期刊
ADVANCED ENERGY MATERIALS
卷 8, 期 9, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201701771
关键词
active site imprinting; FeN4 active sites; metal-nitrogen coordination; non-noble metal catalysts; oxygen reduction reaction
类别
资金
- German Federal Ministry of Education and Research (BMBF)
- DAAD-RISE program
- 7th framework project EUROLIS [314515]
Iron-or cobalt-coordinated heteroatom doped carbons are promising alternatives for Pt-based cathode catalysts in polymer-electrolyte fuel cells. Currently, these catalysts are obtained at high temperatures. The reaction conditions complicate the selective and concentrated formation of metal-nitrogen active sites. Herein a mild procedure is introduced, which is conservative toward the carbon support and leads to active-site formation at low temperatures in a wet-chemical metal-coordination step. Active-site imprinted nitrogen doped carbons are synthesized via ionothermal carbonization employing Lewis-acidic Mg2+ salt. The obtained carbons with large tubular porosity and imprinted N-4 sites lead to very active catalysts with a half-wave potential (E-1/2) of up to 0.76 V versus RHE in acidic electrolyte after coordination with iron. The catalyst shows 4e-selectivity and exceptional stability with a half-wave potential shift of only 5 mV after 1000 cycles. The X-ray absorption fine structure as well as the X-ray absorption near edge structure profiles of the most active catalyst closely match that of iron(II) phthalocyanine, proving the formation of active and stable FeN4 sites at 80 degrees C. Metal-coordination with other transition metals reveals that Zn-Nx sites are inactive, while cobalt gives rise to a strong performance increase even at very low concentrations.
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