期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 7, 期 28, 页码 16920-16936出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ta01837a
关键词
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资金
- National Research Foundation (NRF) - Ministry of Science and ICT & Future Planning of Republic of Korea [2017R1A2B3004917]
A porous, efficient, and durable nonprecious electrocatalyst for the oxygen reduction reaction (ORR) under both alkaline and acidic conditions is synthesized by a green, solvent-free, one-pot, economical, scalable, and template-free strategy. In situ formed graphitic carbon nitride (g-C3N4) is utilized as a sacrificial template for constructing the core-shell Fe3C@NSC electrocatalyst with a highly porous substructure and nanosheet-like morphology. The presence of glucose facilitates the homogeneous distribution of nanoparticles and establishes the nanosheet structure, otherwise agglomeration and formation of nanotubes occur in the Fe3C@NSC electrocatalyst. Optimizing the synthetic conditions generates a highly active ORR electrocatalyst with a unique mesoporous architecture, large surface area, high nitrogen doping level, encapsulated Fe3C nanoparticles in NS co-doped carbon layers and multiple exposed edge active centers. The best performing electrocatalyst displays outstanding ORR performance under alkaline conditions with onset potential and half-wave potential (E-1/2) values of 1.059 and 0.938 V vs. the reversible hydrogen electrode (RHE), much higher than those of the state-of-the-art commercial Pt/C (20%), and admirable performance in acidic media. In addition, it exhibits 4e(-) selectivity, tolerance toward methanol, and superb durability with zero degradation after 12 000 potential cycles under both alkaline and acidic conditions. These exceptional characteristics make the as-synthesized electrocatalyst one of the top-level non-precious ORR electrocatalysts reported to date.
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