High-valence metal-doped amorphous IrOx as active and stable electrocatalyst for acidic oxygen evolution reaction

doi:10.1016/S1872-2067(23)64517-6

Abstract

Abstract:

Proton-exchange membrane water electrolysis, particularly driven by renewable electricity, is a sustainable strategy for green hydrogen production. However, developing highly active and stable electrocatalysts to accelerate the oxygen evolution reaction (OER) remains challenging. Herein, we introduce an effective strategy for constructing high-valence metal-doped IrO_x with abundant oxygen vacancies, while simultaneously enhancing the catalytic activity and stability of the acidic OER. The synthesized Ta-doped IrO_x (350-Ta@IrO_x) exhibits ultramicroscopic nanoparticle morphology and abundant surface oxygen vacancies, enabling a rapid OER process with a low overpotential of 223 mV at 10 mA cm^-2 and 147.7 times higher mass activity (1207.4 A g_Ir^-1) than that of commercial IrO₂ at 1.55 V versus the reversible hydrogen electrode. More importantly, 350-Ta@IrO_x affords excellent stability with insignificant potential degradation after 500 h of electrolysis at 10 mA cm^-2, originating from the low operating potential and suppressed dissolution and oxidation of oxygen vacancy active sites via Ta doping. Density functional theory calculations suggest that Ta doping and oxygen defect engineering are effective in facilitating the nucleophilic attack of water molecules, thereby accelerating the rate-determining step toward high catalytic OER activity on Ta-doped IrO_x. We anticipate that this study will provide an effective method to obtain active and stable electrocatalysts via high-valence metal doping.

Key words: Acidic oxygen evolution reaction, High-valence metal doping, Iridium oxide, Oxygen defect, Electrocatalysis

Ning Zhang, Jiayi Du, Na Zhou, Depeng Wang, Di Bao, Haixia Zhong, Xinbo Zhang. High-valence metal-doped amorphous IrO_x as active and stable electrocatalyst for acidic oxygen evolution reaction[J]. Chinese Journal of Catalysis, 2023, 53: 134-142.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64517-6

https://www.cjcatal.com/EN/Y2023/V53/I10/134

Figures/Tables 4

Fig. 1. Morphology characterization of 350-Ta@IrOx. (a) TEM image; (b) HR-TEM image with lattice spacing; (c) SAED image; (d-g) Elemental mapping images.

Fig. 2. (a) XRD patterns of Ta@IrOx electrocatalysts and commercial IrO2. (b) Ir 4f XPS spectra of 350-Ta@IrOx. (c) Ta 4f XPS spectra of 350-Ta@IrOx. (d) O 1s XPS spectra of 350-Ta@IrOx, 400-Ta@IrOx, and 450-Ta@IrOx.

Fig. 3. (a) LSV curves of 350-Ta@IrOx, 400-Ta@IrOx, 450-Ta@IrOx, and commercial IrO2. (b) Tafel slope plots. (c) CP curves of 350-Ta@IrOx and 350-IrOx. (d) Comparisons of 350-Ta@IrOx with other representative acidic OER electrocatalysts. (e) Current retention of 350-Ta@IrOx and commercial IrO2 after the OER. (f) XPS spectra of 350-Ta@IrOx and 350-IrOx after the OER.

Fig. 4. (a) Four-step OER proceeding through the formation of *OH, *O, and *OOH on Ta-doped IrOx. (b) Predicted free energy profiles of acidic OER on Ta-doped IrOx (* denotes the active site of the catalyst).

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