Journal
LANGMUIR
Volume 31, Issue 19, Pages 5529-5536Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.langmuir.5b00310
Keywords
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Funding
- New Energy and Industrial Technology Development Organization (NEDO), Japan
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The iron (Fe) electrodeposition-electrochemical dissolution has been employed on nitrogen-doped carbon material (P-PI) prepared via multi-step pyrolysis of a polyimide precursor to achieve the introduction of Fe species, and its influence on the oxygen reduction reaction (ORR) is investigated by cyclic and rotating ring-disk electrode voltammetry in 0.5 M H2SO4. After the electrochemical treatment, the overpotential and H2O2 production percentage of ORR on the P-PI are decreased and the number of electrons transferred is increased in the meanwhile. In combination with the results of X-ray absorption fine structure spectra, the presence of Fe-N-x sites (Fe ions coordinated by nitrogen) is believed to be responsible for the improved ORR performance. Further kinetic analysis indicates that a two-electron reduction of O-2 is predominant on the untreated P-PI with coexistence of a direct four-electron transformation of O-2 to H2O, while the introduction of Fe species leads to a larger increase in the rate constant for the four-electron reduction than that for the two-electron process, being in good agreement with the view that Fe-N-x sites are active for four-electron ORR.
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