Enhancing oxygen reduction of Fe-N-C active sites onto graphene via bismuth sacrifice for Zn-air batteries

doi:10.1016/S1872-2067(24)60002-1

Abstract

Abstract:

Synthesizing low-cost electrocatalysts with rich metal-nitrogen-carbon active sites for the oxygen reduction reaction (ORR) is critical for developing high-performance Zn-air batteries. However, it is challenging for the pyrolysis cheap molecular precursors (such as melamine and iron salts) is challenging because of the spontaneous aggregation of metal components and undesired byproducts during pyrolysis. Herein, we describe an approach to generate graphene-supported accessible Fe-N-C active sites by introducing a removable bismuth compound that efficiently inhibits the formation of iron-related particles and tubular carbon structures. The graphene-supported Fe(Bi)-N-C electrocatalyst exhibited high ORR activity under both alkaline (E_1/2 ~0.916 V) and acidic (E_1/2 ~0.784 V) conditions, along with excellent durability (15 mV degradation after 10 k cycles accelerated test). Using the catalytic material as the cathode, the Zn-air battery delivered a high power density of 201.4 mW cm^-2 and a high stability over 1000 cycles. This investigation presents a promising controlled pyrolysis solution for the scalable synthesis of low-cost, high-performance metal-nitrogen-carbon-based catalytic materials.

Key words: Oxygen reduction reaction, Bismuth, Graphene, Zn-air battery, Fe-N-C

Zhiyuan Yang, Yan Zhang, Juanding Xiao, Junying Wang, Junzhong Wang. Enhancing oxygen reduction of Fe-N-C active sites onto graphene via bismuth sacrifice for Zn-air batteries[J]. Chinese Journal of Catalysis, 2024, 59: 272-281.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60002-1

https://www.cjcatal.com/EN/Y2024/V59/I4/272

Figures/Tables 7

Fig. 1. Schematic illustration of the synthesis of dense Fe-N-C sites anchored onto graphene.

Fig. 2. Material synthesis and structure characterization. XRD patterns (a,b) and Raman spectra (c) of the catalysts. (d) Isothermal N2 adsorption-desorption plots of Fe(Bi)-N-C/G-A, Fe-N-C/G-A, and (Bi)-N-C/G-A.

Fig. 3. Morphology characterization of Fe(Bi)-N-C/G-A. (a) SEM image. (b) TEM image. (c,d) EDS elemental mappings. (e) HAADF-STEM micrographs of Fe(Bi)-N-C/G-A. (f) EELS of the framed area in (e).

Fig. 4. (a) XPS survey spectrum of Fe(Bi)-N-C/G-A, Fe-N-C/G-A, (Bi)-N-C/G-A, and N-C/G-A. (b,c) High-resolution Fe 2p and N 1s XPS spectra of Fe(Bi)-N-C/G-A and Fe-N-C/G-A. (d) N species in Fe(Bi)-N-C/G-A and Fe-N-C/G-A.

Fig. 5. Atomic structural analysis of as-prepared samples. (a) Fe K-edge XANES spectra. (b) FT k2-weighted Fe K-edge EXAFS spectra. (c,d) EXAFS fitting results in R space. (e) Fe K-edge wavelet transform of EXAFS for Fe(Bi)-N-C/G-A, with Fe-N-C/G-A, FePc, and Fe foil used as references.

Fig. 6. Electrochemical ORR activity of as-prepared samples. LSV curves (a) and Jk (at 0.9 V) and E1/2 (b). (c) Corresponding Tafel profile. (d) Polarization curves for Fe(Bi)-N-C/G-A at different rotation speeds (inset: K-L plot for Fe(Bi)-N-C/G-A). (e) Electron transfer numbers and H2O2 yield of Fe(Bi)-N-C/G-A, Fe-N-C/G-A, (Bi)-N-C/G-A, N-C/G-A, and Pt/C in 0.1 mol L-1 KOH solution. (f) Stability measurement of Fe(Bi)-N-C/G-A, Fe-N-C/G-A and Pt/C in O2-saturated 0.1 mol L-1 KOH solution. (g) Double-layer capacitor (Cdl) of Fe(Bi)-N-C/G-A and Fe-N-C/G-A. (h) LSV curves of Fe(Bi)-N-C/G-A, Fe-N-C/G-A, (Bi)-N-C/G-A, N-C/G-A, and commercial Pt/C at a sweep rate of 5 mV s-1 in O2-saturated 0.1 mol L-1 HClO4 solution.

Fig. 7. Zn-air battery performance. Open-circuit potential curves (a), discharge polarization and the corresponding power density curves (b) of Zn-air batteries with Fe(Bi)-N-C/G-A, Fe-N-C/G-A, and Pt/C as air cathodes. (c) Specific capacity plot at 20 mA cm-2. (d) Galvanostatic charging/discharging cycling curves of Fe(Bi)-N-C/G-A + RuO2 and Pt/C + RuO2 air cathodes at 5 mA cm-2.

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