Abstract
The large-scale and controllable synthesis of novel N-doped three-dimensional (3D) carbon nanocage-decorated carbon skeleton sponges (Co-NCMS) is introduced. These Co-NCMS were highly active and durable non-noble metal catalysts for the oxygen reduction reaction (ORR). This hybrid electrocatalyst showed high ORR activity with a diffusion-limiting current of 5.237 mA·cm-2 in 0.1 M KOH solution through the highly efficient 4e- pathway, which was superior to that of the Pt/C catalyst (4.99 mA·cm-2), and the ORR Tafel slope is ca. 67.7 mV·dec-1 at a high potential region, close to that of Pt/C. Furthermore, Co-NCMS exhibited good ORR activity in acidic media with an onset potential comparable to that of the Pt/C catalyst. Most importantly, the prepared catalyst showed much higher stability and better methanol tolerance in both alkaline and acidic solutions. The power density obtained in a proton exchange membrane fuel cell was as high as 0.37 W·cm-2 at 0.19 V compared with 0.45 W·cm-2 at 0.56 V for the Pt/C catalyst. In Co-NCMS, the N-doped carbon nanocages facilitated the diffusion of the reactant, maximizing the exposure of active sites on the surface and protecting the active metallic core from oxidation. This made Co-NCMS one of the best non-noble metal catalysts and potentially offers an alternative approach for the efficient utilization of active transition metals in electrocatalyst applications.