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微波水热合成花球状BiOCl光催化降解甲硝唑
罗伟, 冯晓青, 黄影, 谢宏杰, 宋雄伟, 徐梓淞, 黄闻宇
中国环境科学 ›› 2020, Vol. 40 ›› Issue (4) : 1545-1554.
PDF(1161 KB)
PDF(1161 KB)
微波水热合成花球状BiOCl光催化降解甲硝唑
Photocatalytic degradation of metronidazole using flower-like BiOCl prepared by microwave hydrothermal method
以五水硝酸铋，氯化钾，乙二醇和P123为原料，用微波水热合成法制备出具有花球状的BiOCl.通过优化微波功率，温度和微波保持时间3种因素，发现微波功率为600W，温度为120℃，保持时间为30min时制备的BiOCl在模拟太阳光下对甲硝唑的降解效果最为显著.利用XRD和SEM对制备的BiOCl进行表征，考察了BiOCl的晶体结构和表面特征.同时研究了BiOCl投加量，甲硝唑浓度及pH值对甲硝唑降解的影响.结果表明，当BiOCl的投加量为2g/L，甲硝唑的初始浓度为5mg/L，体系初始pH值为3时，BiOCl对甲硝唑的降解效果达到98.3%.通过自由基捕获剂实验，发现光催化降解甲硝唑反应中的主要活性物种为空穴（h+）和过氧自由基（·O2-）.
In this paper, BiOCl was prepared by microwave-assisted hydrothermal synthesis method using bismuth nitrate pentahydrate, potassium chloride, ethylene glycol and P123 as raw materials. Microwave power, temperature and microwave holding time were changed to determine the conditions of the BiOCl preparation for the best photocatalytic degradation of metronidazole. The optimal synthetic condition of BiOCl was determined to be 600W, 120℃ and 30 min, under which the synthetic product showed the best degradation on metronidazole under simulated sunlight. The prepared materials were characterized by XRD and SEM to investigate crystal structure and surface characteristics of BiOCl. Besides, the effect of reaction conditions such as catalyst dosage, metronidazole initial concentration and pH on the degradation of metronidazole were also investigated. At the condition of catalyst dosage 2.5g/L, metronidazole concentration 5mg/L and pH 3, the degradation efficiency of metronidazole reached to 98.3%. The capture experiment indicated the main active species wereholes (h+) and superoxide radical (·O2-) in the degradation of metronidazole.
bismuth oxychloride / metronidazole / microwave hydrothermal / photocatalytic
[1] 徐瑞岭,陈娟.甲硝唑的不良反应特点及其用药监护探讨[J]. 基层医学论坛, 2016,20(28):3912-3914. Xu R L, Chen J. Literature analysis of adverse drug reactions of Metronidazole and drug monitoring[J]. The Medical Forum, 2016, 20(28):3912-3914.
[2] 柴晴雯,吕艳,张周,等.Cu2O@ZnO复合光催化剂对难生物降解有机物的光降解[J]. 中国环境科学, 2019,39(7):2822-2830. Chai Q W, Lü Y, Zhang Z, et al. Photodegradation of refractory organic compounds by Cu2O@ZnO composite photocatalyst[J]. China Environmental Science, 2019,39(7):2822-2830.
[3] Ismail M, Wu Z, Zhang L H, et al. High-efficient synergy of piezocatalysis and photocatalysis in bismuth oxychloride nanomaterial for dye decomposition.[J]. Chemosphere, 2019,228:212-218.
[4] Song Z, Dong X L, Fang J D, et al. Improved photocatalytic degradation of perfluorooctanoic acid on oxygen vacancies-tunable bismuth oxychloride nanosheets prepared by a facile hydrolysis[J]. Journal of Hazardous Materials, 2019,377:371-380.
[5] Yao H Y, Li H P, Hu T X, et al. Solvent-Free Synthesis of Bismuth Oxychloride Microflower/Nanosheet Homojunctions for Photoactivity Enhancement[J]. Chem Cat Chem, 2018,10(17):3726-3735.
