Active non-bonding oxygen mediate lattice oxygen oxidation on NiFe2O4 achieving efficient and stable water oxidation

doi:10.1016/S1872-2067(24)60276-7

Abstract

Abstract:

The oxygen evolution reaction (OER) serves as a fundamental half-reaction in the electrolysis of water for hydrogen production, which is restricted by the sluggish OER reaction kinetics and unable to be practically applied. The traditional lattice oxygen oxidation mechanism (LOM) offers an advantageous route by circumventing the formation of M-OOH* in the adsorption evolution mechanism (AEM), thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M-O bond order. Fortunately, the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen, which could be activated by rational band structure design for direct O-O coupling, where the M-O bond maintains its initial bond order. Here, non-bonding oxygen was introduced into NiFe₂O₄ via annealing in an oxygen-deficient atmosphere. Then, in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons, thereby facilitating the transformation of the redox center from metal to oxygen. LOM based on non-bonding oxygen (LOM_NB) was successfully activated within NiFe₂O₄, exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm^-2 and excellent durability of stable operation for over 150 h. Additionally, catalysts featuring varying band structures were synthesized for comparative analysis, and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2p holes are critical prerequisites for triggering and sustaining the LOM_NB pathway in transition metal spinel oxides. These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.

Key words: Non-bonding oxygen, Lattice oxygen oxidation mechanism, Oxygen evolution reaction, NiFe₂O₄, Spinel oxide

Jiangyu Tang, Xiao Wang, Yunfa Wang, Min Shi, Peng Huo, Jianxiang Wu, Qiaoxia Li, Qunjie Xu. Active non-bonding oxygen mediate lattice oxygen oxidation on NiFe₂O₄ achieving efficient and stable water oxidation[J]. Chinese Journal of Catalysis, 2025, 72: 164-175.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60276-7

https://www.cjcatal.com/EN/Y2025/V72/I5/164

Figures/Tables 6

Scheme 1. Preparation process and catalytic mechanism of Ar-NFO-S.

Fig. 1. (a) SEM image of the Ar-NFO-S. (b-d) TEM image of Ar-NFO-S in different TEM mode. (e) HRTEM image of Ar-NFO-S. (f) Elemental mapping of Ni, Fe, O, S, and C in Ar-NFO-S. (g) XRD patterns of all catalysts. (h) Metal weight ratios of Air-NFO, Ar-NFO, and Ar-NFO-S.

Fig. 2. (a) Raman spectra of all samples. Ni 2p (b), Fe 2p (c), O 1s (d) XPS spectra of Ar-NFO-S, Ar-NFO, and Air-NFO. (e) EPR spectra of Ar-NFO-S, Ar-NFO, and Air-NFO. (f) Projected DOS of Ni (3d), Fe (3d), and O (2p). (g) Schematic energy bands of Air-NFO, Ar-NFO, and Ar-NFO-S in consideration of Mott-Hubbard splitting.

Fig. 3. (a) LSV curves (90% IR compensation) at a scan rate of 5 mV/s in O2 saturated 1 mol/L KOH electrolyte. Tafel plots (b) and Nyquist plots (c) of Ar-NFO-S, Ar-NFO, Air-NFO-S and Air-NFO. (d) TOF-j column chart of Ar-NFO-S, Ar-NFO and Air-NFO. (e) LSV curves of Ar-NFO-S before and after 2000 cycles from 1 to 2 V vs. RHE. (f) Chronoamperometric measurement on Ar-NFO-S catalyst at 1.435 mV vs. RHE producing constant current density ~10 mA/cm2 for 150 h in 1 mol/L KOH electrolyte. (g) The OER performance of Ar-NFO-S and other Ni-based catalysts recently reported (Table S5).

Fig. 4. (a) CV curve of Ar-NFO-S, Ar-NFO, and Air-NFO in alkaline electrolytes at a scan rate of 10 mV/s. (b) Bode plots for Ar-NFO-S, Ar-NFO, and Air-NFO at a potential of 1.3 V vs. RHE. (c) Bode plots for Ar-NFO-S, Ar-NFO and Air-NFO-S at different potentials vs. RHE during OER. (d) In-suit Raman spectra of Ar-NFO-S at different potential vs. RHE during OER. (e) OER specific activities of Ar-NFO-S, Ar-NFO, and Air-NFO at 1.5 (V vs. RHE) in different pH of KOH. (f) LSV curve of Ar-NFO-S and Ar-NFO in different resolution.

Fig. 5. (a) Proposed LOMNB mechanisms on NiFe2O4 with different configurations. (b) Free energies of OER steps via LOMNB mechanisms on NiFe2O4 with different configuration. (c) Free energies of OER steps via AEM mechanisms on different site including Feoct, Nioct and Nioct adjacent to the sulfate (Nioct-S) of NiFe2O4.

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Active non-bonding oxygen mediate lattice oxygen oxidation on NiFe₂O₄ achieving efficient and stable water oxidation

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