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Experimental and theoretical insights into the borohydride-based reduction-induced metal interdiffusion in Fe-Oxide@NiCo2O4 for enhanced oxygen evolution

Jo, Yongcheol, Cho, Sangeun, Seo, Jiwoo, Ahmed, Abu Talha Aqueel, Lee, Chi Ho, Seok, Jun Ho, Hou, Bo ORCID: https://orcid.org/0000-0001-9918-8223, Patil, Supriya A., Park, Youngsin, Shrestha, Nabeen K., Lee, Sang Uck, Kim, Hyungsang and Im, Hyunsik 2021. Experimental and theoretical insights into the borohydride-based reduction-induced metal interdiffusion in Fe-Oxide@NiCo2O4 for enhanced oxygen evolution. ACS Applied Materials and Interfaces 13 (45) , 53725–53735. 10.1021/acsami.1c13694

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Abstract

The oxygen evolution reaction (OER) plays a key role in determining the performance of overall water splitting, while a core technological consideration is the development of cost-effective, efficient, and durable catalysts. Here, we demonstrate a robust reduced Fe-oxide@NiCo2O4 bilayered non-precious-metal oxide composite as a highly efficient OER catalyst in an alkaline medium. A bilayered oxide composite film with an interconnected nanoflake morphology (Fe2O3@NiCo2O4) is reduced in an aqueous NaBH4 solution, which results in a mosslike Fe3O4@NiCo2O4 (reduced Fe-oxide@NiCo2O4; rFNCO) nanostructured film with an enhanced electrochemical surface area. The rFNCO film demonstrates an outstanding OER activity with an extraordinary low overpotential of 189 mV at 10 mA cm–2 (246 mV at 100 mA cm–2) and a remarkably small Tafel slope of 32 mV dec–1. The film also shows excellent durability for more than 50 h of continuous operation, even at 100 mA cm–2. Furthermore, density functional theory calculations suggest that the unintentionally in situ doped Ni during the reduction reaction possibly improves the OER performance of the rFNCO catalyst shifting d-band centers of both Fe and Ni active sites.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Physics and Astronomy
Publisher: American Chemical Society
ISSN: 1944-8244
Date of First Compliant Deposit: 20 November 2021
Date of Acceptance: 25 October 2021
Last Modified: 07 Nov 2023 04:45
URI: https://orca.cardiff.ac.uk/id/eprint/145639

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