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Hierarchically porous Fe-N-C nanospindles derived from porphyrinic coordination network for Oxygen Reduction Reaction


We report a size and morphology-controlled synthesis of PCN-222 crystals, a class of zirconium-based iron porphyrinic coordination network, and their pyrolytic derivation of hierarchically porous Fe-N-C electrocatalysts for the oxygen reduction reaction (ORR). By optimizing the precursors concentrations, nanometer-scaled and spindle-shaped PCN-222 crystals are obtained through a solvo-thermal method. A NaCl salt-assisted pyrolysis is employed to convert the PCN-222 crystals to Fe-N-C catalyst, so as to inherit the nanospindle morphology and the Fe-N coordination structure in the PCN precursor, and in the meantime to increase the graphitization degree. A post-activation procedure using concentrated sulfuric acid is further designed to exert a controlled NaCl removal and carbon etching process that optimizes the porous structures and surface properties of the final nanospindle Fe-N-C catalyst. The reaction between the concentrated sulfuric acid and NaCl produces heat to activate acid etching of carbon, and on the other hand consumes the acid to prevent the carbon from over-etching. The unique nanospindle shape and hierarchically porous structure allow efficient exposure of the high-density active sites and their accessibility to reactants; while the high graphitization ensures efficient conduction of electrons involved in the electrocatalytic reaction and good stability of the carbon matrix during the electrocatalytic processes. In results, the as-prepared Fe-N-C catalyst exhibits remarkable ORR performance, with a half-wave potential which is ca. 30 mV more positive than that of the state-of-the-art Pt catalyst and excellent stability in alkaline solution, as well as an ORR activity comparable to Pt in acid solution.

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Publication details

The article was received on 24 Jan 2018, accepted on 02 Mar 2018 and first published on 02 Mar 2018

Article type: Paper
DOI: 10.1039/C8CY00168E
Citation: Catal. Sci. Technol., 2018, Accepted Manuscript
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    Hierarchically porous Fe-N-C nanospindles derived from porphyrinic coordination network for Oxygen Reduction Reaction

    X. Hua, J. Luo, C. Shen and S. Chen, Catal. Sci. Technol., 2018, Accepted Manuscript , DOI: 10.1039/C8CY00168E

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