4.8 Article

Engineering Structurally Ordered High-Entropy Intermetallic Nanoparticles with High-Activity Facets for Oxygen Reduction in Practical Fuel Cells


Volume 145, Issue 20, Pages 11140-11150


DOI: 10.1021/jacs.3c00868



Ask authors/readers for more resources

This study reports the superior performance of structurally ordered PtIrFeCoCu high-entropy intermetallic nanoparticles (PIFCC-HEI NPs) in oxygen reduction reaction (ORR) and fuel cell applications. The PIFCC-HEI NPs exhibit ultrahigh mass activity and durability, making them highly effective catalysts. This work not only provides a new avenue for the fabrication of high-activity facets in catalysts, but also highlights the significance of structurally ordered high-entropy intermetallic nanoparticles in energy conversion technologies.
High-entropy solid-solution alloys have generated significant interest in energy conversion technologies. However, structurally ordered high-entropy intermetallic (HEI) nanoparticles (NPs) have been rarely reported in electrocatalysis applications. Here, we demonstrate structurally ordered PtIrFeCoCu HEI (PIFCC-HEI) NPs with extremely superior performance for both oxygen reduction reaction (ORR) and H2/O2 fuel cells. The PIFCC-HEI NPs show an average diameter of 6 nm. Atomic structural characterizations including atomic-resolution energy-dispersive spectroscopy (EDS) mapping technology confirm the ordered intermetallic structure of PIFCC-HEI NPs. As an electrocatalyst for ORR, the PIFCC-HEI/C achieves an ultrahigh mass activity of 7.14 A mgnoble metals -1 at 0.85 V and extraordinary durability over 60 000 potential cycles. Moreover, the fuel cell assembled with PIFCC-HEI/C as the cathode delivers an ultrahigh peak power density of 1.73 W cm-2 at a back pressure of 1.0 bar and almost no working voltage decay after 80 h operation, certifying the top-level performance among reported fuel cells. Theoretical calculations combined with experimental results reveal that the superior performance of PIFCC-HEI/C for ORR and fuel cells is attributed to its ultrahigh-activity facets. Especially, the (001) facet affords the lowest activation barriers for the rate-limiting step, the optimal downshift of the d-band center, and more efficient regulation of electron structures for ORR. This work not only opens up a new avenue for the fabrication of high-activity facets in the catalysts but also highlights structurally ordered HEI NPs as sufficiently effective catalysts in practical fuel cells and other potential energy-related applications.


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


Primary Rating

Not enough ratings

Secondary Ratings

Scientific rigor
Rate this paper


No Data Available
No Data Available