Nitrogen-doped graphite encapsulated Fe/Fe3C nanoparticles and carbon black for enhanced performance towards oxygen reduction

doi:10.1016/j.jmst.2019.07.008

Abstract

Abstract:

Non-noble metal (NNM) catalysts have recently attracted intensive interest for their high catalytic performance towards oxygen reduction reaction (ORR) at low cost. Herein, a novel NNM catalyst was synthesized by the simple pyrolysis of carbon black, urea and a Fe-containing precursor, which exhibits excellent ORR catalytic activity, superior durability and methanol tolerance versus the Pt/C catalyst in both alkaline and acidic solutions. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction (XRD) characterizations demonstrate that the product is a nitrogen-doped hybrid of graphite encapsulated Fe/Fe₃C nanoparticles and carbon black. X-ray photoelectron spectrum (XPS) and electrochemical analyses indicate that the catalytic performance and chemical stability correlate closely with a nitrogen-rich layer on the Fe/Fe₃C nanoparticle after pyrolysis with presence of urea, leading to the same four-electron pathway towards ORR as the Pt/C catalyst. The hybrid is prospective to be an efficient ORR electrocatalyst for direct methanol fuel cells with high catalytic performance at low cost.

Key words: Nitrogen doping, Hybrid, Fe/Fe₃C, Carbon black, Oxygen reduction reaction

Zhu Jie, Xiong Zewei, Zheng Jiming, Luo Zhihong, Zhu Guangbin, Xiao Chao, Meng Zhengbing, Li Yibing, KunLuo. Nitrogen-doped graphite encapsulated Fe/Fe₃C nanoparticles and carbon black for enhanced performance towards oxygen reduction[J]. J. Mater. Sci. Technol., 2019, 35(11): 2543-2551.

Figures/Tables 8

Fig. 1. Morphologies of the as-synthesized Fe/Fe3C@NC/CB hybrid: (a) SEM image; (b) TEM image; (c) HRTEM image; (d) EDS element mapping.

Fig. 2. XRD (a) and BET (b) analyses of the Fe/Fe3C@NC/CB hybrid (V: volume; W: pore size).

Fig. 3. Characterization of catalytic activity towards ORR: (a) reduction segments of the CV curves of the Fe/Fe3C@NC/CB and Pt/C catalysts in O2-saturated 0.1 M KOH electrolyte at a scan rate of 50 mV s-1; (b) RDE polarization curves of the Fe/Fe3C@NC/CB and Pt/C catalysts with a scan rate of 5 mV s-1 at 1600 rpm in O2-saturated 0.1 M KOH electrolyte; (c) Tafel plots of the Fe/Fe3C@NC/CB and Pt/C catalysts extracted from (b); (d) RDE polarization curves of the Fe/Fe3C@NC/CB and Pt/C catalysts with a scan rate of 5 mV s-1 at 1600 rpm in O2-saturated 0.1 M HClO4 electrolyte.

Fig. 4. ORR durability and methanol tolerance of the Fe/Fe3C@NC/CB and Pt/C catalysts: (a) chronoamperometric (i-t) responses at -0.2 V (vs. Hg/HgO) with a rotation rate of 400 rpm in O2-saturated 0.1 M KOH solution; (b) i-t responses at -0.2 V (vs. Hg/HgO) with a rotation rate of 400 rpm in O2-saturated 0.1 M KOH solution with addition of 3 M CH3OH; (c) i-t responses at 0.1 V (vs. SCE) with a rotation rate of 400 rpm in O2-saturated 0.1 M HClO4 solution; (d) i-t responses at 0.1 V (vs. SCE) with a rotation rate of 400 rpm in O2-saturated 0.1 M HClO4 solution with addition of 3 M CH3OH (I: current; I0: initial current).

Fig. 5. Morphologies and structure analyses: (a) SEM image of the Fe/Fe3C@C/CB hybrid; (b) SEM image of the NCB; (c) TEM image of the Fe/Fe3C@C/CB hybrid; (d) HRTEM image of the Fe/Fe3C@C/CB hybrid; (e) HRTEM micrograph of the NCB; (f) HRTEM micrograph of the TEM image of the Fe/Fe3C@C/CB-A hybrid; (g) HRTEM image of the Fe/Fe3C@NC/CB-A hybrid; (h) XRD analysis of the Fe/Fe3C@C/CB, NCB, Fe/Fe3C@C/CB-A and Fe/Fe3C@NC/CB-A hybrids.

Fig. 6. RDE analysis of ORR kinetics with a scan rate of 5 mV s-1 at 1600 rpm in O2-saturated 0.1 M KOH electrolyte: (a) LSV profiles of the pure CB, NCB, Fe/Fe3C@C/CB, Fe/Fe3C@C/CB-A and Fe/Fe3C@NC/CB-A; (b) K-L plot of the Fe/Fe3C@NC/CB hybrid; (c) K-L plot of the Fe/Fe3C@C/CB hybrid; (d) K-L plot of the NCB.

Fig. 7. XPS analysis of the Fe/Fe3C@NC/CB hybrid: (a) Fitting of the resolved C1s signal; (b) Fitting of the resolved O1s signal; (c) Fitting of the resolved N1s signal; (d) Fitting of the resolved Fe2p signal.

Fig. 8. Schematic structure and ORR reaction of the Fe/Fe3C@NC/CB hybrid.

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Nitrogen-doped graphite encapsulated Fe/Fe₃C nanoparticles and carbon black for enhanced performance towards oxygen reduction

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