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Research Article

High entropy spinel oxide for efficient electrochemical oxidation of ammonia

Shi He1Vasishta Somayaji1Mengdi Wang1Seung-Hoon Lee1Zhijia Geng1Siyuan Zhu1Peter Novello1Chakrapani V. Varanasi2Jie Liu1( )
Department of Chemistry, Duke University, Durham, NC 27708, USA
U.S. Army Research Office P.O. Box 12211, Research Triangle Park, NC 27709, USA
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Graphical Abstract

This work introduces a new family of earth-abundant transition metal high entropyoxide electrocatalysts forammonia oxidation reaction (AOR), thus heralding a newparadigm of catalyst design for enabling ammonia as an energy carrier.

Abstract

Ammonia has emerged as a promising energy carrier owing to its carbon neutral content and low expense in long-range transportation. Therefore, development of a specific pathway to release the energy stored in ammonia is therefore in urgent demand. Electrochemical oxidation provides a convenient and reliable route to attain efficient utilization of ammonia. Here, we report that the high entropy (Mn, Fe, Co, Ni, Cu)3O4 oxides can achieve high electrocatalytic activity for ammonia oxidation reaction (AOR) in non-aqueous solutions. The AOR onset overpotential of (Mn, Fe, Co, Ni, Cu)3O4 is 0.70 V, which is nearly 0.2 V lower than that of their most active single metal cation counterpart. The mass spectroscopy study reveals that (Mn, Fe, Co, Ni, Cu)3O4 preferentially oxidizes ammonia to environmentally friendly diatomic nitrogen with a Faradic efficiency of over 85%. The X-ray photoelectron spectroscopy (XPS) result indicates that the balancing metal d-band of Mn and Cu cations helps retain a long-lasting electrocatalytic activity. Overall, this work introduces a new family of earth-abundant transition metal high entropy oxide electrocatalysts for AOR, thus heralding a new paradigm of catalyst design for enabling ammonia as an energy carrier.

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Nano Research
Pages 4785-4791
Cite this article:
He S, Somayaji V, Wang M, et al. High entropy spinel oxide for efficient electrochemical oxidation of ammonia. Nano Research, 2022, 15(6): 4785-4791. https://doi.org/10.1007/s12274-021-3665-8
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Received: 04 April 2021
Revised: 04 June 2021
Accepted: 08 June 2021
Published: 01 July 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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