溶剂热法制备Bi<sub>2</sub>O<sub>3</sub>/BiOI复合光催化材料及对四环素的降解应用

高艳林; 景红霞; 李龙祥; 王旭; 杨晓峰

doi:10.13801/j.cnki.fhclxb.20210513.001

溶剂热法制备Bi₂O₃/BiOI复合光催化材料及对四环素的降解应用

doi: 10.13801/j.cnki.fhclxb.20210513.001

中北大学　理学院，太原 030051

基金项目: 山西省自然科学基金(201901D111138)；山西省回国留学人员科研资助项目(2019)

详细信息

通讯作者:
景红霞，博士，副教授，研究生导师，研究方向为超细材料的制备及应用　E-mail: jhx820215@126.com

中图分类号: O643.36
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出版历程
- 收稿日期: 2021-03-01
- 修回日期: 2021-04-26
- 录用日期: 2021-05-06
- 网络出版日期: 2021-05-13
- 刊出日期: 2022-02-01

Preparation of Bi₂O₃/BiOI composite photocatalytic material by solvothermal method and its application to the degradation of tetracycline

School of Science, North University of China, Taiyuan 030051, China

摘要

摘要: 四环素作为一种广泛使用的抗生素，长期存在于水环境中难以自然降解，对生态环境和人类健康有很大危害。采用简单的室温搅拌法和溶剂热法制备了BiOI和Bi₂O₃/BiOI光催化剂，通过XRD、SEM、FTIR、UV-Vis DRS、PL和EIS等手段对材料的形貌和结构进行了表征，并考察了不同制备条件对Bi₂O₃/BiOI复合光催化材料在模拟太阳光下对四环素降解效果的影响。结果表明，当Bi₂O₃与BiOI的摩尔比为0.8∶1时，在pH=5、180℃下反应20 h得到的Bi₂O₃/BiOI复合光催化材料对四环素的降解效果最佳，在3 h内对四环素的降解率可达75%，其动力学速率常数分别是单一BiOI、Bi₂O₃的1.75倍和1.56倍。还提出了一种二元异质结光催化剂的催化机制用于解释提高的光催化活性。
- 溶剂热法 /
- Bi₂O₃/BiOI /
- 光催化 /
- 四环素 /
- 催化机制
Abstract: As a widely used antibiotic, tetracycline exists in water environment for a long time and is difficult to be degraded naturally, which does great harm to ecological environment and human health. BiOI and Bi₂O₃/BiOI photocatalysts were prepared by simple room temperature stirring method and solvothermal method. The morphology and structure of the materials were characterized by XRD, SEM, FTIR, UV-Vis, PL and EIS. The effects of different preparation conditions on the degradation of tetracycline by Bi₂O₃/BiOI composite photocatalytic material under simulated sunlight were investigated. The results show that when the molar ratio of Bi₂O₃to BiOI is 0.8∶1, the reaction pH is 5, the reaction temperature is 180℃, the reaction time is 20 h, the composite photocatalytic material has the best degradation effect on tetracycline, which can reach 75% in 3 h. And the kinetic rate constants are 1.75 times and 1.56 times of that of single BiOI and Bi₂O₃, respectively. A catalytic mechanism of binary heterojunction photocatalyst is proposed to explain the improved photocatalytic activity.
- solvothermal method /
- Bi₂O₃/BiOI /
- photocatalysis /
- tetracycline /
- catalytic mechanism

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图 1 不同光催化材料的XRD图谱

Figure 1. XRD patterns of different photocatalytic materials

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图 2 不同光催化材料的SEM图像

Figure 2. SEM images of different photocatalytic materials

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图 3 Bi₂O₃/BiOI复合光催化材料的FTIR图谱

Figure 3. FTIR spectra of Bi₂O₃/BiOI composite photocatalytic material

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图 4 不同光催化材料的紫外漫反射图谱

Figure 4. UV-Vis DRS of different photocatalytic materials

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图 5 不同光催化材料的禁带宽度

Figure 5. Band gaps of different photocatalytic materials

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图 6 不同光催化材料的荧光光谱图

Figure 6. Fluorescence spectroscopy of different photocatalytic materials

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图 7 不同光催化材料的阻抗图

Figure 7. Impedance diagrams of different photocatalytic materials

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图 8 不同摩尔比 (a)、反应温度 (b)、反应时间 (c) 及pH (d) 对Bi₂O₃/BiOI光催化材料性能的影响

