Novel Mn-/Co-N x Moieties Captured in N-Doped Carbon Nanotubes for Enhanced Oxygen Reduction Activity and Stability in Acidic and Alkaline Media

Abstract

Fe-N-C-based electrocatalysts have been developed as an encouraging substitute compared to their expensive Pt-containing equivalents for the oxygen reduction reaction (ORR). However, they still face major durability challenges from the in- situ production of Fenton radicals. Therefore, the synthesis of Fe-free ORR catalysts is among the emerging concerns. Herein, we have precisely applied a multistep heating strategy to produce mesoporous N-doped carbon nanostructures with Mn-/Co-Nx dual moieties from mixed-metal zeolitic imidazolate frameworks (ZIFs). It is found that their unique structure, with dual-metallic active sites, not only offers a high electrochemical performance for the ORR (E1/2 = 0.83 V vs reversible hydrogen electrode (RHE) in acid media), but also enhances the operational durability of the catalyst after 20 000 cycles with 97% of retention and very low H2O2 production (<5%) in 0.1 M HClO4. In addition, the catalyst performs well toward the ORR also in alkaline solution (exhibiting E1/2 = 0.90 V and 30 000 cyclic stability). © 2021 American Chemical Society.