Well-Combined Magnetically Separable Hybrid Cobalt Ferrite/Nitrogen-Doped Graphene as Efficient Catalyst with Superior Performance for Oxygen Reduction Reaction

Catalysts with low‐cost, high activity and stability toward oxygen reduction reaction (ORR) are extremely desirable, but its development still remains a great challenge. Here, a novel magnetically separable hybrid of multimetal oxide, cobalt ferrite (CoFe2O4), anchored on nitrogen‐doped reduced graphene oxide (CoFe2O4/NG) is prepared via a facile solvothermal method followed by calcination at 500 °C. The structure of CoFe2O4/NG and the interaction of both components are analyzed by several techniques. The possible formation of Co/FeN interaction in the CoFe2O4/NG catalyst is found. As a result, the well‐combination of CoFe2O4 nanoparticles with NG and its improved crystallinity lead to a synergistic and efficient catalyst with high performance to ORR through a four‐electron‐transfer process in alkaline medium. The CoFe2O4/NG exhibits particularly comparable catalytic activity as commercial Pt/C catalyst, and superior stability against methanol oxidation and CO poisoning. Meanwhile, it has been proved that both nitrogen doping and the spinel structure of CoFe2O4 can have a significant contribution to the catalytic activity by contrast experiments. Multimetal oxide hybrid demonstrates better catalysis to ORR than a single metal oxide hybrid. All results make the low‐cost and magnetically separable CoFe2O4/NG a promising alternative for costly platinum‐based ORR catalyst in fuel cells and metal‐air batteries. Multimetal oxide hybrid of cobalt ferrite with N‐doped graphene (NG) as an efficient catalyst for oxygen reduction reaction is prepared via a solvothermal method. Its electrocatalytic activity outperforms NG, CoFe2O4, CoFe2O4/graphene, Co3O4/NG, Fe3O4/NG, and unannealed CoFe2O4/NG. The hybrid also shows comparable catalytic activity as commercial Pt/C, with superior resistance to methanol and CO and long durability.