Samireddi SAishwarya VShown IMuthusamy SUnni S.MKEN-TSUNG WONGChen K.-HChen L.-C.2022-12-142022-12-14202116136810https://www.scopus.com/inward/record.uri?eid=2-s2.0-85117163267&doi=10.1002%2fsmll.202103823&partnerID=40&md5=1d43e1f02acfebcc86d7c7f6d371872dhttps://scholars.lib.ntu.edu.tw/handle/123456789/626371A heterobimetallic corrole complex, comprising oxygen reduction reaction (ORR) active non-precious metals Co and Fe with a corrole-N4 center (PhFCC), is successfully synthesized and used to prepare a dual-atom molecular catalyst (DAMC) through subsequent low-temperature pyrolysis. This low-temperature pyrolyzed electrocatalyst exhibited impressive ORR performance, with onset potentials of 0.86 and 0.94 V, and half-wave potentials of 0.75 and 0.85 V, under acidic and basic conditions, respectively. During potential cycling, this DAMC displayed half-wave potential losses of only 25 and 5 mV under acidic and alkaline conditions after 3000 cycles, respectively, demonstrating its excellent stability. Single-cell Nafion-based proton exchange membrane fuel cell performance using this DAMC as the cathode catalyst showed a maximum power density of 225 mW cm−2, almost close to that of most metal–N4 macrocycle-based catalysts. The present study showed that preservation of the defined CoN4 structure along with the cocatalytic Fe–Cx site synergistically acted as a dual ORR active center to boost overall ORR performance. The development of DAMC from a heterobimetallic CoN4-macrocyclic system using low-temperature pyrolysis is also advantageous for practical applications. © 2021 Wiley-VCH GmbH.corroles; dual-atom molecular catalyst; fuel cells; metal–N4 macrocycles; non-precious electrocatalysts; oxygen reduction reaction[SDGs]SDG7Alkalinity; Atoms; Electrocatalysts; Electrolytic reduction; Molecular oxygen; Polypyrroles; Proton exchange membrane fuel cells (PEMFC); Pyrolysis; Corroles; Dual-atom molecular catalyst; Heterobimetallics; Low-temperature pyrolysis; Lows-temperatures; Macrocycles; Metal–n4 macrocycle; Molecular catalysts; Non-precious electrocatalyst; Oxygen reduction reaction; Temperaturejournal article10.1002/smll.202103823346655222-s2.0-85117163267