4.8 Article

Ordering-Dependent Hydrogen Evolution and Oxygen Reduction Electrocatalysis of High-Entropy Intermetallic Pt4FeCoCuNi

Journal

ADVANCED MATERIALS
Volume 35, Issue 28, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202302067

Keywords

electrocatalysis; high-entropy intermetallics; hydrogen evolution reaction; oxygen reduction reaction; tunable crystal and electronic structures

Ask authors/readers for more resources

Disordered solid-solution high-entropy alloys have been extensively studied as robust electrocatalysts, while ordered high-entropy intermetallics remain poorly explored with unknown effects on catalytic activity. In this study, a series of multicomponent intermetallic Pt4FeCoCuNi nanoparticles with tunable ordering degrees were fabricated, and the transformation mechanism from disordered to ordered structure was revealed. The electrocatalytic performance of Pt4FeCoCuNi nanoparticles was found to be correlated with their crystal and electronic structures, with increasing ordering degree promoting catalytic performance. The highly ordered Pt4FeCoCuNi nanoparticles achieved the highest mass activities for both acidic oxygen reduction reaction (ORR) and alkaline hydrogen evolution reaction (HER), outperforming commercial Pt/C by 18.9-fold and 5.6-fold, respectively.
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 Pt4FeCoCuNi 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 Pt4FeCoCuNi 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 Pt4FeCoCuNi 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 Pt4FeCoCuNi 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.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

No Data Available
No Data Available