Mg-doped SrTaO2N as a visible-light-driven H2-evolution photocatalyst for accelerated Z-scheme overall water splitting

doi:10.1016/S1872-2067(24)60082-3

Abstract

Abstract:

Perovskite SrTaO₂N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting. However, the formation of defect states during thermal nitridation severely hinders the separation of charges, resulting in poor photocatalytic activity. In the present study, we successfully synthesize SrTaO₂N photocatalyst with low density of defect states, uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping. Some important parameters, such as the size of unit cell, the content of nitrogen, and microstructure, prove the successful doping of Mg. The defect-related carrier recombination has been significantly reduced by Mg doping, which effectively promotes the charge separation. Moreover, Mg doping induces a change of the band edge, which makes proton reduction have a stronger driving force. After modifying with the core/shell-structured Pt/Cr₂O₃ cocatalyst, the H₂ evolution activity of the optimized SrTaO₂N:Mg is 10 times that of the undoped SrTaO₂N, with an impressive apparent quantum yield of 1.51% at 420 nm. By coupling with Au-FeCoO_x modified BiVO₄ as an O₂-evolution photocatalyst and [Fe(CN)₆]³⁻/[Fe(CN)₆]⁴⁻ as the redox couple, a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36% at 420 nm. This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.

Key words: Photocatalytic overall water splitting, SrTaO₂N photocatalyst, Mg doping, Defect density, Cocatalyst

Jun Xu, Ying Luo, Qiaoqi Guo, Wenzheng Sun, Shanshan Chen, Zheng Wang, Hong He. Mg-doped SrTaO₂N as a visible-light-driven H₂-evolution photocatalyst for accelerated Z-scheme overall water splitting[J]. Chinese Journal of Catalysis, 2024, 65: 70-78.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60082-3

https://www.cjcatal.com/EN/Y2024/V65/I10/70

Figures/Tables 6

Fig. 1. (a) XRD patterns of Mg-doped SrTaO2N samples with various Sr/Ta ratios (Mg/Ta = 0.1). (b) SrTaO2N:Mg using the I4/mcm space group (the refinement converges with low factor values, Rp = 7.25%, Rwp = 9.45% and χ2 = 1.58); the inserted image illustrate the schematics of the refined crystal structures. (c) UV-vis DRS of SrTaO2N:Mg and SrTaO2N. (d) Mg 1s XPS spectra of SrTaO2N:Mg and SrTaO2N. (e) Ta 4f XPS spectra of SrTaO2N:Mg and SrTaO2N.

Fig. 2. SEM images of SrTaO2N (a) and SrTaO2N:Mg (b). TEM image (c) and HRTEM image (d) of SrTaO2N:Mg.

Fig. 3. (a) The rates of H2-evolution activity for Mg-doped SrTaO2N samples with different Mg/Ta ratios at Sr/Ta = 1.1. Conditions: 50 mg Pt/Cr2O3-loaded Mg-doped SrTaO2N (Pt: 0.7%, Cr: 1.05%), 100 mL of 25 mmol L-1 sodium potassium buffer solution (pH = 6.0) containing K4[Fe(CN)6] (10 mmol L-1), 300 W xenon lamp equipped with a cut-off filter (λ ≥ 420 nm), Pyrex top-irradiation type. (b) H2 evolution rates of the SrTaO2N:Mg as a function of the cut-off wavelength of the incident light. Conditions: 50 mg Pt/Cr2O3-loaded SrTaO2N:Mg (Pt: 0.7%, Cr: 1.05%), 100 mL 25 mmol L-1 sodium potassium buffer solution (pH 6.0) containing K4[Fe(CN)6] (10 mmol L-1), 300 W Xenon lamp equipped with a various of band-pass filters.

Fig. 4. (a) M-S plots of SrTaO2N:Mg and SrTaO2N electrodes. Photocurrent under visible light irradiation (λ ≥ 420 nm) (b) and EIS Nyquist plots (c) of SrTaO2N:Mg and SrTaO2N samples. (d) TRPL decay spectra of SrTaO2N:Mg and SrTaO2N samples.

Table 1 Fitted parameters from the TRPL decay of SrTaO2N and SrTaO2N:Mg samples.

Sample	τ₁ (ns)	A₁	τ₂ (ns)	A₂	<τ> (ns)
SrTaO₂N	0.91	95.9%	5.08	4.1%	1.71
SrTaO₂N:Mg	1.27	77.1%	5.15	22.9%	3.39

Fig. 5. (a) The evolution rates of H2 and O2 during Z-scheme OWS reaction using Mg-doped SrTaO2N samples with various Sr/Ta ratios (Mg/Ta = 0.1) as HEPs. (b) Time courses of gas evolution during Z-scheme water splitting reaction using Pt/Cr2O3-loaded Mg-doped SrTaO2N as an HEP, Au-FeCoOx loaded BiVO4(/BiVO4) as an OEP, and [Fe(CN)6]3-/[Fe(CN)6]4- as the redox couple. Conditions: 50 mg Pt/Cr2O3-loaded SrTaO2N:Mg (Pt: 0.7%, Cr: 1.05%), 50 mg Au-FeCoOx loaded BiVO4, 100 mL of 25 mmol L-1 sodium potassium buffer solution (pH = 6.0) containing K4[Fe(CN)6] (10 mmol L-1), 300 W xenon lamp equipped with a cut-off filter (λ ≥ 420 nm), Pyrex top-irradiation type. (c) Schematic representation of Z-scheme process in the SrTaO2N:Mg-[Fe(CN)6]3-/[Fe(CN)6]4--BiVO4 system.

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Mg-doped SrTaO₂N as a visible-light-driven H₂-evolution photocatalyst for accelerated Z-scheme overall water splitting

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