Synergizing Amino Tethering and Carbon Shell Confinement Enables Confinement Synthesis of PtCo Intermetallic Catalysts for Highly Durable Fuel Cells

Intermetallic compounds possess superior catalytic performance over their disordered alloy counterparts, while their synthesis usually requires high-temperature treatment, which causes the sintering of catalysts. This work demonstrates the high-temperature confinement synthesis (HTCS) of PtCo intermetallic compounds for oxygen reduction reaction (ORR) by integrating ultrathin nitrogen-doped carbon shell (NCS) confined PtCo alloy into −NH 2 functionalized black pearls 2000 carbon architectures (PtCo@NCS/BP-NH 2 ). Benefiting from amino tethering and carbon shell confinement, high-temperature sintering behavior is effectively inhibited. PtCo@NCS/BP-NH 2 possesses outstanding ORR performance, and the assembled single cell exhibits a small peak power density loss rate of 4% after the accelerated durability test (ADT), outperforming PtCo/BP (12.5%) and commercial Pt/C (18.9%). Theoretical calculations along with experiments reveal that PtCo and NCS synergically optimize the electronic structure, weaken the Pt–O dipole effect, and lower the reaction barrier for ORR. The study provides insight into the HTCS of catalysts and unveils intrinsic electronic interaction for ORR.