Highly efficient single-crystalline NaNb1-XTaXO3 (X = 0.125) wires: The synergistic effect of tantalum-doping and morphology on photocatalytic hydrogen evolution

doi:10.1016/j.jmst.2020.05.006

Abstract

Abstract:

For the first time in this work, we manage to synthesize single-crystalline NaNb_0.875Ta_0.125O₃ wires by combining the advantages of one-dimensional (1D) nanostructure and heteroatom doping strategy. Careful Ta doping was performed to figure out the correlation between morphological and structural evolution as well as the photocatalytic performance towards H₂ generation. It was found that, the as-prepared NaNb_0.875Ta_0.125O₃ wires presented a highest and stable photocatalytic performance, which was appropriately 41 and 2 folds higher than that of bare NaTaO₃ and NaNbO₃. The optical activity was mainly ascribed to the synergistic effect between appropriate Ta doping and perfect 1D wire-like morphology, which resulted in fewer defects, improved charge transfer efficiency and higher reduction capability of electrons. On the other hand, a possible photocatalytic mechanism of photocatalytic H₂ production was proposed in detail. This work creates a new perspective into designing multi-component materials and understanding the mechanism of H₂ evolution, which offers new opportunities for solar-energy conversion.

Key words: NaNb_0.875Ta_0.125O₃ wires Single crystal, Ta-doping effect, Photocatalytic H₂ production Mechanism

Qianqian Liu, Quan Zhang, Lu Zhang, Wei-Lin Dai. Highly efficient single-crystalline NaNb_1-_XTa_XO₃ (X = 0.125) wires: The synergistic effect of tantalum-doping and morphology on photocatalytic hydrogen evolution[J]. J. Mater. Sci. Technol., 2020, 54: 20-30.

Figures/Tables 12

Fig. 1. XRD patterns of NaNb1-XTaXO3 samples: (a) the whole patterns; (b) the patterns of certain angle.

Fig. 2. SEM images of NaNb0.875Ta0.125O3 (a, b), NaNb0.75Ta0.25O3 (c) and NaNb0.5Ta0.5O3 (d).

Fig. 3. TEM image of NaNb0.875Ta0.125O3 (a) and the corresponding elemental mapping results (b); the HRTEM image (c), SAED (d) and EDS pattern (e) of NaNb0.875Ta0.125O3.

Fig. 4. EPR spectrum at 103 K (a) and crystal structure of NaNb0.875Ta0.125O3 ( NbO6 unit, TaO6 unit) (b).

Fig. 5. FT-IR spectra of NaNb1-XTaXO3 samples: (a) the survey spectra; (b) the spectra of certain angle.

Fig. 6. Raman spectra of NaNb1-XTaXO3 samples: (a) the survey spectra; (b) the spectra of certain angle.

Fig. 7. The survey XPS spectra of NaNb1-XTaXO3 (a) and the XPS spectra of NaNb1-XTaXO3 in the Nb 3d (b) and Ta 4f (c) regions.

Fig. 8. UV-vis diffuse-reflectance spectra of different NaNb1-XTaXO3 photocatalysts (a) and the plot of (ahν)n vs. photon energy (hν) of NaNbO3 (b), NaTaO3 (c).

Fig. 9. Photocatalytic H2 production under sunlight irradiation (a, b) and the H2 production rates of various photocatalysts (error bars represent the standard deviation for three parallel experiments) (c).

Fig. 10. Recyclability of NaNb0.875Ta0.125O3 for the photocatalytic H2 production.

Fig. 11. Emission photoluminescence (PL) spectra (a), photocurrent (b), electrochemical impedance spectra (c) and time-resolved PL decay curves (d) of pure NaNbO3 and NaNb0.875Ta0.125O3.

Scheme 1. Schematic illustration of the mechanism of NaNb0.875Ta0.125O3 during photocatalytic H2 production.

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Highly efficient single-crystalline NaNb_1-_XTa_XO₃ (X = 0.125) wires: The synergistic effect of tantalum-doping and morphology on photocatalytic hydrogen evolution

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