Oxygen Molecule Activation

Non-metal-hybridized platinum-based compositionally complex alloys for efficient oxygen reduction reaction in fuel cells

Incorporating light non-metallic elements into compositionally complex alloy (CCA) electrocatalysts can potentially overcome the activity–stability trade-off challenge. However, practical realization of this potential is limited by the lack of a generic method to incorporate multiple types of non-metal into single-phase CCAs. Here we present a facile solvothermal strategy enabling the incorporation of fluorine, boron and nitrogen into the interstitial sites of Pt-based CCAs. Mechanistic investigations unravel three decisive factors for the synthesis: prior formation of Pt clusters catalysing 3d-transition-metal reduction, coordination and activation of non-metal precursors by 3d-transition-metal ions, and rational selection of non-metal-containing functional groups. This methodology yields a library of non-metal-hybridized interstitial CCAs with tuneable compositions. Notably, selected Pt-based CCAs demonstrate exceptional performance as oxygen reduction electrocatalysts for fuel cells, with outstanding activity and durability surpassing state-of-the-art benchmarks. These non-metal-hybridized interstitial CCAs offer a promising platform for tackling demanding electrocatalytic processes involving complex tandem reaction steps.