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We demonstrated that the oxygen reduction reaction (ORR) activity over catalysts derived from pyrolyzed cobalt zeolitic imidazolate frameworks (ZIFs) depends strongly on the imidazole ligand structure and cobalt content. The activity and durability of these catalysts were tested in the proton exchange membrane fuel cell for the first time. The membrane electrode assembly containing a catalyst derived from Co/Zn bimetallic ZIF at the cathode achieved an open-circuit voltage of 0.93 V, a current density of 28 mA cm−2 at 0.8 V iR-free, and a peak power density of 374 mW cm−2. [ABSTRACT FROM AUTHOR]