Abstract

Network-like metallic alloys of solid nanoparticles have been frequently reported as promising electrocatalysts for fuel cells. The three-dimensional structure of such networks is rich in pores in the form of voids between nanoparticles, which collectively expose a large surface area for catalytic activity. Herein, we present a novel solution to this problem using a precursor comprising a flocculent core-shell PtNi@Ni to produce PtNi network catalysts with nanoparticle intraporosity after carefully controlled electrochemical dealloying. Physical characterization shows a hierarchical level of nanoporosity (intrapores within nanoparticles and pores between them) evolves during the controlled electrochemical dealloying, and that a Pt-rich surface also forms after 22 cycles of Ni leaching. In ORR cycling, the PtNi networks gain 4-fold activity in both jECSA and jmass over a state of the art Pt/C electrocatalyst, and also significantly exceed previously reported PtNi networks. In ORR degradation tests, the PtNi networks also proved stable, dropping by 30.4% and 62.6% in jECSA and jmass respectively. The enhanced performance of the catalyst is evident, and we also propose that the presented synthesis procedure can be generally applied to developing other metallic networks.

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