[6] Xiong J Y, Cheng G, Li G F, et al. Well-crystallized square-like 2D BiOCl nanoplates:mannitol-assisted hydrothermal synthesis and improved visible-light-driven photocatalytic performance[J]. RSC Advances, 2011,1(8):1542-1553.
[7] Bo S, Xue Y U, Liang W, et al. Enhanced visible light photocatalytic oxidative desulfurization by BiOBr-graphene composite[J]. Journal of Fuel Chemistry & Technology, 2016,44(9):1074-1081.
[8] 张可可.卤氧化铋及其复合物光催化剂的低温合成与性能研究[D]. 江苏:南京理工大学, 2016. Zhang K K. Synthesis of bismuth oxyhalides and their composites photocatalysts at low temperature and study of their properties[D]. Nanjing:Nanjing University of Science & technology, 2016.
[9] 陈颖,赵宇,李静,等.共模板法一步合成绣球状BiOCl/Br固溶体光催化剂[J]. 高等学校化学学报, 2017,38(11):2045-2052. Chen Y, Zhao Y, Li J, et al. Onestep synthesis of hydrangea-like BiOCl/Br solid solution photocatalyst with co-template method[J]. Chemical Journal of Chinese Universities, 2017,38(11):2045-2052.
[10] Gao Y, Wang L, Li Z, et al. Microwave-assisted synthesis of flower-like Ag-BiOCl nanocomposite with enhanced visible-light photocatalytic activity[J]. Materials Letters, 2014,136:295-297.
[11] Bijanzad K, Tadjarodi A, Khiavi M M, et al. Microwave-assisted synthesis of bismuth oxybromochloride nanoflakes for visible light photodegradation of pollutants[J]. Physica B Condensed Matter, 2015,475(4):14-20.
[12] 袁丹.苦草废弃生物质基磁性颗粒/成型多孔炭球的制备及吸附性能研究[D]. 广西:广西大学, 2018. Yuan D. Study on preparation and adsorption properties of magnetic particles/shaped porous carbon pellets derived from waste biomass of Vallisneria Natans[D]. Guangxi:Guangxi University, 2018.
[13] Hua Z L, Wan S G, Sun L, et al. Role of non-ion surfactants in three-dimensional ordered porous biomass carbon foam derived from the liquefied eucalyptus sawdust for metronidazole adsorption[J]. Journal of Chemical Technology and Biotechnology, 2018,93(10):3044-3055.
[14] 刘瑜.溴氧化铋的制备及光催化降解苯的性能研究[D]. 山东:山东大学, 2016. Liu Y. Synthesis process of BiOBr and its photocatalytic properties for benzene[D]. Shandong:Shandong University, 2016.
[15] He J, Wang J, Liu Y Y, et al. Microwave-assisted synthesis of BiOCl and its adsorption and photocatalytic activity[J]. Ceramics International, 2015,41(6):8028-8033.
[16] Gao X Y, Peng W, Tang G B, et al. Highly efficient and visible-light-driven BiOCl for photocatalytic degradation of carbamazepine[J]. Journal of Alloys and Compounds, 2018,757:455-465.
[17] Wang C Y, Zhang Y J, Wang W K, et al. Enhanced photocatalytic degradation of bisphenol A by Co-doped BiOCl nanosheets under visible light irradiation[J]. Applied Catalysis B:Environmental, 2018, 221:320-328.
[18] Sun Y Y, Li G Y, Wang W J, et al. Photocatalytic defluorination of perfluorooctanoic acid by surface defective BiOCl:Fast microwave solvothermal synthesis and photocatalytic mechanisms[J]. Journal of Environmental Sciences, 2019,84(10):69-79.
[19] Wang X Y, Liu X M, Liu G, et al. Rapid synthesis of BiOCl graded microspheres with highly exposed (110) facets and oxygen vacancies at room temperature to enhance visible light photocatalytic activity[J]. Catalysis Communications, 2019,130:105769.
[20] Song J, Mao C, Niu H, et al. Hierarchical structured bismuth oxychlorides:self-assembly from nanoplates to nanoflowers via a solvothermal route and their photocatalytic properties[J]. Cryst Eng Comm, 2010,12:3875-3881.
