Design and Preparation of Fe-N5 Catalytic Sites in Single-Atom Catalysts for Enhancing the Oxygen Reduction Reaction in Fuel Cells
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The strain effect of high-entropy intermetallic (HEI) catalysts on oxygen reduction reaction (ORR) performance remains largely unexplored, primarily due to the significant challenges associated with characterizing and calculating the intricate local coordination environments. Here, we design a nitrogen (N)-doped L1 0 -ordered PtCoNiFeCu intermetallic catalyst supported on Ketjenblack carbon (N-HEI/KB), and reveal the origin of the sub-angstrom strain in N-HEI and its impact on ORR performance by combining atomic-scale characterization and theoretical calculations. The synergistic interplay of the sub-angstrom strain, the pinning effect of metal-N bonds, and the high-entropy effect contribute to the competitive stability of N-HEI/KB catalysts, providing high current density of 1388 mA cm -2 at 0.7 V after 90,000 cycles even under harsh heavy-duty vehicle conditions. These findings broaden the avenues for designing high-performance high-entropy intermetallic cathode electrocatalysts.
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Proper kinetic and thermodynamic models are important in addressing durability as a major issue facing PGM-free ORR electrocatalysts.
In this report, we demonstrate how a uniform angstrom-level oxide overcoat (0.7–1.5 Å) by atomic layer deposition is highly effective not only in enhancing the thermal stability of underlying infiltrated ceria nanoparticles but also in facilitating electrode kinetics.
Fluoroalkyl phosphonic acids are demonstrated to be an efficient radical scavenger for Nafion™, showing a 58% lower fluoride emission rate than the state of the art, cerium.