Molecular dynamics simulations of ternary PtxPdyAuz fuel cell nanocatalyst growth

Molecular dynamics simulation of PEMFC cathodes based on ternary Pt70Pd15Au15 and Pt50Pd25Au25 nanocatalysts dispersed on carbon indicate systematic Au segregation from the particle bulk to the surface, leading to an Au layer coating the cluster surface and to the spontaneous formation of a Pt@Pd@Au core-shell structure. For Au content below 25 at%, surface PtxPdy active sites are available for efficient oxygen reduction reaction, in agreement with DFT calculations and experimental data. Simulations of direct core@shell system prepared in conditions mimicking those of plasma sputtering deposition pointed out an increase of the number of accessible PtxPdy surface active sites. Core-shell nanocatalyst morphology changes occur due to impinging Pt kinetic energy confinement and dissipation.