Phosphate-decorated Fe-N-C to promote electrocatalytic oxygen reaction activities for highly stable zinc-air batteries

doi:10.1016/S1872-2067(23)64432-8

Abstract

Abstract:

An obvious challenge for rechargeable Zn-air batteries (ZABs) is the impact of large charge potentials on the oxidation of their cathode catalysts, which accelerates the corrosion of the carbon electrodes, and significantly compromises their stability. It is therefore necessary to design simple methods aimed at facilitating the oxygen evolution reaction (OER) processes of ZABs to suppress the corrosion of their cathode materials. Herein, a biomass-derived N-doped porous carbon material coupled with Fe₃O₄ and Fe₂N nanoparticles and modified with phosphorus (P-Fe₃O₄/Fe₂N@NPC) was designed as an air-cathode to reduce the charging voltage of ZABs. It exhibited excellent ORR/OER bifunctional electrocatalytic activities, and the assembled ZAB displayed an ultra-long service life. DFT calculations showed that the P-modification modulated the electronic state and coordination environment of the active iron atom, thereby significantly enhancing the OER activity of P-Fe₃O₄/Fe₂N@NPC.

Key words: Fe-N-C catalyst, Phosphate-decoration, Oxygen reduction reaction Oxygen evolution reaction, Zinc-air battery

Guangying Zhang, Xu Liu, Xinxin Zhang, Zhijian Liang, Gengyu Xing, Bin Cai, Di Shen, Lei Wang, Honggang Fu. Phosphate-decorated Fe-N-C to promote electrocatalytic oxygen reaction activities for highly stable zinc-air batteries[J]. Chinese Journal of Catalysis, 2023, 49: 141-151.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64432-8

https://www.cjcatal.com/EN/Y2023/V49/I6/141

Figures/Tables 6

Fig. 1. (a) Schematic illustration of the construction of P-Fe3O4/Fe2N@NPC. TEM (b) and HRTEM (c?e) images of P-Fe3O4/Fe2N@NPC. (f) STEM and EDS elemental mapping images of C, N, O, P and Fe elements in P-Fe3O4/Fe2N@NPC.

Fig. 2. XRD patterns (a), Raman spectra (b) and N2 sorption isotherms (c) of Fe3O4/Fe2N@NPC and P-Fe3O4/Fe2N@NPC. Wide XPS spectra (d), high-resolution XPS spectra of Fe 2p (e), P 2p (f), C 1s (g), N 1s (h) and O 1s (i) for Fe3O4/Fe2N@NPC and P-Fe3O4/Fe2N@NPC.

Fig. 3. (a) LSV curves of Fe3O4/Fe2N@NPC, P-Fe3O4/Fe2N@NPC and commercial Pt/C catalysts tested in 0.1 mol L?1 KOH electrolyte at 1600 r min?1 and a sweep rate of 5 mV s-1. (b) ORR Tafel plots of the catalysts. (c) K-L plots of J?1 versus ω?1/2 at potentials of 0.3?0.5 V and the inset shows the LSV curve in the speed range of 400?2025 r min?1. (d) Calculated n and H2O2 yields (%) based on the RRDE of P-Fe3O4/Fe2N@NPC. (e) ORR stability test of P-Fe3O4/Fe2N@NPC before and after 10000 cycles. (f) iR-compensated OER polarization curves of the catalyst in 1 mol L?1 KOH electrolyte. (g) OER Tafel plots. (h) OER stability test of P-Fe3O4/Fe2N@NPC at different current densities, and the inset represents the OER performance before and after 5000 CV cycle. (i) LSV curves of Fe3O4/Fe2N@NPC, P-Fe3O4/Fe2N@NPC in the full OER/ORR region in 0.1 mol L?1 KOH.

Fig. 4. The optimized structures for O2 adsorption on Fe3O4 (a), P-Fe3O4 (b) and Fe2N(c), P-Fe2N (d). (e) Density of states. (f,g) Free energy diagrams of the OER and ORR on Fe3O4, P-Fe3O4, Fe2N and P-Fe2N at potentials of 0 and 1.23 V.

Fig. 5. (a) Schematic diagram of rechargeable ZAB. (b) Specific discharging capacities for liquid state ZABs assembled by P-Fe3O4/Fe2N@NPC and Pt/C+RuO2 at 5 mA cm?2. (c) Cyclic performance of rechargeable ZABs with duration of 10 min per cycle at 10 mA cm?2 for Fe3O4/Fe2N@NPC, P-Fe3O4/Fe2N@NPC and Pt/C+RuO2. (d) Discharge polarization curves and power density curves. (e) The corresponding galvanostatic charge-discharge plots of Fe3O4/Fe2N@NPC and P-Fe3O4/Fe2N@NPC for the 300?312 cycles. (f) The photograph of the battery electrolyte using Fe3O4/Fe2N@NPC (①) and P-Fe3O4/Fe2N@NPC (②) as the air electrode after 10000 cycles.

Fig. 6. (a) Schematic diagram of solid-state ZAB. (b) Open-circuit voltages for solid-state ZABs assembled with P-Fe3O4/Fe2N@NPC by PVA+rGO. (c) Galvanostatic discharge-charge cycling profiles of P-Fe3O4/Fe2N@NPC enabled all-solid-state ZAB by PVA+KOH and PVA+rGO+KOH solid electrolyte at 2 mA cm?2. (d) Photograph of a timepiece is driven by two all-solid-state ZABs in series. (e) Charge-discharge polarization curves for battery tests under different bending degrees at 2 mA cm?2.

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