Cobalt Nanoparticles on Plasma-Controlled Nitrogen-Doped Carbon as High-Performance ORR Electrocatalyst for Primary Zn-Air Battery

Metal–air batteries and fuel cells have attracted much attention as powerful candidates for a renewable energy conversion system for the last few decades. However, the high cost and low durability of platinum-based catalysts used to enhance sluggish oxygen reduction reaction (ORR) at air electrodes prevents its wide application to industry. In this work, we applied a plasma process to synthesize cobalt nanoparticles catalysts on nitrogen-doped carbon support with controllable quaternary-N and amino-N structure. In the electrochemical test, the quaternary-N and amino-N-doped carbon (Q-A)/Co catalyst with dominant quaternary-N and amino-N showed the best onset potential (0.87 V vs. RHE) and highest limiting current density (−6.39 mA/cm2). Moreover, Q-A/Co was employed as the air catalyst of a primary zinc–air battery with comparable peak power density to a commercial 20 wt.% Pt/C catalyst with the same loading, as well as a stable galvanostatic discharge at −20 mA/cm2 for over 30,000 s. With this result, we proposed the synergetic effect of transitional metal nanoparticles with controllable nitrogen-bonding can improve the catalytic activity of the catalyst, which provides a new strategy to develop a Pt-free ORR electrocatalyst.