Controllable synthesis of a self-assembled ultralow Ru, Ni-doped Fe2O3 lily as a bifunctional electrocatalyst for large-current-density alkaline seawater electrolysis

doi:10.1016/S1872-2067(22)64093-2

Abstract

Abstract:

Highly efficient and stable bifunctional electrocatalysts that can be used for large-current-density electrolysis of alkaline seawater are highly desirable for carbon-neutral economies, but their facile and controllable synthesis remains a challenge. Here, self-assembled ultralow Ru, Ni-doped Fe₂O₃ with a lily shaped morphology was synthesized on iron foam (RuNi-Fe₂O₃/IF) via a facile one-step hydrothermal process, in which the intact lily shaped RuNi-Fe₂O₃/IF was obtained by adjusting the ratio of Ru/Ni. Benefitting from the Ru/Ni chemical substitution, the as-synthesized RuNi-Fe₂O₃/IF can act as free-standing dual-function electrodes that are applied to electrocatalysis for the hydrogen evolution (HER) and oxygen evolution reactions (OER) in 1.0 mol L^‒1 KOH, requiring an overpotential of 75.0 mV to drive 100 mA cm^-2 for HER and 329.0 mV for OER. Moreover, the overall water splitting catalyzed by RuNi-Fe₂O₃/IF only demands ultralow cell voltages of 1.66 and 1.73 V to drive 100 mA cm^-2 in 1.0 mol L^‒1 KOH and 1.0 mol L^‒1 KOH seawater electrolytes, respectively. The electrodes show remarkable long-term durability, maintaining current densities exceeding 100 mA cm^-2 for more than 100 h and thus outperforming the two-electrode system composed of noble catalysts. This work provides an efficient, economical method to synthesize self-standing bifunctional electrodes for large-current-density alkaline seawater electrolysis, which is of significant importance for ecological protection and energy exploitation.

Key words: RuNi-Fe₂O₃/IF, Lily shape, Bifunctional electrocatalyst, Alkaline seawater splitting, Large current density

Tong Cui, Xuejun Zhai, Lili Guo, Jing-Qi Chi, Yu Zhang, Jiawei Zhu, Xuemei Sun, Lei Wang. Controllable synthesis of a self-assembled ultralow Ru, Ni-doped Fe₂O₃ lily as a bifunctional electrocatalyst for large-current-density alkaline seawater electrolysis[J]. Chinese Journal of Catalysis, 2022, 43(8): 2202-2211.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64093-2

https://www.cjcatal.com/EN/Y2022/V43/I8/2202

Figures/Tables 5

Fig. 1. (a) Schematic diagram of the one-step hydrothermal synthesis of RuNi-Fe2O3/IF. (b) SEM image of RuNi-Fe2O3/IF. TEM (c) and HRTEM (d) images of RuNi-Fe2O3/IF. SEM images of Ni-Fe2O3/IF (e), RuNi-Fe2O3/IF (1:4) (f), RuNi-Fe2O3/IF (1:1) (g), RuNi-Fe2O3/IF (4:1) (h), and Ru-Fe2O3/IF (i). (j) TEM and the corresponding EDX element mappings of Ni, Fe, Ru, and O for RuNi-Fe2O3/IF.

Fig. 2. (a) XRD pattern of RuNi-Fe2O3/IF. High-resolution XPS spectra of Fe 2p (b), Ni 2p (c), and Ru 3p (d). Structure models (e) and the density of states (f) RuNi-Fe2O3 and Fe2O3.

Fig. 3. HER performance of the as-prepared catalysts: polarization curves (a), overpotential at 100, 500, and 1000 mA cm-2 (b), and corresponding Tafel plots (c). OER performance of the as-prepared catalysts for (b) overpotential at 100, 500, and 1000 mA cm-2: polarization curves (d). Corresponding Tafel plots (e). (f) Chronoamperometry i-t curve of 20 h for HER and OER.

Fig. 4. (a) HER activity and OER activity of RuNi-Fe2O3/IF in 1.0 mol L?1 KOH, 1.0 mol L?1 KOH + 0.5 mol L?1 NaCl, and 1.0 mol L?1 KOH seawater electrolytes. (b) Overpotential of as-prepared catalysts at 100, 500, and 1000 mA cm-2 for HER and OER. Corresponding Tafel plots for OER (c) and HER (d). (e) Comparison of the overpotentials for OER (at 100 mA cm-2) and HER (at 100 mA cm-2) of the RuNi-Fe2O3/IF and other bifunctional electrocatalysts in 1.0 mol L?1 KOH electrolyte. (f) EIS Nyquist plots of the RuNi-Fe2O3/IF catalyst in different solutions. (g) Polarization curves of the RuNi-Fe2O3/IF catalyst before and after 3000 cycles. (h) Chronoamperometry i-t curve of 24 h for HER and OER in 1.0 mol L?1 KOH seawater.

Fig. 5. (a) The LSV curves of overall water splitting in 1.0 mol L?1 KOH, 1.0 mol L?1 KOH seawater. (b) Chronoamperometry i-t curve of 100 h for RuNi-Fe2O3/IF in 1.0 mol L?1 KOH seawater. Photographs of the homemade two-electrode cell (c) and the gas generation at the anode and cathode at different times (d). (e) Comparison between the amounts of experimental and theoretical gaseous products of H2 and O2 versus time. (f) Schematic diagram of seawater splitting by Stirling engine. (g) Diagrammatic sketch of the electricity generated by solar panels for seawater splitting.

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Controllable synthesis of a self-assembled ultralow Ru, Ni-doped Fe₂O₃ lily as a bifunctional electrocatalyst for large-current-density alkaline seawater electrolysis

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