Ultralow Ru-doped NiMoO4@Ni3(PO4)2 core-shell nanostructures for improved overall water splitting

doi:10.1016/S1872-2067(24)60038-0

Abstract

Abstract:

The potential of sustainable hydrogen production technology through water splitting necessitates the rational design of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) bi-functional electrocatalysts. In this context, we initially synthesized and empirically evaluated ultralow Ru-doped NiMoO₄@Ni₃(PO₄)₂ core-shell nanostructures on nickel foam (Ru-NiMoO₄@Ni₃(PO₄)₂/NF). The hydrous NiMoO₄ nanopillars were hydrothermally grown on NF, followed by successive RuCl₃ etching and subsequent phosphorylation processes, leading to the final Ru-NiMoO₄@Ni₃(PO₄)₂/NF. The catalyst demonstrated impressive HER overpotential values of −14.8 and −57.1 mV at 10 and 100 mA cm^-2, respectively, with a Tafel slope of 35.8 mV dec^-1. For OER at 100 mA cm^-2, an overpotential of 259.7 mV was observed, with a Tafel slope of 21.6 mV dec^-1. The cell voltage required for overall water splitting was 1.43 V at 10 mA cm^-2 and 1.68 V at 100 mA cm^-2. Moreover, the catalyst exhibited superior stability for 150 h, emphasizing its practical utility for long-term applications. Subsequent density functional theory calculations aligned with these empirical findings, indicating a low water dissociation energy barrier (ΔG_b = 0.46 eV), near-zero free adsorption energy for HER (∆G_*H = 0.02 eV), and suitable free adsorption energy for OER (ΔG_*OOH − ΔG_*OH = 2.74 eV), alongside a high density of states near the Fermi level. These results, informed by both experimental evaluation and theoretical validation, highlight the potential of Ru-NiMoO₄@Ni₃(PO₄)₂/NF as a high-performance catalyst for water splitting, setting a solid foundation for advancements in sustainable energy technologies.

Key words: Electrocatalysis, Core-shell structure, Doping, Density functional theory, Hydrogen evolution reaction, Oxygen evolution reaction, Water splitting

Adel Al-Salihy, Ce Liang, Abdulwahab Salah, Abdel-Basit Al-Odayni, Ziang Lu, Mengxin Chen, Qianqian Liu, Ping Xu. Ultralow Ru-doped NiMoO₄@Ni₃(PO₄)₂ core-shell nanostructures for improved overall water splitting[J]. Chinese Journal of Catalysis, 2024, 60: 360-375.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60038-0

https://www.cjcatal.com/EN/Y2024/V60/I5/360

Figures/Tables 7

Fig. 1. (a) Schematic illustration of the preparation process of NiMoO4 nanopillars encapsulated with ultra-doping Ru and Ni3(PO4)2 sheath as integrated core-shell electrodes. Low and high-magnification SEM images for NiMoO4/NF (b,c) and Ru-NiMoO4@Ni3(PO4)2/NF (d,e). Structural characterization of Ru-NiMoO4@Ni3(PO4)2 core-shell: (f,g) TEM images; (h) HRTEM Image (inset is SAED pattern); (i) the corresponding FFT images and calculations; (j) HAADF-STEM images and the corresponding elemental mapping images for Ni, Mo, O, P, and Ru (inset is EDS line scan spectrum).

Fig. 2. (a) XRD pattern of Ru-NiMoO4@Ni3(PO4)2/NF. Raman spectrum (b) and FTIR spectra (c) for NiMoO4/NF, NiMoO4@Ni3(PO4)2/NF, and Ru-NiMoO4@Ni3(PO4)2/NF electrocatalysts.

Fig. 3. High-resolution XPS spectra for Full XPS spectrum (a), Ru 3p (b), P 2p (c) of Ru-NiMoO4@Ni3(PO4)2 electrocatalyst. Ni 2p (d), Mo 3d (e), and O 1s (f) of Ru-NiMoO4@Ni3(PO4)2, NiMoO4@Ni3(PO4)2, and NiMoO4 electrocatalysts.

Fig. 4. Electrocatalytic performance of various samples for HER in 1.0 mol/L KOH. (a) LSV curves after iR correction. (b) Overpotentials at 10 and 100 mA cm-2 current densities. (c) Tafel slopes. (d) Comparison of Ru-NiMoO4@Ni3(PO4)2/NF with reported HER electrocatalysts. (e) Electrochemical impedance spectroscopy, and the inset shows the equivalent circuit for the Nyquist plots fitting. Cdl (f) and multistep chronopotentiometric curve (g) obtained with Ru-NiMoO4@Ni3(PO4)2/NF electrode (without iR-correction). (h) Chronoamperometry curve of Ru-NiMoO4@Ni3(PO4)2/NF at overpotentials of ?57 mV in 1 mol L-1 KOH, and the inset shows the polarization curve of Ru-NiMoO4@Ni3(PO4)2/NF before and after stability test.

Fig. 5. Electrocatalytic performance of various samples for OER in 1.0 mol L-1 KOH. (a) LSV curves after iR correction. (b) Overpotentials at 100 and 300 mA cm-2 current densities. (c) Tafel slopes. (d) Comparison of Ru-NiMoO4@Ni3(PO4)2/NF with reported HER electrocatalysts. (e) Electrochemical impedance spectroscopy, and the inset shows the equivalent circuit for the Nyquist plots fitting. (f) Chronoamperometry curve of Ru-NiMoO4@Ni3(PO4)2/NF at overpotentials of 259.7 mV in 1 mol L-1 KOH, and the inset shows the polarization curve Ru-NiMoO4@Ni3(PO4)2/NF before and after stability test and before and after 3000 CV cycles.

Fig. 6. Electrocatalytic performance of Ru-NiMoO4@Ni3(PO4)2/NF||Ru-NiMoO4@Ni3(PO4)2/NF for overall water splitting in 1.0 mol L-1 KOH. (a) A Photograph and schematic illustration of an overall water splitting electrolyzer. (b) Polarization curve after iR correction. (c) A comparative against previously reported electrocatalysts. (d) A durability curve, obtained while operating at a constant current of 100 mA cm-2 without iR correction. Inset: Polarization curves before and after the stability test. (e) The faradaic efficiency for H2 and O2 evolution at several current values.

Fig. 7. DFT calculations. (a) Schematic models; (b) Free energy diagrams for HER; (c) Free energy diagram for OER; (d) Gibbs free energy profile for water dissociation on NiMoO4·nH2O, Ru-NiMoO4·nH2O, NiMoO4·nH2O@Ni3(PO4)2, and Ru-NiMoO4·nH2O @Ni3(PO4)2; DOS of NiMoO4·nH2O (e) and Ru-NiMoO4·nH2O (f); PDOS of NiMoO4·nH2O and Ni3(PO4)2 (g), and Ru-NiMoO4·nH2O and Ni3(PO4)2 (h).

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Ultralow Ru-doped NiMoO₄@Ni₃(PO₄)₂ core-shell nanostructures for improved overall water splitting

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