Fe-Cluster Pushing Electrons to N-Doped Graphitic Layers with Fe3C(Fe) Hybrid Nanostructure to Enhance O2 Reduction Catalysis of Zn-Air Batteries
- 18 January 2017
- journal article
- research article
- Published by American Chemical Society (ACS) in ACS Applied Materials & Interfaces
- Vol. 9 (5), 4587-4596
- https://doi.org/10.1021/acsami.6b13166
Abstract
Non-noble metal catalysts with catalytic activity toward oxygen reduction reaction (ORR) comparable or even superior to that of Pt/C are extremely important for the wide application of metal–air batteries and fuel cells. Here, we develop a simple and controllable strategy to synthesize Fe-cluster embedded in Fe3C nanoparticles (designated as Fe3C(Fe)) encased in nitrogen-doped graphitic layers (NDGLs) with graphitic shells as a novel hybrid nanostructure as an effective ORR catalyst by directly pyrolyzing a mixture of Prussian blue (PB) and glucose. The pyrolysis temperature was found to be the key parameter for obtaining a stable Fe3C(Fe)@NDGL core–shell nanostructure with an optimized content of nitrogen. The optimized Fe3C(Fe)@NDGL catalyst showed high catalytic performance of ORR comparable to that of the Pt/C (20 wt %) catalyst and better stability than that of the Pt/C catalyst in alkaline electrolyte. According to the experimental results and first principle calculation, the high activity of the Fe3C(Fe)@NDGL catalyst can be ascribed to the synergistic effect of an adequate content of nitrogen doping in graphitic carbon shells and Fe-cluster pushing electrons to NDGL. A zinc–air battery utilizing the Fe3C(Fe)@NDGL catalyst demonstrated a maximum power density of 186 mW cm–2, which is slightly higher than that of a zinc–air battery utilizing the commercial Pt/C catalyst (167 mW cm–2), mostly because of the large surface area of the N-doped graphitic carbon shells. Theoretical calculation verified that O2 molecules can spontaneously adsorb on both pristine and nitrogen doped graphene surfaces and then quickly diffuse to the catalytically active nitrogen sites. Our catalyst can potentially become a promising replacement for Pt catalysts in metal-air batteries and fuel cells.Keywords
Funding Information
- Guangdong Province (2013N080)
- Shenzhen Municipality (JCYJ20140509093817681, JCYJ20140903101617271, JCYJ20140903101633318, ZDSY20130331145131323)
- Science Technology and Innovation Committee of Shenzhen Municipality (KYPT20141016105435850)
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