Abstract
Precisely controlling the strain of Pt-based intermetallic to ensure high performance and stability is a massive task for sustainable proton-exchange-membrane-fuel-cells. Herein, the Al single-atom was trapped into the L12-Pt3Co intermetallic core to precisely tailor the strain state on the Pt-skin for fast oxygen reduction reaction kinetics. Theoretical calculations firstly predicted that only tailored tension can accelerate the protonation of O2 on L12-Pt3Co@Pt without creating an additional energy barrier for subsequent oxygen-containing intermediates desorption. Experimentally, Al single-atom confined in the L12-Pt3Co lattice by substituting partial Co occupancy, imposing tailored ∼ 0.2 % tension on Pt-skin compared to the L12-Pt3Co. L12-Al-Pt3Co@Pt/C exhibits enhanced mass activity which is ten-time improvement over commercial Pt/C. More significantly, XAS and DFT results reveal that the Al single-atom can strengthen the Pt-Co bonding, enhancing the stability of L12-Al-Pt3Co@Pt/C in oxygen reduction. This work provides an avenue to design the strain by single-atom for sustainable energy conversion technologies.
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