期刊
SMALL
卷 17, 期 46, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202103823
关键词
corroles; dual-atom molecular catalyst; fuel cells; metal-N4 macrocycles; non-precious electrocatalysts; oxygen reduction reaction
类别
资金
- Ministry of Science and Technology (MOST) [107-2745-M-002-001-ASP, 108-2119-M-002-030, 109-2123-M-002-004]
- Center of Atomic Initiative for New Materials, National Taiwan University [108L9008, 109L9008]
- Department of Science and Technology, New Delhi, India [DST/INSPIRE/04/2018/003308]
- Academia Sinica
A heterobimetallic corrole complex containing Co and Fe was successfully synthesized and used to prepare a dual-atom molecular catalyst through low-temperature pyrolysis, showing impressive ORR performance and stability. The catalyst exhibited a high power density in proton exchange membrane fuel cells, close to that of most metal-N4 catalysts.
A 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.
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