Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 5, Issue 24, Pages 12243-12251Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7ta01896g
Keywords
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Funding
- National Key Research and Development Program of China [2016YFB0700204]
- NSFC [51602332, 51502327]
- Science and Technology Commission of Shanghai Municipality [15520720400, 15YF1413800, 14DZ2261203, 16DZ2260603]
- Key Project for Young Researcher of State Key Laboratory of High Performance Ceramics and Superfine Microstructure
- One Hundred Talent Plan of Chinese Academy of Sciences
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The replacement of platinum (Pt) by nonprecious catalysts with superior activity and stability for the oxygen reduction reaction (ORR) remains challenging for fuel cell devices. Herein, we describe a controllable strategy to prepare hollow graphitic carbon spheres with Fe-N-doped mesoporous shells via in situ polymerization and functionalization. The optimized catalyst exhibits very superior ORR activity with a half-wave potential (E-1/2) of 0.886 V in 0.1 M KOH, 15 mV more positive than that of commercial Pt/C catalysts. Even in acidic solution, it also shows a competitive 4e(-) ORR activity compared to Pt/C. Most importantly, it demonstrates much better long-term stability and resistance to methanol crossover than Pt/C in both alkaline and acidic media. The outstanding activity is contributed by the synergy of chemical functions (Fe-Nx-coordinated moieties) and excellent structural properties (hollow large cores (similar to 91 nm), open mesopores (similar to 2.1 nm) throughout the shells, and highly graphitic microstructures), ensuring rapid mass-diffusion and electron-transfer kinetics and full accessibility of catalytic sites.
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