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Issue 1, 2019
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Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy

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Abstract

Development of platinum group metal (PGM)-free catalysts for oxygen reduction reaction (ORR) is essential for affordable proton exchange membrane fuel cells. Herein, a new type of atomically dispersed Co doped carbon catalyst with a core–shell structure has been developed via a surfactant-assisted metal–organic framework approach. The cohesive interactions between the selected surfactant and the Co-doped zeolitic imidazolate framework (ZIF-8) nanocrystals lead to a unique confinement effect. During the thermal activation, this confinement effect suppressed the agglomeration of Co atomic sites and mitigated the collapse of internal microporous structures of ZIF-8. Among the studied surfactants, Pluronic F127 block copolymer led to the greatest performance gains with a doubling of the active site density relative to that of the surfactant-free catalyst. According to density functional theory calculations, unlike other Co catalysts, this new atomically dispersed Co–N–C@F127 catalyst is believed to contain substantial CoN2+2 sites, which are active and thermodynamically favorable for the four-electron ORR pathway. The Co–N–C@F127 catalyst exhibits an unprecedented ORR activity with a half-wave potential (E1/2) of 0.84 V (vs. RHE) as well as enhanced stability in the corrosive acidic media. It also demonstrated high initial performance with a power density of 0.87 W cm−2 along with encouraging durability in H2–O2 fuel cells. The atomically dispersed Co site catalyst approaches that of the Fe–N–C catalyst and represents the highest reported PGM-free and Fe-free catalyst performance.

Graphical abstract: Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy

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Supplementary files

Article information


Submitted
14 Sep 2018
Accepted
23 Oct 2018
First published
23 Oct 2018

Energy Environ. Sci., 2019,12, 250-260
Article type
Paper
Author version available

Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy

Y. He, S. Hwang, D. A. Cullen, M. A. Uddin, L. Langhorst, B. Li, S. Karakalos, A. J. Kropf, E. C. Wegener, J. Sokolowski, M. Chen, D. Myers, D. Su, K. L. More, G. Wang, S. Litster and G. Wu, Energy Environ. Sci., 2019, 12, 250
DOI: 10.1039/C8EE02694G

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