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

作者：Guang Feng, Fanghua Ning, Yue Pan, Tao Chen, Song Jin, Yucheng Wang, Ruqiang Zou, Dong Su, Dingguo Xia · 发表于：Journal of the American Chemical Society · 年份：2023 · 被引用次数：169 · 研究领域：Electrocatalysts for Energy Conversion、Fuel Cells and Related Materials、High Entropy Alloys Studies

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 H 2 /O 2 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 mg noble 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. Th...