Just Accepted Articles have been posted online after technical editing and typesetting for immediate view. The final edited version with page numbers will appear in the Current Issue soon.
Addressing the CO-sensitive and catalytic efficiency issues of noble metal-based electrocatalysts towards alkaline hydrogen oxidation reaction (HOR) are indispensable for the practical commercialization of advanced anion exchange membrane fuel cells (AEMFCs). Here, Ni-N-C supported Ir catalysts denoted as Ir/Ni-N-C have been constructed and demonstrated greatly improved resistance towards CO impurities compared to conventional N-C or pure C anchored Ir nanoparticles after long-term CO poisoning. Besides, Ir/Ni-N-C possesses superior specific and mass activity of 0.557 mA cm-2 and 1.15 mA mgPGM-1, which is approximately 2-times higher than that of Ir/C and even outperforms the state-of-the-art commercial Pt/C catalysts. Combining in-situ surface-enhanced infrared absorption spectroscopy and density functional calculation, the band structure modulation and coordination effect of Ni-N-C supports lead to strengthened hydroxyl binding energy, promoted CO oxidative desorption under working potential, and lowered activation barrier of the rate-determining process of alkaline HOR. This work sheds light on the importance of metal-N-C substrates for solving the CO-tolerance and intrinsic activity challenges, provides new insights for noble-metal based catalysts designing.