Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi

Disordered solid-solution high-entropy alloys have attracted wide research attention as robust electrocatalysts. In comparison, ordered high-entropy intermetallics have been hardly explored and the effects of the degree of chemical ordering on catalytic activity remain unknown. In this study, a seri...

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Main Authors: Wang, Yong, Gong, Na, Liu, Hongfei, Ma, Wei, Hippalgaonkar, Kedar, Liu, Zheng, Huang, Yizhong
Other Authors: School of Materials Science and Engineering
Format: Journal Article
Language:English
Published: 2023
Subjects:
Online Access:https://hdl.handle.net/10356/170062
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author Wang, Yong
Gong, Na
Liu, Hongfei
Ma, Wei
Hippalgaonkar, Kedar
Liu, Zheng
Huang, Yizhong
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Wang, Yong
Gong, Na
Liu, Hongfei
Ma, Wei
Hippalgaonkar, Kedar
Liu, Zheng
Huang, Yizhong
author_sort Wang, Yong
collection NTU
description Disordered solid-solution high-entropy alloys have attracted wide research attention as robust electrocatalysts. In comparison, ordered high-entropy intermetallics have been hardly explored and the effects of the degree of chemical ordering on catalytic activity remain unknown. In this study, a series of multicomponent intermetallic Pt4 FeCoCuNi nanoparticles with tunable ordering degrees is fabricated. The transformation mechanism of the multicomponent nanoparticles from disordered structure into ordered structure is revealed at the single-particle level, and it agrees with macroscopic analysis by selected-area electron diffraction and X-ray diffraction. The electrocatalytic performance of Pt4 FeCoCuNi nanoparticles correlates well with their crystal structure and electronic structure. It is found that increasing the degree of ordering promotes electrocatalytic performance. The highly ordered Pt4 FeCoCuNi achieves the highest mass activities toward both acidic oxygen reduction reaction (ORR) and alkaline hydrogen evolution reaction (HER) which are 18.9-fold and 5.6-fold higher than those of commercial Pt/C, respectively. The experiment also shows that this catalyst demonstrates better long-term stability than both partially ordered and disordered Pt4 FeCoCuNi as well as Pt/C when subject to both HER and ORR. This ordering-dependent structure-property relationship provides insight into the rational design of catalysts and stimulates the exploration of many other multicomponent intermetallic alloys.
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spelling ntu-10356/1700622023-08-23T02:03:18Z Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi Wang, Yong Gong, Na Liu, Hongfei Ma, Wei Hippalgaonkar, Kedar Liu, Zheng Huang, Yizhong School of Materials Science and Engineering Engineering::Materials Electrocatalysis High-Entropy Intermetallics Disordered solid-solution high-entropy alloys have attracted wide research attention as robust electrocatalysts. In comparison, ordered high-entropy intermetallics have been hardly explored and the effects of the degree of chemical ordering on catalytic activity remain unknown. In this study, a series of multicomponent intermetallic Pt4 FeCoCuNi nanoparticles with tunable ordering degrees is fabricated. The transformation mechanism of the multicomponent nanoparticles from disordered structure into ordered structure is revealed at the single-particle level, and it agrees with macroscopic analysis by selected-area electron diffraction and X-ray diffraction. The electrocatalytic performance of Pt4 FeCoCuNi nanoparticles correlates well with their crystal structure and electronic structure. It is found that increasing the degree of ordering promotes electrocatalytic performance. The highly ordered Pt4 FeCoCuNi achieves the highest mass activities toward both acidic oxygen reduction reaction (ORR) and alkaline hydrogen evolution reaction (HER) which are 18.9-fold and 5.6-fold higher than those of commercial Pt/C, respectively. The experiment also shows that this catalyst demonstrates better long-term stability than both partially ordered and disordered Pt4 FeCoCuNi as well as Pt/C when subject to both HER and ORR. This ordering-dependent structure-property relationship provides insight into the rational design of catalysts and stimulates the exploration of many other multicomponent intermetallic alloys. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) National Research Foundation (NRF) This work was supported by the Ministry of Education (MOE) Singapore Tier 1 FG79/20. K.H. acknowledges funding from the Accelerated Materials Development for Manufacturing Program at A*STAR via the AME Programmatic Fund by the Agency for Science, Technology, and Research under grant no.A1898b0043. K.H. also acknowledges support from the NRF FellowshipNRF-NRFF13-2021-0011. 2023-08-23T02:03:18Z 2023-08-23T02:03:18Z 2023 Journal Article Wang, Y., Gong, N., Liu, H., Ma, W., Hippalgaonkar, K., Liu, Z. & Huang, Y. (2023). Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi. Advanced Materials, 35(28), e2302067-. https://dx.doi.org/10.1002/adma.202302067 0935-9648 https://hdl.handle.net/10356/170062 10.1002/adma.202302067 37165532 2-s2.0-85159838099 28 35 e2302067 en FG79/20 A1898b0043 NRF-NRFF13-2021-0011 Advanced Materials © 2023 Wiley-VCH GmbH. All rights reserved.
spellingShingle Engineering::Materials
Electrocatalysis
High-Entropy Intermetallics
Wang, Yong
Gong, Na
Liu, Hongfei
Ma, Wei
Hippalgaonkar, Kedar
Liu, Zheng
Huang, Yizhong
Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi
title Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi
title_full Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi
title_fullStr Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi
title_full_unstemmed Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi
title_short Ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic Pt₄ FeCoCuNi
title_sort ordering dependent hydrogen evolution and oxygen reduction electrocatalysis of high entropy intermetallic pt₄ fecocuni
topic Engineering::Materials
Electrocatalysis
High-Entropy Intermetallics
url https://hdl.handle.net/10356/170062
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