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https://hdl.handle.net/10356/138960
Title: | Enlarged Co-O covalency in octahedral sites leading to highly efficient spinel oxides for oxygen evolution reaction | Authors: | Zhou, Ye Sun, Shengnan Song, Jiajia Xi, Shibo Chen, Bo Du, Yonghua Fisher, Adrian C. Cheng, Fangyi Wang, Xin Zhang, Hua Xu, Zhichuan Jason |
Keywords: | Engineering::Materials | Issue Date: | 2018 | Source: | Zhou, Y., Sun, S., Song, J., Xi, S., Chen, B., Du, Y., Fisher, A. C., Cheng, F., Wang, X., Zhang, H. & Xu, Z. J. (2018). Enlarged Co-O covalency in octahedral sites leading to highly efficient spinel oxides for oxygen evolution reaction. Advanced Materials, 30(32), 1802912-. https://dx.doi.org/10.1002/adma.201802912 | Journal: | Advanced Materials | Abstract: | Cobalt-containing spinel oxides are promising electrocatalysts for the oxygen evolution reaction (OER) owing to their remarkable activity and durability. However, the activity still needs further improvement and related fundamentals remain untouched. The fact that spinel oxides tend to form cation deficiencies can differentiate their electrocatalysis from other oxide materials, for example, the most studied oxygen-deficient perovskites. Here, a systematic study of spinel ZnFex Co2-x O4 oxides (x = 0-2.0) toward the OER is presented and a highly active catalyst superior to benchmark IrO2 is developed. The distinctive OER activity is found to be dominated by the metal-oxygen covalency and an enlarged CoO covalency by 10-30 at% Fe substitution is responsible for the activity enhancement. While the pH-dependent OER activity of ZnFe0.4 Co1.6 O4 (the optimal one) indicates decoupled proton-electron transfers during the OER, the involvement of lattice oxygen is not considered as a favorable route because of the downshifted O p-band center relative to Fermi level governed by the spinel's cation deficient nature. | URI: | https://hdl.handle.net/10356/138960 | ISSN: | 0935-9648 | DOI: | 10.1002/adma.201802912 | Schools: | School of Chemical and Biomedical Engineering School of Materials Science and Engineering Interdisciplinary Graduate School (IGS) |
Research Centres: | Energy Research Institute @ NTU (ERI@N) Solar Fuels Laboratory |
Rights: | This is the peer reviewed version of the following article: Zhou, Y., Sun, S., Song, J., Xi, S., Chen, B., Du, Y., Fisher, A. C., Cheng, F., Wang, X., Zhang, H. & Xu, Z. J. (2018). Enlarged Co-O covalency in octahedral sites leading to highly efficient spinel oxides for oxygen evolution reaction. Advanced Materials, 30(32), 1802912-, which has been published in final form at https://doi.org/10.1002/adma.201802912. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. | Fulltext Permission: | open | Fulltext Availability: | With Fulltext |
Appears in Collections: | ERI@N Journal Articles IGS Journal Articles MSE Journal Articles SCBE Journal Articles |
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8 Manuscript.pdf | 12.93 MB | Adobe PDF | View/Open |
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