We
report a rapid solution-phase strategy to synthesize alloyed
PtNi nanoparticles which demonstrate outstanding functionality for
the oxygen reduction reaction (ORR). This one-pot coreduction colloidal
synthesis results in a monodisperse population of single-crystal nanoparticles
of rhombic dodecahedral morphology with Pt-enriched edges and compositions
close to Pt
1
Ni
2
. We use nanoscale 3D compositional
analysis to reveal for the first time that oleylamine (OAm)-aging
of the rhombic dodecahedral Pt
1
Ni
2
particles
results in Ni leaching from surface facets, producing aged particles
with concave faceting, an exceptionally high surface area, and a composition
of Pt
2
Ni
1
. We show that the modified atomic
nanostructures catalytically outperform the original PtNi rhombic
dodecahedral particles by more than two-fold and also yield improved
cycling durability. Their functionality for the ORR far exceeds commercially
available Pt/C nanoparticle electrocatalysts, both in terms of mass-specific
activities (up to a 25-fold increase) and intrinsic area-specific
activities (up to a 27-fold increase).
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