior to the benchm...
| Main Authors: | , , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2021
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/153349 |
| _version_ | 1811686190569488384 |
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| author | Wu, Tianze Sun, Shengnan Song, Jiajia Xi, Shibo Du, Yonghua Chen, Bo Sasangka, Wardhana Aji Liao, Hanbin Gan, Chee Lip Scherer, Günther G. Zeng, Lin Wang, Haijiang Li, Hui Grimaud, Alexis Xu, Zhichuan Jason |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Wu, Tianze Sun, Shengnan Song, Jiajia Xi, Shibo Du, Yonghua Chen, Bo Sasangka, Wardhana Aji Liao, Hanbin Gan, Chee Lip Scherer, Günther G. Zeng, Lin Wang, Haijiang Li, Hui Grimaud, Alexis Xu, Zhichuan Jason |
| author_sort | Wu, Tianze |
| collection | NTU |
| description | The development of efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) is critical for improving the efficiency of water electrolysis. Here, we report a strategy using Fe substitution to enable the inactive spinel CoAl2O4 to become highly active and superior to the benchmark IrO2. The Fe substitution is revealed to facilitate surface reconstruction into active Co oxyhydroxides under OER conditions. It also activates deprotonation on the reconstructed oxyhydroxide to induce negatively charged oxygen as an active site, thus significantly enhancing the OER activity of CoAl2O4. Furthermore, it promotes the pre-oxidation of Co and introduces great structural flexibility due to the uplift of the oxygen 2p levels. This results in the accumulation of surface oxygen vacancies along with lattice oxygen oxidation that terminates as Al3+ leaches, preventing further reconstruction. We showcase a promising way to achieve tunable electrochemical reconstruction by optimizing the electronic structure for low-cost and robust spinel oxide OER catalysts. |
| first_indexed | 2024-10-01T04:56:29Z |
| format | Journal Article |
| id | ntu-10356/153349 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:56:29Z |
| publishDate | 2021 |
| record_format | dspace |
| spelling | ntu-10356/1533492021-12-04T20:11:09Z Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation Wu, Tianze Sun, Shengnan Song, Jiajia Xi, Shibo Du, Yonghua Chen, Bo Sasangka, Wardhana Aji Liao, Hanbin Gan, Chee Lip Scherer, Günther G. Zeng, Lin Wang, Haijiang Li, Hui Grimaud, Alexis Xu, Zhichuan Jason School of Materials Science and Engineering Interdisciplinary Graduate School (IGS) Nanyang Environment and Water Research Institute Energy Research Institute @ NTU (ERI@N) Solar Fuels Laboratory Engineering::Materials::Energy materials Electrocatalysis Energy The development of efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) is critical for improving the efficiency of water electrolysis. Here, we report a strategy using Fe substitution to enable the inactive spinel CoAl2O4 to become highly active and superior to the benchmark IrO2. The Fe substitution is revealed to facilitate surface reconstruction into active Co oxyhydroxides under OER conditions. It also activates deprotonation on the reconstructed oxyhydroxide to induce negatively charged oxygen as an active site, thus significantly enhancing the OER activity of CoAl2O4. Furthermore, it promotes the pre-oxidation of Co and introduces great structural flexibility due to the uplift of the oxygen 2p levels. This results in the accumulation of surface oxygen vacancies along with lattice oxygen oxidation that terminates as Al3+ leaches, preventing further reconstruction. We showcase a promising way to achieve tunable electrochemical reconstruction by optimizing the electronic structure for low-cost and robust spinel oxide OER catalysts. Ministry of Education (MOE) National Research Foundation (NRF) Accepted version The authors acknowledge support from the Singapore Ministry of Education Tier 2 Grant (MOE2017-T2-1-009) and the Singapore National Research Foundation under its Campus for Research Excellence and Technological Enterprise (CREATE) programme. 2021-11-25T05:51:27Z 2021-11-25T05:51:27Z 2019 Journal Article Wu, T., Sun, S., Song, J., Xi, S., Du, Y., Chen, B., Sasangka, W. A., Liao, H., Gan, C. L., Scherer, G. G., Zeng, L., Wang, H., Li, H., Grimaud, A. & Xu, Z. J. (2019). Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation. Nature Catalysis, 2(9), 763-772. https://dx.doi.org/10.1038/s41929-019-0325-4 2520-1158 https://hdl.handle.net/10356/153349 10.1038/s41929-019-0325-4 2-s2.0-85070209933 9 2 763 772 en MOE2017-T2-1-009 Nature Catalysis © 2019 The Author(s), under exclusive licence to Springer Nature Limited. This paper was published in Nature Catalysis and is made available with permission of The Author(s). application/pdf |
| spellingShingle | Engineering::Materials::Energy materials Electrocatalysis Energy Wu, Tianze Sun, Shengnan Song, Jiajia Xi, Shibo Du, Yonghua Chen, Bo Sasangka, Wardhana Aji Liao, Hanbin Gan, Chee Lip Scherer, Günther G. Zeng, Lin Wang, Haijiang Li, Hui Grimaud, Alexis Xu, Zhichuan Jason Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation |
| title | Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation |
| title_full | Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation |
| title_fullStr | Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation |
| title_full_unstemmed | Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation |
| title_short | Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation |
| title_sort | iron facilitated dynamic active site generation on spinel coal₂o₄ with self termination of surface reconstruction for water oxidation |
| topic | Engineering::Materials::Energy materials Electrocatalysis Energy |
| url | https://hdl.handle.net/10356/153349 |
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