Journal
ACS CATALYSIS
Volume 11, Issue 7, Pages 3923-3929Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c05503
Keywords
single-atom catalyst; high coordination number; hierarchically porous structure; oxygen reduction reaction; proton-exchange membrane fuel cell
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Funding
- National Key R&D Program of China 2017YFA [0208300, 0700104]
- National Natural Science Foundation of China [21671180, 21673087, 21873032, 22073033, 21903032]
- DNL Cooperation Fund, CAS [NDL201918]
- Fundamental Research Funds for the Central Universities [2019kfyRCPY116]
- CAS Fujian Institute of Innovation
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The study introduces a hard-template method to synthesize rare-earth single cerium-atom-doped metal-organic frameworks with a hierarchically macro-meso-microporous structure, demonstrated by spherical aberration correction electron microscopy. The Ce sites embedded in the hierarchically macromeso-microporous N-doped carbon catalyst show high half-wave potential and power density in the oxygen reduction reaction.
Fe-N-C electrocatalysts, as a representative of platinum group metal-free (PGM-free) catalysts, exhibit a comparable oxygen reduction reaction (ORR) activity but insufficient stability to that of commercial Pt/C in proton-exchange membrane fuel cells (PEMFCs), due to the unavoidable Fenton's reactions. Herein, we report a hard-template approach to synthesize the rare-earth singlecerium-atom-doped metal-organic frameworks with a hierarchically macro-meso-microporous structure. Spherical aberration correction electron microscopy confirms the atomic dispersion of Ce sites. Additionally, X-ray absorption spectroscopy (XAS) was employed to further verify the coordination environment of Ce sites, which were stabilized by four-coordinated nitrogen atoms and six-oxygen atoms (Ce-N-4/O-6). The Ce sites were embedded in a hierarchically macromeso-microporous N-doped carbon (Ce SAS/HPNC) catalyst, which exhibits a half-wave potential of 0.862 V in ORR and the highest power density of 0.525 W cm(-2) under 2.0 bar H-2/O-2 in the fuel cell test.
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