Graphene-supported Fe-N/C Composite Catalyst for Oxygen Reduction†

doi:10.7503/cjcu20150232

Abstract

Abstract:

NG/Fe-N/C composite catalysts with sandwich nanostructure were synthesized by an impregnation method using polypyrrole as ligand. Nitrogen-doped graphene was doped into the Fe-N/C catalyst during the process of synthesis. By the synergistic reaction between graphene and Fe-N/C, the catalytic activity and stability of catalyst were improved. XRD, SEM, TEM and XPS were used to character the physical structure, morphology and chemical composite of catalysts. The results show that the catalyst has the optimal oxyen reductive reaction(ORR) activity when the mass ratio of grapheme to BP2000 is 1∶4 and the heat treatment temperature is 800 ℃. The accelerated aging test(AAT) test shows that catalyst NG/Fe-N/C-25 is more stable than commercial 20% Pt/C catalyst in acidic medium. The total N content of NG/Fe-N/C-25 catalyst is about 5.17%, and the content of graphite nitrogen and pyridine nitrogen are about 44.35% and 32.66%, respectively. These high content of graphitic nitrogen and pyridine nitrogen may result in the high ORR activity and stability.

Key words: Proton exchange membrane fuel cell, Polypyrrole, Nitrogen-doped graphene, Oxygen reductive reaction, Stability, Sandwich nanostructural NG/Fe-N/C composite catalyst

CLC Number:

O643

TrendMD:

LI Shang, LI Pei, ZHAO Wei, KANG Huan, PAN Mu. Graphene-supported Fe-N/C Composite Catalyst for Oxygen Reduction^†[J]. Chem. J. Chinese Universities, 2015, 36(9): 1737.

Figures/Tables 8

Fig.1 XRD patterns of NG/Fe-N/C-25 samples after heat treatment in NH3Heat treatment temperature/℃: a. 600; b. 700; c. 800; d. 900.

Fig.2 SEM images of NG/Fe-N/C-25 composite before(A) and after(B) heat treatment at 800 ℃

Fig.3 TEM images(A—C) and HRTEM image(D) of NG/Fe-N/C-25 composite before(A, B) and after(C, D) heat treatment with different magnifications

Fig.4 Effect of heat treatment temperature on ORR curves on a glassy carbon electrode coated with NG/Fe-N/C-25 catalystsElectrode: O2-saturated 0.5 mol/L H2SO4 solution; electrode rotating rate: 400 r/min; potential scan rate: 5 mV/s; NG/Fe-N/C-25 catalysts loading: 0.40 mg/cm2. The inset shows the ORR kinetic activity potential at 0.5 mA/cm2 vs. heat treatment temperature.

Fig.5 Effect of doping content of N-doped graphene on ORR curves on a glassy carbon electrode coated with the NG/Fe-N/C catalysts at 800 ℃ with different doping ratiosElectrode: O2-saturated 0.5 mol/L H2SO4 solution; electrode rotating rate: 400 r/min; potential scan rate: 5 mV/s; NG/Fe-N/C-25 catalysts loading: 0.40 mg/cm2.

Fig.6 XPS spectra of N1s for NG/Fe-N/C-25 catalyst

Table 1 Percentage of C, O, N and Fe elements on the surface of NG/Fe-N/C-25 catalyst

Element	C₁_s	O₁_s	N₁_s	Fe₂_p
Atomic fraction(%)	85.62	8.1	5.17	1.12

Fig.7 ORR polarization curves for NG/Fe-N/C-25 catalyst(A) and 20%Pt/C catalyst(B) before(a) and after AAT(b)The ORR tests were performed in O2 saturated 0.5 mol/L H2SO4 at room temperature with a rotation speed of 1600 r/min and a sweep rate of 5 mV/s.

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