[21] Gao X Y, Zhang X C, Wang Y W, et al. Rapid synthesis of hierarchical BiOCl microspheres for efficient photocatalytic degradation of carbamazepine under simulated solar irradiation[J]. Chemical Engineering Journal, 2015,263:419-426.
[22] Li Y, Yao L, Xu D, et al. Enhanced UV-Vis-NIR activated photocatalytic activity from Fe3+-doped BiOBr:Yb3+/Er3+ upconversion nanoplates:synergistic effect and mechanism insight[J]. Inorg. Chem. Front., 2019,6:126-136.
[23] RiveraU J, Prados J G, Sanchez P M, et al. Removal of nitroimidazole antibiotics from aqueous solution by adsorption/bioadsorption on activated carbon[J]. Journal of Hazardous Materials, 2009,170(1):298-305.
[24] 毛晓明.新型BiOCl光催化剂的可控合成及性能强化研究[D]. 太原:太原理工大学, 2014. Mao X M. Study on the controlled synthesis of novel BiOCl photocatalysts and their enhanced performance[D]. Taiyuan:Taiyuan University of Technology, 2014.
[25] 张钱新,陈平,王枫亮,等.g-C3N4在可见光下协同PDS降解磺胺二甲嘧啶的机制研究[J]. 环境科学学报, 2017,37(10):3772-3779. Zhang Q X, Chen P, Wang F L, et al. Photocatalytic degradation mechanism of sulfamethazine using PDS/g-C3N4 under visible light irradiation[J]. Acta Scientiae Circumstantiae, 2017,37(10):3772-3779.
[26] 邓智瀚,刘国,谢志豪,等.PDS协同g-C3N4可见光催化降解水体中布洛芬[J]. 环境工程, 2019,37(3):67-74. Deng Z H, Liu G, Xie Z H, et al. Photocatalytic degradation of Ibuprofen in water by synergism of PDS and g-C3N4[J]. Environmental Engineering, 2019,37(3):67-74.
[27] 苏海英,王盈霏,王枫亮,等.g-C3N4/TiO2复合材料光催化降解布洛芬的机制[J]. 中国环境科学, 2017,37(1):195-202. Su H Y, Wang Y F, Wang F L, et al. Preparation of g-C3N4/TiO2 composites and the mechanism research of the photocatalysis degradation of ibuprofen[J]. China Environmental Science, 2017, 37(1):195-202.
[28] Chen P, Wang F, Chen Z F, et al. Study on the photocatalytic mechanism and detoxicity of gemfibrozil by a sunlight-driven TiO2/carbon dots photocatalyst:The significant roles of reactive oxygen species[J]. Applied Catalysis B:Environmental, 2017,204:250-25.
[29] Jia Z H, Li T, Zheng Z F, et al. The BiOCl/diatomite composites for rapid photocatalytic degradation of ciprofloxacin:Efficiency, toxicity evaluation, mechanisms and pathway[J]. Chemical Engineering Journal, 2020,380:122422.
[30] Ma Z Y, Li P H, Ye L Q, et al. Oxygen vacancies induced exciton dissociation of flexible BiOCl nanosheets foreffective photocatalytic CO2 conversion[J]. Journal of Materials Chemistry A, 2017,5:24995-25004.
[31] Li T, Zhang X C, Zhang C M, et al. Theoretical insights into photo-induced electron transfer at BiOX (X=F, Cl, Br, I) (001) surfaces and interfaces[J]. Physical Chemistry Chemical Physics, 2019,21:868-875.
[32] Mao X M, Li X L, Wang Y W, et al. KI/H2O2 assisted synthesis and the changed properties of BiOCl photocatalysts[J]. Chemical Engineering Journal, 2014,247:241-249.
[33] Gao X Y, Yang X X, Guo Q, et al. Enhanced photocatalytic performance of BiOCl for carbamazepine degradation by coupling H-ZSM-5 and modifying phosphate groups:Improved charge separation efficiency with high redox ability[J]. Journal of the Taiwan Institute of Chemical Engineers, 2019,(104):301-309.
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