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

Ferrero, GA; Preuss, K; Marinovic, A; Jorge, AB; Mansor, N; Brett, DJL; Fuertes, AB; ... Titirici, M-M; + view all (2016) Fe-N-Doped Carbon Capsules with Outstanding Electrochemical Performance and Stability for the Oxygen Reduction Reaction in Both Acid and Alkaline Conditions. ACS Nano , 10 (6) pp. 5922-5932. 10.1021/acsnano.6b01247. Green open access

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Abstract

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.

Type: Article
Title: Fe-N-Doped Carbon Capsules with Outstanding Electrochemical Performance and Stability for the Oxygen Reduction Reaction in Both Acid and Alkaline Conditions
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acsnano.6b01247
Publisher version: https://doi.org/10.1021/acsnano.6b01247
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: capsule; carbon nanomaterial; nitrogen-doping; non-noble metal catalysts; oxygen reduction reaction
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10069233
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