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Atomically dispersed Fe–Nₓ active sites within hierarchical mesoporous carbon as efficient electrocatalysts for the oxygen reduction reaction

Gu, Wenling, Wu, Maochun, Sun, Jing, Xu, Jianbo, Zhao, Tianshou
Journal of materials chemistry A 2019 v.7 no.35 pp. 20132-20138
active sites, carbon, catalysts, catalytic activity, cobalt, cost effectiveness, dopamine, durability, electrochemistry, energy conversion, ferric chloride, hydrophilicity, platinum, polymerization, porous media, potassium hydroxide, surface area
It is still a great challenge to develop highly efficient catalysts with earth abundant materials to replace the precious platinum group metal (PGM) catalysts for the oxygen reduction reaction (ORR). Here, we report a self-sacrificing template strategy to synthesize hierarchical mesoporous carbon materials with atomically dispersed Fe–Nₓ active sites. Derived from an Fe–polydopamine precursor obtained via in situ polymerization of dopamine and etching of a cobalt template using an FeCl₃ solution, the resultant catalyst shows a high specific surface area (1229.3 m² g⁻¹), a hierarchical mesoporous structure, an improved hydrophilicity, and abundant atomically dispersed Fe–Nₓ active sites. As a result, the single atom catalyst exhibits a remarkable activity and durability in 0.1 M KOH with an onset and half-wave potential of 1.03 and 0.88 V, respectively, which surpass those of its commercial Pt/C counterpart. In acidic and neutral media, the catalyst also exhibits a comparable electrocatalytic activity to but much greater durability than commercial Pt/C. This work opens a new avenue for synthesis of cost-effective catalysts at the atomic scale for efficient energy conversion.