Figure 8. Effects of different molar ratios (a), reaction temperature (b), reaction time (c) and pH (d) on the properties of Bi₂O₃/BiOI photocatalytic material

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图 9 模拟太阳光照射下不同光催化材料的降解曲线 (a) 及动力学曲线 (b)

Figure 9. Degradation curves (a) and kinetic curves (b) of different photocatalytic materials under simulated sunlight irradiation

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图 10 捕捉BiOI (a)、Bi₂O₃(b)、Bi₂O₃/BiOI (c) 中活性物种的柱状图

Figure 10. Histogram of captured active species in BiOI (a), Bi₂O₃ (b), and Bi₂O₃/ BiOI (c)

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图 11 Bi₂O₃/BiOI复合光催化材料的降解机制

Figure 11. Degradation mechanism of Bi₂O₃/BiOI composite photocatalytic material

TC—Tetracycline; E_g—Band gap

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参考文献(24)

[1]	YANG Wen, WANG Ying. Enhanced electron and mass transfer flow-through cell with C₃N₄-MoS₂ supported on three-dimensional graphene photoanode for the removal of antibiotic and antibacterial potencies in ampicillin wastewater[J]. Applied Catalysis B: Environmental,2021,282:119574. doi: 10.1016/j.apcatb.2020.119574
[2]	YU Yutang, WU Kun, XU Weicheng, et al. Adsorption-photocatalysis synergistic removal of contaminants under antibiotic and Cr(VI) coexistence environment using non-metal g-C₃N₄ based nanomaterial obtained by supramolecular self-assembly method[J]. Journal of Hazardous Materials,2021,404:124171. doi: 10.1016/j.jhazmat.2020.124171
[3]	LIU Shuyuan, RU Jiling, LIU Fanzhe. NiP/CuO composites: Electroless plating synthesis, antibiotic photodegradation and antibacterial properties[J]. Chemosphere,2021,267:129220. doi: 10.1016/j.chemosphere.2020.129220
[4]	ZHANG Hao, TANG Guogang, WAN Xiong, et al. High-efficiency all-solid-state Z-scheme Ag₃PO₄/g-C₃N₄/MoSe₂ photocatalyst with boosted visible-light photocatalytic performance for antibiotic elimination[J]. Applied Surface Science,2020,530:147234. doi: 10.1016/j.apsusc.2020.147234
[5]	ZHONG Shuang, WANG Xiaozhu, WANG Yu, et al. Preparation of Y³⁺-doped BiOCl photocatalyst and its enhancing effect on degradation of tetracycline hydrochloride wastewater[J]. Journal of Alloys and Compounds,2020,843:155598. doi: 10.1016/j.jallcom.2020.155598
[6]	ZHU M T, TONNI A K, YOU Y P, et al. Fabrication, characterization, and application of ternary magnetic recyclable Bi₂WO₆/BiOI@Fe₃O₄ composite for photodegradation of tetracycline in aqueous solutions[J]. Journal of Environmental Management,2020,270:110839.
[7]	JIANG Xueding, LAI Shufeng, XU Weicheng, et al. Novel ternary BiOI/g-C₃N₄/CeO₂catalysts for enhanced photocatalytic degradation of tetracycline under visible-light radiation via double charge transfer process[J]. Journal of Alloys and Compounds,2019,809:151804. doi: 10.1016/j.jallcom.2019.151804
[8]	YANG Yang, ZENG Zhuotong, ZHANG Chen, et al. Construction of iodine vacancy-rich BiOI/Ag@AgI Z-scheme heterojunction photocatalysts for visible-light-driven tetracycline degradation: Transformation pathways and mechanism insight[J]. Chemical Engineering Journal,2018,349:808-821. doi: 10.1016/j.cej.2018.05.093
[9]	GUO Siyao, LUO Huihua, LI Ying, et al. Structure-controlled three-dimensional BiOI/MoS₂ microspheres for boosting visible-light photocatalytic degradation of tetracycline[J]. Journal of Alloys and Compounds,2021,852:157026. doi: 10.1016/j.jallcom.2020.157026
[10]	KANDI Debasmita, BEHERA Arjun, SAHOO Srikant, et al. CdS QDs modified BiOI/Bi₂MoO₆ nanocomposite for degradation of quinolone and tetracycline types of antibiotics towards environmental remediation[J]. Separation and Purification Technology,2020,253:117523. doi: 10.1016/j.seppur.2020.117523
