Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 46, Pages 20465-20469Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009700
Keywords
3D graphene frameworks; metal-organic frameworks; negative pressure; oxygen reduction reaction; single sites
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Funding
- National Key R&D Program of China 2017YFA [0208300, 0700104]
- National Natural Science Foundation of China [21522107, 21671180]
- DNL Cooperation Fund, CAS [NDL201918]
- China Postdoctoral Science Foundation [BX20200317]
- Fujian Institute of Innovation, CAS
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Herein, we report a negative pressure pyrolysis to access dense single metal sites (Co, Fe, Ni etc.) with high accessibility dispersed on three-dimensional (3D) graphene frameworks (GFs), during which the differential pressure between inside and outside of metal-organic frameworks (MOFs) promotes the cleavage of the derived carbon layers and gradual expansion of mesopores. In situ transmission electron microscopy and Brunauer-Emmett-Teller tests reveal that the formed 3D GFs possess an enhanced mesoporosity and external surface area, which greatly favor the mass transport and utilization of metal sites. This contributes to an excellent oxygen reduction reaction (ORR) activity (half-wave potential of 0.901 V vs. RHE). Theoretical calculations verify that selective carbon cleavage near Co centers can efficiently lower the overall ORR theoretical overpotential in comparison with intact atomic configuration.
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