Enhancing hydrogen electrocatalytic oxidation on Ni3N/MoO2 in-plane heterostructures in alkaline solution

doi:10.1016/S1872-2067(22)64126-3

Abstract

Abstract:

Nickel (Ni)-based materials act as one of the most promising candidates as platinum-group-metal-free (PGM-free) electrocatalysts for hydrogen oxidation reaction (HOR) in alkaline solution. Nevertheless, the electrocatalytic activity of pure Ni is significantly limited due to the sluggish kinetics under alkaline condition. To accelerate the kinetics, constructing heterostructures and nitride structures have been developed as two representative strategies. Here, we combined the two methods and presented a facile synthesis of the sheet-like Ni₃N/MoO₂ in-plane heterostructures for enhanced HOR in alkaline electrolytes. Relative to Ni or Ni₃N, the Ni₃N/MoO₂ in-plane heterostructures exhibited a significantly increased mass activity by 8.6-fold or 4.4-fold, respectively. Mechanistic studies revealed that the enhanced activity of Ni₃N/MoO₂ could be attributed to the weakened hydrogen adsorption and strengthened hydroxyl adsorption. This work provides a facile approach to design high-efficiency catalysts for hydrogen-oxidation catalysis and beyond.

Key words: Nickel nitride, In-plane heterostructures, Adsorption, Hydrogen oxidation reaction, Alkaline solution

Lulu An, Shaofeng Deng, Xuyun Guo, Xupo Liu, Tonghui Zhao, Ke Chen, Ye Zhu, Yuxi Fu, Xu Zhao, Deli Wang. Enhancing hydrogen electrocatalytic oxidation on Ni₃N/MoO₂ in-plane heterostructures in alkaline solution[J]. Chinese Journal of Catalysis, 2022, 43(12): 3154-3160.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64126-3

https://www.cjcatal.com/EN/Y2022/V43/I12/3154

Figures/Tables 5

Fig. 1. (a) Schematic illustration of the preparation of Ni3N/MoO2 in-plane heterostructures. SEM (b), TEM (c), HRTEM (d) images, and element mapping (e?i) of Ni3N/MoO2 in-plane heterostructures.

Fig. 2. (a) XRD patterns of Ni3N and Ni3N/MoO2 in-plane heterostructures; Ni 2p (b), N 1s (c) and Mo 3d (d) XPS spectra of Ni3N/MoO2 in-plane heterostructures.

Fig. 3. (a) HOR polarization curves of Ni3N/MoO2, Ni3N, MoO2, Ni and commercial Pt/C with a sweep rate of 2 mV s-1 in H2-saturated KOH solution of 0.1 mol L?1. (b) Polarization curves of Ni3N/MoO2 at varied rotation rate. The inset showed the Koutecky-Levich plot. (c) Polarization curves of Ni3N/MoO2 before and after CV. (d) HOR polarization curves of Ni3N/MoO2 and Pt/C with and without CO.

Fig. 4. (a) Micro-polarization regions of Ni, Ni3N, and Ni3N/MoO2 in-plane heterostructures. (b) Exchange current density and mass activity of Ni, Ni3N, and Ni3N/MoO2 in-plane heterostructures. (c) Tafel plots of the kinetic current densities on Ni3N/MoO2, Ni3N, and Ni in-plane heterostructures. (d) Comparison of the mass activity of various studied HOR catalysts.

Fig. 5. (a) CO stripping curves of Ni3N and Ni3N/MoO2 in KOH solution of 0.1 mol L?1 with a sweep rate of 20 mV s-1. (b) CV curves of Ni3N and Ni3N/MoO2 in H2 or N2-saturated 0.1 mol L?1 KOH, respectively. (c) Schematic illustration of the mechanism for enhanced HOR catalyzed by Ni3N/MoO2 in-plane heterostructures.

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Enhancing hydrogen electrocatalytic oxidation on Ni₃N/MoO₂ in-plane heterostructures in alkaline solution

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