Heterostructured NiSe2/MoSe2 electronic modulation for efficient electrocatalysis in urea assisted water splitting reaction

doi:10.1016/S1872-2067(23)64490-0

Abstract

Abstract:

Efficient heterogeneous catalysts play a very important role in the value-updated green hydrogen production from urea-containing wastewater. Herein, NiSe₂/MoSe₂ heterostructured catalyst with optimized interfacial electron redistribution and urea adsorption energies via a strong built-in electric field was demonstrated effective for the urea-assisted water splitting reactions. Efficient catalytic performance was found on NiSe₂/MoSe₂ hybrid microsphere owing to the combined merits such as the unique structure features, the strong synergetic coupling effects, the increased active sites, and the high amount of intrinsic Ni³⁺ species. Excellent urea oxidation activity was found to drive 10 mA cm^‒2 at the potential of 1.33 V when loaded on the glassy carbon electrode, and a cell voltage of 1.47 V was required in the NiSe₂/MoSe₂||Pt/C urea-water electrolyzer to drive 10 mA cm^‒2, about 220 mV less than that of water electrolysis, indicating a less energy consumption technique during the electrolysis. The spectroscopic and theoretical analysis revealed the effective synergy of the Ni-Se bond and Mo-Se bond that would be promising for efficient catalyst system construction.

Key words: Water electrolysis, Urea oxidation, Heterostructured catalyst, NiSe₂, MoSe₂

Chun Yin, Fulin Yang, Shuli Wang, Ligang Feng. Heterostructured NiSe₂/MoSe₂ electronic modulation for efficient electrocatalysis in urea assisted water splitting reaction[J]. Chinese Journal of Catalysis, 2023, 51: 225-236.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64490-0

https://www.cjcatal.com/EN/Y2023/V51/I8/225

Figures/Tables 5

Fig. 1. XRD patterns (a), TDOS (b), and PDOS (c) of NiSe2/MoSe2, NiSe2, and MoSe2 catalysts. (d) Electron density difference for NiSe2/MoSe2 (yellow: electron depletion and blue: electron accumulation). (e) Total electronic values of Mulliken for NiSe2/MoSe2 and NiSe2. (f) Adsorption energy of urea molecules on the surface of catalysts. XPS spectra of Ni 2p (g), Mo 3d (h), Se 3d (i) of catalysts.

Fig. 2. (a) SEM image of NiSe2/MoSe2. (b,c) TEM images of NiSe2/MoSe2. The high resolution TEM image (d), SAED pattern (e), energy dispersive X-ray spectroscopy (f), STEM (g) and elemental mapping images (g?l) of NiSe2/MoSe2.

Fig. 3. The LSV curves (a) and Tafel plots (b) for the NiSe2/MoSe2, NiSe2, MoSe2, and IrO2 samples. (c) Nyquist plots of NiSe2/MoSe2, NiSe2, and MoSe2 catalysts at 1.54 V. Inset: the equivalent circuit model for electrochemical impedance spectrum. (d) Scan-rate dependence of the current densities derived from double-layer capacitance measurements. (e) The LSV curves of NiSe2/MoSe2 before and after 1000 CV cycles stability test. Inset for the CA curves recorded at 1.54 V of NiSe2/MoSe2 for 10 h. (f) Specific activity polarization curves of NiSe2/MoSe2, NiSe2, and MoSe2.

Fig. 4. CV curves measured in 1 mol L?1 KOH solution (a) and in 1 mol L?1 KOH solution with 0.33 mol L?1 urea (b) for NiSe2/MoSe2, NiSe2, and MoSe2 catalysts at 10 mV s?1. (c) The corresponding Tafel slope of these catalysts. (d) Nyquist plots and fitting curves at 1.36 V. Inset: the equivalent circuit model for electrochemical impedance spectrum. (e) CA curves for urea oxidation at 1.39 V. (f) LSV curve of the water and urea electrolysis of NiSe2/MoSe2||Pt/C. Inset: Time-dependent current density curve for 10 h. (g) Free energy diagram of NiSe2 (210) and NiSe2 (210)/MoSe2 (100) for UOR.

Fig. 5. Morphology observed by TEM for NiSe2/MoSe2 after stability test. (a,b) TEM images. (c) HR-TEM image. (d) SAED pattern. (e) EDS pattern. (f?k) STEM and elemental mapping images. The XPS spectra comparison for NiSe2/MoSe2 catalyst before and after stability test: Ni 2p (l), Mo 3d (m), Se 3d (n).

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Heterostructured NiSe₂/MoSe₂ electronic modulation for efficient electrocatalysis in urea assisted water splitting reaction

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