Selective Se doping of NiFe2O4 on an active NiOOH scaffold for efficient and robust water oxidation

doi:10.1016/S1872-2067(20)63739-1

Abstract

Abstract:

There remains a challenge in designing electrocatalysts for water oxidation to create highly efficient catalytic sites for the oxygen evolution reaction (OER) while maintaining their robustness at large outputs. Herein, an etching-assisted synthesis approach was developed to integrate highly active NiFe₂O₄ nanoparticles with a robust and active NiOOH scaffold directly on commercial stainless steel. A precise selenization strategy was then introduced to achieve selective Se doping of NiFe₂O₄ to further enhance its intrinsic OER activity while maintaining a three-dimensional NiOOH nanosheet array as a robust scaffold for prompt mass transfer and gas evolution. The resulting NiFe₂O_4‒_xSe_x/NiOOH electrode exhibited superior electrocatalytic activity with low overpotentials of 153 and 259 mV to deliver benchmark current densities of 10 and 500 mA cm ^-2, respectively. More importantly, the catalyst exhibited remarkable durability at a stable current output of 100 mA cm ^-2 for hundreds of hours. These findings may open up opportunities for exploring efficient and robust electrocatalysts for scalable hydrogen production with practical materials.

Key words: Water oxidation, Selective selenization, NiFe2O4, NiOOH, Heterostructure

Yuan Huang, Jian-Jun Wang, Yang Zou, Li-Wen Jiang, Xiao-Long Liu, Wen-Jie Jiang, Hong Liu, Jin-Song Hu. Selective Se doping of NiFe₂O₄ on an active NiOOH scaffold for efficient and robust water oxidation[J]. Chinese Journal of Catalysis, 2021, 42(8): 1395-1403.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63739-1

https://www.cjcatal.com/EN/Y2021/V42/I8/1395

Figures/Tables 5

Fig. 1. (a) Scheme for the preparation of NiFe2O4-xSex/NiOOH. XRD patterns (b) and Raman spectra (c). (I) NiFe2O4-xSex/NiOOH; (II) NiFe2O4/NiOOH; (III) stainless steel. High-resolution XPS spectra of NiFe2O4-xSex/NiOOH and NiFe2O4/NiOOH. (d) Fe 2p; (e) Ni 2p; (f) O 1s; (g) Se 3d.

Fig. 2. Typical SEM images of stainless steel (a), NiFe2O4/NiOOH (b), and NiFe2O4-xSex/NiOOH (c); (d) TEM image of NiFe2O4-xSex/NiOOH; (e) HRTEM image of the nanoparticle in (d); HRTEM image (f) and SAED pattern (g) of the nanosheet in (d); (h) STEM image and corresponding elemental mapping images of NiFe2O4-xSex/NiOOH.

Fig. 3. (a) LSV polarization curves of various catalysts for OER without iR-correction. The orange dashed line and the inset are LSV curves of NiFe2O4-xSex/NiOOH with iR-correction. (b) Corresponding Tafel plots. (c) Comparison of overpotentials and Tafel slopes of NiFe2O4-xSex/NiOOH with state-of-the-art analogs. (d) OER Faradaic efficiency of NiFe2O4-xSex/NiOOH. (e) Stability test of NiFe2O4-xSex/NiOOH for OER at different potentials. (f) Multi-chronoamperometric curves for NiFe2O4-xSex/NiOOH recorded at various overpotentials.

Fig. 4. Nyquist plots (the inset is the model of equivalent circuit) (a) and ECSA-normalized LSV curves (b) of NiFe2O4/NiOOH, NiFe2O4-xSex/ NiOOH, and RuO2/SS. Contact angle images of NiFe2O4/NiOOH (c) and NiFe2O4-xSex/NiOOH (d) at different contact times.

Fig. 5. (a) Structures of NiFe2O4 and Se-doped NiFe2O4. Fe atom (golden), Ni atom (gray), O atom (red), Se atom (green). (b) The free-energy landscape of NiFe2O4 and Se-doped NiFe2O4 for OER.

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Selective Se doping of NiFe₂O₄ on an active NiOOH scaffold for efficient and robust water oxidation

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