Large-current polarization-engineered FeOOH@NiOOH electrocatalyst with stable Fe sites for large-current oxygen evolution reaction

doi:10.1016/S1872-2067(24)60062-8

Abstract

Abstract:

NiFe-based (oxy)hydroxides are among the most efficient electrocatalysts for the oxygen evolution reaction (OER). However, significant Fe leakage during the OER results in unsatisfactory stability. Herein, a large-current (1.5 A cm⁻²) galvanostatic reconstruction was used to fabricate FeOOH@NiOOH (eFNO_L) with both fixed Fe sites and exposed high-index crystal facets (HIFs). Compared to FeNiOOH with low-index crystal facets, the phase-separated FeOOH@NiOOH showed a higher binding energy towards Fe, and the HIFs significantly improved the catalytic activity of FeOOH. The optimized eFNO_L catalyst exhibits ultralow overpotentials of 234 and 272 mV, yielding substantial current densities of 100 and 500 mA cm⁻², respectively, with a small Tafel slope of 35.2 mV dec⁻¹. Moreover, due to the stabilized Fe sites, its striking stability over 100 h at 500 mA cm⁻² with 1.5% decay outperforms most NiFe-based OER catalysts reported recently. This study provides an effective strategy for developing highly active and stable catalysts via large-current electrochemical reconstruction.

Key words: Oxygen evolution reaction, FeOOH@NiOOH, Large-current electrochemical, reconstruction, High-index crystal facet, Anchor of Fe site

Qingyun Lv, Weiwei Zhang, Zhipeng Long, Jiantao Wang, Xingli Zou, Wei Ren, Long Hou, Xionggang Lu, Yufeng Zhao, Xing Yu, Xi Li. Large-current polarization-engineered FeOOH@NiOOH electrocatalyst with stable Fe sites for large-current oxygen evolution reaction[J]. Chinese Journal of Catalysis, 2024, 62: 254-264.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60062-8

https://www.cjcatal.com/EN/Y2024/V62/I7/254

Figures/Tables 6

Fig. 1. (a) Schematic preparation of eFNOL. (b) Galvanostatic polarization voltage-time diagram at small (eFNOS) and large currents (eFNOL). (c) XRD spectra of eFNO and 5eFNO. (d) XRD spectra of eFNOL.

Fig. 2. (a) SEM image of eFNOL. (b) TEM image of eFNOL. (c) HRTEM image of 5eFNO. (d?f) HRTEM images of eFNOL. (g) Elemental mapping images of Fe, Ni, and O, and the overlap in eFNOL.

Fig. 3. (a) FTIR spectra of eFNOL, eFNOS, eFNO, and FNO. (b) Raman spectra of eFNOL, eFNOS, eFNO, and FNO. XPS spectra of Ni 2p (c) and Fe 2p (d) for eFNOL, eFNOS, 5eFNO, and eFNO. (e) Variation in the concentration of Fe and Ni ions in the electrolyte with time in the galvanostatic polarization processes at large current and small current. (f) Percentages of Ni, Fe, and O in eFNO, eFNOS, and eFNOL. (g) Schematic of the Fe2O3 to FeOOH transformation by galvanostatic polarization at large and small currents.

Fig. 4. OER activity of eFNO, 5eFNO, eFNOL, eFNOS, and RuO2/NF. (a) LSV polarization graphs; (b) Corresponding Tafel plots; (c) Related Cdl; (d) Nyquist plots corresponding to the LSV curves; (e) OER comparison between this work and other NiFe-based OER catalysts at 100 and 500 mA cm?2.

Fig. 5. (a) Overall water splitting stability tests of 5eFNO‖Pt, eFNOL‖Pt, and eFNO‖Pt for 100 h in 1 mol L?1 KOH at 25 °C. (b) The LSV polarization curves of eFNOL‖Pt before and after the stability test. (c) HRTEM image of eFNOL after the stability test. (d) Concentration of Fe ions in the electrolyte at 0, 5, 10, 20, 50, and 100 h during overall water splitting of 5eFNO‖Pt, eFNOL‖Pt, and eFNO‖Pt, respectively. (e) Percentages of Ni, Fe, and O in eFNO, 5eFNO, and eFNOL before and after the stability test. (f) Variations in the relative energy and corresponding crystal structure of FeNiOOH (101), FeOOH (420), and FeOOH (303) after losing an Fe site, respectively. (g) Stability comparisons of our OER catalyst with other catalysts reported in the literature. The x-axis represents the current, the y-axis represents the retention ratio, and the z-axis represents the measurement time.

Fig. 6. (a) Proposed OER mechanism at Fe sites of FeOOH (420). (b) Crystal structure diagram of FeOOH (304), FeOOH (420), and FeNiOOH (101). (c) Gibbs free energy diagrams of FeNiOOH (101), FeOOH (304), and FeOOH (420) for OER.

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