Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 4, Issue 22, Pages 8645-8657Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6ta01543c
Keywords
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Funding
- NRF [NRF-2010-0029245]
- Global Frontier RAMP
- D Program on Center for Multiscale Energy System - Ministry of Education, Science and Technology of Korea [NRF 2011-0031571]
- National Research Foundation of Korea [2010-0029245, 2011-0031571] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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A new facile template-free method is presented to synthesize Fe-treated N-doped carbon (Fe/N-C) catalysts for oxygen reduction reaction (ORR) by employing a synthesis protocol of pyrolysis-leaching-stabilization (PLS) sequence of polypyrrole in the presence of ferric source, which serves dual purposes of an oxidant for pyrrole polymerization and an iron source. Each step in the PLS sequence is assessed in detail in terms of the related structural properties of the resulting carbon catalysts, and their effects on ORR activities are elaborated to confirm the validity of the current synthesis protocol. It is found that the as-prepared carbon catalyst exhibits outstanding high catalytic activity in both alkaline and acidic conditions. The carbon catalyst prepared at a pyrolysis temperature of 900 degrees C (FePPyC-900) shows remarkably high ORR activity with onset potential of 0.96 V (vs. RHE), which is similar to that of Pt/C, whereas the half-wave potential (E-1/2) of FePPyC-900 is 0.877 V, more positive than that of Pt/C at the same catalyst loading amount under alkaline conditions. Furthermore, the FePPyC-900 catalyst also illustrates exceptionally high activity under acidic conditions with onset and half-wave potentials of 0.814 and 0.740 V, respectively, which are almost comparable to those (0.817 and 0.709 V) of the state-of-the-art Pt/C catalyst, which is rarely observed for non-Pt-based carbon catalysts. In addition, the FePPyC-900 catalyst displays much better stability and methanol tolerance than the Pt/C and exhibits a four electron transfer pathway under both alkaline and acidic conditions. Such extraordinary high ORR activity and stability of the FePPyC-samples can be attributed to the implementation of extra stabilization step in addition to conventional sample preparation steps of pyrolysis and subsequent leaching in current PLS synthesis protocol as well as to the use of highly conducting PPy as a single precursor of carbon and nitrogen in the presence of Fe.
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