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Title: Iron-facilitated dynamic active-site generation on spinel CoAl₂O₄ with self-termination of surface reconstruction for water oxidation
Authors: 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
Keywords: Engineering::Materials::Energy materials
Issue Date: 2019
Source: 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.
Project: MOE2017-T2-1-009 
Journal: Nature Catalysis 
Abstract: 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.
ISSN: 2520-1158
DOI: 10.1038/s41929-019-0325-4
Rights: © 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).
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:ERI@N Journal Articles
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