[11]	HUANG Liying, YANG Lei, LI Yeping, et al. p-n BiOI/Bi₃O₄Cl hybrid junction with enhanced photocatalytic performance in removing methyl orange, bisphenol A, tetracycline and Escherichia coli[J]. Applied Surface Science,2020,527:146748. doi: 10.1016/j.apsusc.2020.146748
[12]	CHEN Yongyang, LIU Yonggang, XIE Xin, et al. Synthesis flower-like BiVO₄/BiOI core/shell heterostructure photocatalyst for tetracycline degradation under visible-light irradiation[J]. Journal of Materials Science: Materials in Electronics,2019,30(10):9311-9321. doi: 10.1007/s10854-019-01261-9
[13]	YAN Qishe, WANG Peiying, GUO Yuan, et al. Constructing a novel hierarchical ZnMoO₄/BiOI heterojunction for efficient photocatalytic degradation of tetracycline[J]. Journal of Materials Science: Materials in Electronics,2019,30(20):19069-19076. doi: 10.1007/s10854-019-02264-2
[14]	HAO Rong, XIAO Xin, ZUO Xiaoxi, et al. Efficient adsorption and visible-light photocatalytic degradation of tetracycline hydrochloride using mesoporous BiOI microspheres[J]. Journal of Hazardous Materials,2012,209:137-145.
[15]	YUAN Ding, HUANG Liying, LI Yeping, et al. A novel AgI/BiOI/pg-C₃N₄ composite with enhanced photocatalytic activity for removing methylene orange, tetracycline and E. coli[J]. Dyes and Pigments,2020,177:108253. doi: 10.1016/j.dyepig.2020.108253
[16]	WANG Qi, SHI Xiaodong, LIU Enqin, et al. Facile synthesis of AgI/BiOI-Bi₂O₃ multi-heterojunctions with high visible light activity for Cr(VI) reduction[J]. Journal of Hazardous Materials,2016,317:8-16. doi: 10.1016/j.jhazmat.2016.05.044
[17]	CONG Yanqing, JI Yun, GE Yaohua, et al. Fabrication of 3D Bi₂O₃-BiOI heterojunction by a simple dipping method: Highly enhanced visible-light photoelectrocatalytic activity[J]. Chemical Engineering Journal,2017,307:572-582. doi: 10.1016/j.cej.2016.08.114
[18]	HAN Suiqi, LI Jia, YANG Kailun, et al. Fabrication of a β-Bi₂O₃/BiOI heterojunction and its efficient photocatalysis for organic dye removal[J]. Chinese Journal of Catalysis,2015,36(12):2119-2126.
[19]	CHAKRABORTY A K, GANGULI S, BERA S, et al. Preparation of CdS/BiOCl/Bi₂O₃double composite system for visible light active photocatalytic applications[J]. Journal of Photochemistry & Photobiology A: Chemistry,2018,364:159-168.
[20]	XIE Xin, WANG Shenbo, ZHANG Yongjiang, et al. Facile construction for new core-shell Z-scheme photocatalyst GO/AgI/Bi₂O₃ with enhanced visible-light photocatalytic activity[J]. Journal of Colloid and Interface Science,2021,581:148-158. doi: 10.1016/j.jcis.2020.07.128
[21]	LI Bo, NENGZI Lichao, GUO Ruonan, et al. Novel synthesis of Z-scheme α-Bi₂O₃/g-C₃N₄composite photocatalyst and its enhanced visible light photocatalytic performance: Influence of calcination temperature[J]. Chinese Chemical Letters,2020,31(10):2705-2711. doi: 10.1016/j.cclet.2020.04.026
[22]	LI Binrong, CHU Jinyu, LI Yi, et al. Preparation and performance of visible-light-driven Bi₂O₃/ZnS heterojunction functionalized porous CA membranes for effective degradation of Rhodamine B[J]. Physica Status Solidi A: Applications and Materials Science,2018,215(11):1701061.
[23]	WEI Zhiping, ZHENG Nan, DONG Xiaoli, et al. Green and controllable synthesis of one-dimensional Bi₂O₃/BiOI heterojunction for highly efficient visible-light-driven photocatalytic reduction of Cr(VI)[J]. Chemosphere,2020,257:127210.
[24]	LI Yongyu, WANG Jianshe, YAO Hongchang, et al. Chemical etching preparation of BiOI/Bi₂O₃ heterostructures with enhanced photocatalytic activities[J]. Catalysis Communications, 2011, 12(7): 660-664.