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Reduction of transition-metal columbite-tantalite as a highly efficient electrocatalyst for water splitting

Bacirhonde, Patrick M., Dzade, Nelson Y., Chalony, Carmen, Park, Jeesoo, Jeong, Eun-Suk, Afranie, Emmanuel O., Lee, Sunny, Kim, Cheol Sang, Kim, Do-Hwan and Park, Chan Hee 2022. Reduction of transition-metal columbite-tantalite as a highly efficient electrocatalyst for water splitting. ACS Applied Materials and Interfaces 14 (13) , 15090–15102. 10.1021/acsami.1c21742

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Abstract

We successfully report a liquid–liquid chemical reduction and hydrothermal synthesis of a highly stable columbite-tantalite electrocatalyst with remarkable hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance in acidic media. The reduced Fe0.79Mn0.21Nb0.16Ta0.84O6 (CTr) electrocatalyst shows a low overpotential of 84.23 mV at 10 mA cm–2 and 103.7 achieved at 20 mA cm–2 current density in situ for the HER and OER, respectively. The electrocatalyst also exhibited low Tafel slopes of 104.97 mV/dec for the HER and 57.67 mV/dec for the OER, verifying their rapid catalytic kinetics. The electrolyzer maintained a cell voltage of 1.5 V and potential–time stability close to that of Pt/C and RuO2. Complementary first-principles density functional theory calculations identify the Mn sites as most active sites on the Fe0.75Mn0.25Ta1.875Nb0.125O6 (100) surface, predicting a moderate Gibbs free energy of hydrogen adsorption (ΔGH* ≈ 0.08 eV) and a low overpotential of η = 0.47 V. The |ΔGMnH*| = 0.08 eV on the Fe0.75Mn0.25Ta1.875Nb0.125O6 (100) surface is similar to that of the well-known and highly efficient Pt catalyst (|ΔGPtH*| ≈ 0.09 eV).

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Publisher: American Chemical Society
ISSN: 1944-8244
Date of Acceptance: 15 March 2022
Last Modified: 09 May 2022 10:30
URI: https://orca.cardiff.ac.uk/id/eprint/149500

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