Abstract
In recent years, researchers have focused on developing zeolite imidazolate frameworks (ZIFs) as an alternative to Pt electrocatalysts for various applications, including water splitting, lithium-air batteries, zinc-air batteries, and fuel cells. In this study, we synthesized CoCu-ZIF to be used as a precursor in the development of cathode catalysts for the oxygen reduction reaction (ORR) in fuel cells. Hydrazine played a crucial role in maintaining uniformity in the development and particle size of the ZIF-67 structures. Moreover, it facilitated the rapid formation of the ZIF-67 structures at higher temperatures. A unique pseudorhombic dodecahedral morphology was obtained at a Co/Cu molar ratio of 7:3. Among all the synthesized N-doped carbon nanostructures embedded with Co and Cu nanoparticles, CoCu@NC-750, pyrolyzed at 750 °C, showed superior ORR catalytic performance. This catalyst exhibited a notably higher half-wave potential of 0.816 V and demonstrated a clear 4-electron transfer mechanism. The overpotential of CoCu@NC-750 shifted by only 11 mV over 10,000 cyclic voltammetry cycles, whereas a 55 mV shift was observed for Pt/C. CoCu@NC-750 exhibited a ∼0.8% decrease in current density during a 12-h ORR, in contrast to the 8.3% decline shown by Pt/C. This superior catalytic activity and stability can be attributed to factors such as higher oxygen adsorption induced by the N-doped carbon layer due to the localized changes in electron density and the enhanced stability of the bimetallic core. Our findings suggest that CoCu@NC-750 is a promising alternative to Pt/C in fuel cell cathodes.