ZrO2 modification of homogeneous nitrogen-doped oxide MgTa2O6-xNx for promoted photocatalytic water splitting

doi:10.1016/S1872-2067(23)64534-6

Abstract

Abstract:

Homogeneous nitrogen-doped oxides are of wide visible light utilization for promising photocatalytic water splitting to produce hydrogen, but currently the poor charge separation severely limits their photocatalytic performances. In this work, a homogeneous nitrogen-doped tunneled oxide of MgTa₂O_6-_xN_x with an absorption edge of 570 nm was selected as a prototype to investigate the influence of ZrO₂ modification on the charge separation as well as photocatalytic performance. It is interesting to observe that the formation of the reduced tantalum species, regarded as recombination centers, in the MgTa₂O_6-_xN_x sample could be effectively inhibited via the surface passivation with ZrO₂ nanoparticles, based on which the photocatalytic water reduction and oxidation half-reaction activities could be remarkably promoted. Together with modification of the deposited Pt cocatalyst, the optimized H₂ evolution rate over Pt-ZrO₂/MgTa₂O_6-_xN_x (Zr/Ta = 0.10) photocatalyst was almost 4.5 times as high as that of the pristine Pt-MgTa₂O_6-_xN_x sample free of ZrO₂ modification, whose apparent quantum yield at 420 nm (± 15 nm) achieved herein was superior to those of other reported homogeneous nitrogen-doped photocatalysts. The improved charge separation probably attributes to the introduction of Zr-O-Ta bond after ZrO₂ modification, which is helpful to stabilize the tantalum species at more cationic state and inhibit the formation of the reduced tantalum species. This work extends the application territory of ZrO₂ modification to the homogeneous nitrogen-doped oxide photocatalysts, and demonstrates its feasibility and effectiveness for remarkably enhanced photocatalytic water splitting performance.

Key words: MgTa₂O_6-_xN_x, Nitrogen doping, Photocatalyst, Water splitting, ZrO₂ modification

Ningning Wang, Shuo Wang, Can Li, Chenyang Li, Chunjiang Liu, Shanshan Chen, Fuxiang Zhang. ZrO₂ modification of homogeneous nitrogen-doped oxide MgTa₂O_6-_xN_x for promoted photocatalytic water splitting[J]. Chinese Journal of Catalysis, 2023, 54: 220-228.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64534-6

https://www.cjcatal.com/EN/Y2023/V54/I11/220

Figures/Tables 5

Fig. 1. Structural characterizations of ZrO2/MgTa2O6-xNx samples with different molar ratios of Zr/Ta. (a) Crystalline structure of MgTa2O6. (b) XRD patterns. (c) Enlarged XRD patterns.

Fig. 2. (a) UV-vis DRS of ZrO2/MgTa2O6-xNx samples with different molar ratios of Zr/Ta. (b) Ta 4f XPS of MgTa2O6-xNx (i) and ZrO2/MgTa2O6-xNx (ii) samples. Herein, the molar ratio of Zr/Ta was 0.10 for the ZrO2/MgTa2O6-xNx sample.

Fig. 3. Microscopy characterization of ZrO2/MgTa2O6-xNx sample with a Zr/Ta molar ratio of 0.10. (a,b) SEM images. (c) STEM image. (d-f) EDS elemental mapping images. (g,h) HRTEM images. Herein, elements of Ta (d), Zr (e), and a superimposition of both elements (f) were showed in the EDS elemental mapping images.

Fig. 4. Photocatalytic H2 (a) and O2 (b) evolution rates of ZrO2/MgTa2O6-xNx samples with different molar ratios of Zr/Ta. Reaction conditions: photocatalyst (0.1 g); ascorbic acid aqueous solution (10 mmol/L, 100 mL); 300 W Xe lamp with a cutoff filter (λ ≥ 420 nm) for (a). Photocatalyst (0.1 g); AgNO3 aqueous solution (50 mmol/L, 100 mL); La2O3 (0.1 g); 300 W Xe lamp with a cutoff filter (λ ≥ 420 nm) for (b). Herein, 0.2 wt% Pt or 1.0 wt% CoOx was loaded on the photocatalyst for H2 or O2 evolution reaction, respectively.

Fig. 5. Analysis of the roles of ZrO2 modification on the MgTa2O6-xNx sample. (a) PL emission spectra. (b,c) Schematic illustration. Herein, 0.2 wt% Pt was deposited, and the molar ratio of Zr/Ta was 0.10 for the ZrO2/MgTa2O6-xNx sample.

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ZrO₂ modification of homogeneous nitrogen-doped oxide MgTa₂O_6-_xN_x for promoted photocatalytic water splitting

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