Abstract

The mass kinetic current density (mass JK ) of most extensively reported M-N/C catalysts (M represents non-precious metal elements such as Fe, Co, and Cu), a potential alternative to noble metal catalysts in fuel cells, is poorer than that of commercial Pt/C. Thus, deep understanding of the intrinsic roles of carbon supports may contribute to the development of M-N/C catalysts from a practical point of view. Herein, the routinely used carbon supports, i.e. carbon black (CB) and carbon nanotubes (CNT) that have different morphology and crystallinity, were investigated to uncover the factors that affected the mass JK of Fe-N/C in electrocatalytic oxygen reduction. When immobilized on CB, the ionic liquids-derived Fe-N/C exhibited an enhanced mass JK (4.45 A g-1 at 0.80 V vs. RHE) by a factor of 2.14 times, comparable to that of Pt/C (5.79 A g-1 ) and higher than most reported M-N/C catalysts to our best knowledge. In contrast, the CNT support system showed no improvement. It was revealed that a compatible interface between the Fe-N/C precursors and the carbon supports was vital to ensure in-situ growth of a uniform catalyst layer on the supports during pyrolysis. This subsequently promotes the mass JK by exposing more embedded active sites and introducing favorable slit pores for effective mass-diffusion. This work would be promising to address the long-term overlooked challenge of the low mass JK of M-N/C catalysts in replacing noble-metal catalysts for practical fuel cell applications.

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