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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sg-ntu-dr.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. |
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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 |
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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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School of Materials Science and Engineering |
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School of Materials Science and Engineering Wang, Yong Gong, Na Liu, Hongfei Ma, Wei Hippalgaonkar, Kedar Liu, Zheng Huang, Yizhong |
format |
Article |
author |
Wang, Yong Gong, Na Liu, Hongfei Ma, Wei Hippalgaonkar, Kedar Liu, Zheng Huang, Yizhong |
author_sort |
Wang, Yong |
title |
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_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_sort |
ordering-dependent hydrogen evolution and oxygen reduction electrocatalysis of high-entropy intermetallic pt₄ fecocuni |
publishDate |
2023 |
url |
https://hdl.handle.net/10356/170062 |
_version_ |
1779156711289913344 |