Z-scheme N-doped K4Nb6O17/g-C3N4 heterojunction with superior visible-light-driven photocatalytic activity for organic pollutant removal and hydrogen production

doi:10.1016/S1872-2067(20)63608-7

Abstract

Abstract:

A simple calcination method was employed to prepare a Z-scheme N-doped K₄Nb₆O₁₇/g-C₃N₄ (KCN) heterojunction photocatalyst, in which the electronic structure of K₄Nb₆O₁₇ was regulated by N-doping, and g-C₃N₄ was formed both on the surface and within the interlayer spaces of K₄Nb₆O₁₇. The KCN composite showed profoundly improved photocatalytic activity for both H₂ generation and RhB degradation compared to its counterparts. This improved performance was attributed to the synergistic effects of N-doping, which broadened its light harvesting ability, and heterojunction formation, which increased the charge separation rate. The relatively low BET specific surface area of the KCN composite had little effect on its photocatalytic activity. Based on ESR spectroscopy studies, •O₂^-, •OH, and h ⁺ are the main active species in the photocatalytic degradation of RhB. Thus, it is reasonable to propose a Z-scheme photocatalytic mechanism over the KCN composite, which exhibits the dual advantages of efficient charge separation and high redox ability. Our work provides a simple approach for constructing large-scale Z-scheme heterojunction photocatalysts with high photocatalytic performance.

Key words: Photocatalysis, K₄Nb₆O₁₇, g-C₃N₄, Z-scheme, Heterojunction

Chao Liu, Yue Feng, Zitong Han, Yao Sun, Xiaoqiu Wang, Qinfang Zhang, Zhigang Zou. Z-scheme N-doped K₄Nb₆O₁₇/g-C₃N₄ heterojunction with superior visible-light-driven photocatalytic activity for organic pollutant removal and hydrogen production[J]. Chinese Journal of Catalysis, 2021, 42(1): 164-174.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63608-7

https://www.cjcatal.com/EN/Y2021/V42/I1/164

Figures/Tables 9

Fig. 1. SEM images of (a) g-C3N4, (b) K4Nb6O17, and (c) the KCN composite. (d, e) TEM and (f, g) HRTEM images, and (h) EDS profile of the KCN composite. (i) STEM-HAADF image of the combined elements and (j-n) the distribution of the elements C/N/O/K/Nb on the KCN composite.

Fig. 2. (a) TG curves, (b) XRD patterns, and (c) UV-visible diffuse reflectance and (d) FT-IR spectra of the as-prepared samples.

Fig. 3. (a) XPS survey and XPS profiles of (b) Nb 3d, (c) O 1s, and (d) N 1s of the as-prepared samples.

Fig. 4. (a) Rate of H2 production on K4Nb6O17, Me-K4Nb6O17, g-C3N4, and KCN; (b) Cycling test of photocatalytic H2 production over the KCN composite under visible light. (Reaction conditions: 100 mg photocatalyst in 200 mL of an aqueous solution containing 10 vol% TEOA and 2 wt% Pt.)

Fig. 5. (a) Visible-light photocatalytic degradation rate of RhB solution over different samples. (b) UV-vis spectral changes. (c) TOC removal (relative to C0) and (d) photocatalytic degradation stability of RhB over KCN under visible-light irradiation.

Fig. 6. (a) PL spectra and (b) time-resolved PL decay spectra of the as-prepared samples.

Fig. 7. ESR spectra of a KCN dispersion in the dark and under visible light irradiation: (a) DMPO-?O2-, (b) DMPO-?OH, and (c) TEMPO-h+.

Fig. 8. (a) Transient photocurrent responses and (d) electrochemical impedance spectra of K4Nb6O17, Me-K4Nb6O17, g-C3N4, and the KCN composite.

Fig. 9. Schematic of the two possible photocatalytic mechanisms, i.e., the Z-scheme system and type-II heterojunction, for charge-transfer in the KCN composite under visible light. The energy levels of K4Nb6O17 and g-C3N4 in the KCN composite are referenced to the normal hydrogen electrode (NHE) at pH 7.

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Z-scheme N-doped K₄Nb₆O₁₇/g-C₃N₄ heterojunction with superior visible-light-driven photocatalytic activity for organic pollutant removal and hydrogen production

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