Journal
Energy & Environmental Science
Volume 9, Issue 12, Pages 3736-3745Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6ee01867j
Keywords
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Funding
- Ministry of Science and Technology of China [2013CB933100, 2012CB215500]
- National Natural Science Foundation of China [21573222, U1532117, 91545202]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020200]
- CAS Youth Innovation Promotion
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A coordinatively unsaturated copper-nitrogen architecture in copper metalloenzymes is essential for its capability to catalyze the oxygen reduction reaction (ORR). However, the stabilization of analogous active sites in realistic catalysts remains a key challenge. Herein, we report a facile route to synthesize highly doped and exposed copper(I)-nitrogen (Cu(I)-N) active sites within graphene (Cu-N(C)C) by pyrolysis of coordinatively saturated copper phthalocyanine, which is inert for the ORR, together with dicyandiamide. Cu(I)-N is identified as the active site for catalyzing the ORR by combining physicochemical and electro-chemical studies, as well as density function theory calculations. The graphene matrix could stabilize the high density of Cu(I)-N active sites with a copper loading higher than 8.5 wt%, while acting as the electron-conducting path. The ORR activity increases with the specific surface area of the Cu-N(C)C catalysts due to more exposed Cu(I)-N active sites. The optimum Cu-N(C)C catalyst demonstrates a high ORR activity and stability, as well as an excellent performance and stability in zinc-air batteries with ultralow catalyst loading.
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