Fe–N-Doped Carbon Capsules with Outstanding Electrochemical Performance and Stability for the Oxygen Reduction Reaction in Both Acid and Alkaline Conditions

氧还原反应 兴奋剂 氧气 无机化学 碳纤维 电化学 氧还原 还原(数学) 材料科学 化学工程 化学 纳米技术 电极 有机化学 光电子学 物理化学 数学 复合数 工程类 几何学 复合材料
作者
Guillermo A. Ferrero,Kathrin Preuß,Adam Marinovic,Ana Jorge Sobrido,Noramalina Mansor,Dan J. L. Brett,Antonio B. Fuertes,Marta Sevilla,Maria‐Magdalena Titirici
出处
期刊:ACS Nano [American Chemical Society]
卷期号:10 (6): 5922-5932 被引量:417
标识
DOI:10.1021/acsnano.6b01247
摘要

High surface area N-doped mesoporous carbon capsules with iron traces exhibit outstanding electrocatalytic activity for the oxygen reduction reaction in both alkaline and acidic media. In alkaline conditions, they exhibit more positive onset (0.94 V vs RHE) and half-wave potentials (0.83 V vs RHE) than commercial Pt/C, while in acidic media the onset potential is comparable to that of commercial Pt/C with a peroxide yield lower than 10%. The Fe-N-doped carbon catalyst combines high catalytic activity with remarkable performance stability (3500 cycles between 0.6 and 1.0 V vs RHE), which stems from the fact that iron is coordinated to nitrogen. Additionally, the newly developed electrocatalyst is unaffected by the methanol crossover effect in both acid and basic media, contrary to commercial Pt/C. The excellent catalytic behavior of the Fe-N-doped carbon, even in the more relevant acid medium, is attributable to the combination of chemical functions (N-pyridinic, N-quaternary, and Fe-N coordination sites) and structural properties (large surface area, open mesoporous structure, and short diffusion paths), which guarantees a large number of highly active and fully accessible catalytic sites and rapid mass-transfer kinetics. Thus, this catalyst represents an important step forward toward replacing Pt catalysts with cheaper alternatives. In this regard, an alkaline anion exchange membrane fuel cell was assembled with Fe-N-doped mesoporous carbon capsules as the cathode catalyst to provide current and power densities matching those of a commercial Pt/C, which indicates the practical applicability of the Fe-N-carbon catalyst.
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