Preparation of g-C3N4/Ag/BiOBr Composite and Photocatalytic Reduction of Nitrate

doi:10.11901/1005.3093.2022.627

Chinese Journal of Materials Research

2023, Vol. 37

Issue (10): 781-790 DOI: 10.11901/1005.3093.2022.627

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Preparation of g-C₃N₄/Ag/BiOBr Composite and Photocatalytic Reduction of Nitrate

LIU Zhihua¹^,³^,⁴(

), YUE Yuanchao², QIU Yifan², BU Xiang¹^,³^,⁴, YANG Tao¹^,³^,⁴

^1.School of Hydraulic and Environmental Engineering, Changsha University of Science & Technology, Changsha 410114, China
^2.School of Chemistry and Chemical Engineering, Changsha University of Science & Technology, Changsha 410114, China
^3.Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province, Changsha 410114, China
^4.Engineering and Technical Center of Hunan Provincial Environmental Protection for River-Lake Dredging Pollution Control, Changsha 410114, China

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LIU Zhihua, YUE Yuanchao, QIU Yifan, BU Xiang, YANG Tao. Preparation of g-C₃N₄/Ag/BiOBr Composite and Photocatalytic Reduction of Nitrate. Chinese Journal of Materials Research, 2023, 37(10): 781-790.

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Abstract

Nitrate as one of the water pollutants is one of the major environmental problems. Photocatalytic reduction of nitrate nitrogen has attracted a lot of attention because of its high efficiency and environmental friendliness. The g-C₃N₄/Ag/BiOBr composite photocatalyst was prepared by high temperature calcination, reaction synthesis and photoreduction. The photocatalysts were characterized by SEM, XRD, EPMA、FT-IR, XPS and UV-vis, and the reduction effect of the composite on nitrate nitrogen (50 mg/L) under the irradiation of metal halide lamp was studied. The results showed that when 1g/L g-C₃N₄/Ag/BiOBr catalyst was used, the nitrate concentration was 2.4 mg/L, and the removal rate was 95.2% after 180 min photoreaction. Compared with g-C₃N₄, BiOBr and g-C₃N₄/BiOBr photocatalysts, the removal rates increased by 38.8%, 34.6% and 13.1%, respectively. Nitrogen was the main product in the photocatalytic conversion of nitrate nitrogen. The proportion of N₂ in the main products of nitrate nitrogen photocatalyzed by g-C₃N₄/Ag/BiOBr was the highest (88.0%), and the selectivity of nitrogen was 92.4%. Ag can be used as an electron trapping agent to effectively reduce the recombination of electron-hole pairs in photocatalytic materials. Under the action of silver, the photogenerated electrons of BiOBr are transferred to the valence band of g-C₃N₄ by silver elemental material, forming a Z-type composite photocatalytic structure. Nitrate nitrogen can be directly oxidized by the composite photocatalyst, and the hole scavenger formic acid can be converted into a strong oxidizing substance (COO.-) under the action of the composite hole, which can further reduce nitrate nitrogen.

Key words: inorganic non-metallic materials g-C₃N₄/Ag/BiOBr nitrate nitrogen composite photocatalysis nitrogen selectivity

Received: 25 November 2022

ZTFLH:

O643

Fund: Outstanding Youth Program of Hunan Education Department(19B040);Young Teacher Development Program of Changsha University of Science and Technology(2019QJCZ038);Postgraduate Practice Innovation Program of Changsha University of Science and Technology(SJCX202189)

Corresponding Authors: LIU Zhihua, Tel: 13574872739, E-mail: liuzhihua@csust.edu.cn

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https://www.cjmr.org/EN/10.11901/1005.3093.2022.627 OR https://www.cjmr.org/EN/Y2023/V37/I10/781

Fig.1 XRD patterns of the different photocatalyst

Fig.2 XPS analysis of BiOBr, C₃N₄ and C₃N₄-Ag-BiOBr (a) survey spectrum, (b) Bi4f, (c) Br3d, (d) C1s, (e) N1s, (f) O1s, (g) Ag3d

Fig.3 FT-IR analysis of the different photocatalyst

Fig.4 SEM images of BiOBr and Ag/BiOBr (a) g-C₃N₄, (b) BiOBr, (c) g-C₃N₄/BiOBr, (d) Ag/g-C₃N₄, (e) Ag/BiOBr, (f) g-C₃N₄/Ag/BiOBr

Fig.5 Element mapping of g-C₃N₄/Ag/BiOBr

Fig.6 UV-vis diffuse reflectance spectra of the different photocatalyst

Fig.7 Influence of the different photocatalyst on nitrate reduction process

Fig.8 Effect of the different photocatalyst on nitrate reduction and its products

Photocatalyst	Hole scavenger	Light source	R_N/%	S $N 2$ /%	Ref.
g-C₃N₄/Ag/BiOBr	Formic acid	Halide lamp	95.2	92.4	This work
Ag/TiO₂	Formic acid	Xe lamp	95	90	[48]
Au/TiO₂	Oxalic acid	High-pressure Hg lamp	44	49.9	[49]
0.5TiO₂/Ti₃C₂/g-C₃N₄	Formic acid	High-pressure Hg lamp	93.3	96.62	[29]
Fe-LiNbO₃	Formic acid	High-pressure Hg lamp	90	88	[50]
ZnSe/BiVO₄	Formic acid	High-pressure Hg lamp	89.84	91.03	[14]
NH₂-MIL-101(Fe)/BiVO₄	Formic acid	High-pressure Hg lamp	94.8	93.5	[51]
Ag/SiO₂@cTiO₂	Formic acid	High-pressure Hg lamp	95.8	93.6	[22]

Table 1 Photocatalytic reduction of nitrate in this work and previous literature studies

Fig.9 Photoreduction mechanism of g-C₃N₄/Ag/BiOBr photocatalytic materials

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