Study on visible light photocatalytic degradation of dibutyl phthalate in water

doi:10.3969/j.issn.1000-1565.2022.05.005

Abstract

Abstract: The composite material g-C₃N₄/Bi₄O₅I₂ was synthesized and characterized. The influencing factors of photocatalytic degradation of dibutyl phthalate(DBP)in water under visible light irradiation using the as-synthesized catalyst were studied, including catalyst dosage, initial solution concentration, pH and common anion Cl^-, NO^-₃ and SO^2-₄ in water. Through the analysis of degradation products, the possible degradation mechanism was proposed. The results showed that the optimum dosage of g-C₃N₄/Bi₄O₅I₂ was 0.6 g/L. The higher the initial concentration in the study range, the lower the degradation rate. When the solution was neutral, the photocatalytic degradation effect of DBP in water was the best. Cl^-, NO^-₃ and SO^2-₄ all inhibited the photocatalytic degradation to a certain extent. Through the analysis of the degradation products after the reaction, it is speculated that the side chain of DBP breaks first under the attack of active substances, and then continues to degrade into small molecular substances. The research results have important practical significance and reference value for the removal of phthalates in water environment. - DOI:10.3969/j.issn.1000-1565.2022.05.005可见光催化降解水中邻苯二甲酸二丁酯雷源¹,刘桂随²,朱爱雪²,李牧原²,刘芃岩¹(1.河北大学生态环境学院(筹),河北保定 071002;2.河北大学化学与环境科学学院,河北保定 071002)摘要:合成了复合材料g-C₃N₄/Bi₄O₅I₂,并进行了表征分析,以其为催化剂,研究了可见光照射下,水中邻苯二甲酸二丁酯(DBP)光催化降解的影响因素:催化剂投加量、溶液初始浓度、pH及水中常见阴离子Cl^-、NO^-₃和SO^2-₄等,并通过对降解产物的分析,提出了可能的降解机理. 结果表明:g-C₃N₄/Bi₄O₅I₂的最佳投加量为0.6 g/L;在研究范围内初始浓度越高,降解率越低;当溶液为中性时,对水中DBP的光催化降解效果最好;Cl^-、NO^-₃和SO^2-₄都对光催化降解产生了一定的抑制作用. 通过对反应后降解产物的分析,推测DBP是在活性物质的攻击下,侧链先发生断裂,再继续降解为小分子物质. 研究结果对水环境中邻苯二甲酸酯类的去除具有重要的实际意义和参考价值. 关键词:可见光;邻苯二甲酸二丁酯;光催化降解;g-C₃N₄/Bi₄O₅I₂中图分类号:X703 文献标志码:A 文章编号:1000-1565(2022)05-0474-09Study on visible light photocatalytic degradation of dibutyl phthalate in water LEI Yuan¹, LIU Guisui², ZHU Aixue², LI Muyuan², LIU Pengyan¹(1. School of Eco-Environment, Hebei University, Baoding 071002,China; 2. College of Chemistry and Environmental Science, Hebei University, Baoding 071002,China)Abstract: The composite material g-C₃N₄/Bi₄O₅I₂ was synthesized and characterized. The influencing factors of photocatalytic degradation of dibutyl phthalate(DBP)in water under visible light irradiation using the as-synthesized catalyst were studied, including catalyst dosage, initial solution concentration, pH and common anion Cl^-, NO^-₃ and SO^2-₄ in water. Through the analysis of degradation products, the possible degradation mechanism was proposed. The results showed that the optimum dosage of g-C₃N₄/Bi₄O₅I₂ was 0.6 g/L. The higher the initial concentration in the study range, the lower the degradation rate. When the solution was neutral, the photocatalytic degradation effect of DBP in water was the best. Cl^-, NO^-₃ and SO^2-₄ all inhibited the photocatalytic degradation to a certain extent. Through the analysis of the degradation products after the reaction, it is speculated that the side chain of DBP breaks first under the attack of active substances, and then continues to degrade into small molecular substances. The research results have important practical significance and reference value for the removal of phthalates in water environment. - 收稿日期:2021-05-15 基金项目:国家自然科学基金资助项目(21377033);河北省自然科学基金资助项目(B2021201031) 第一作者:雷源(1997—),女,河北邢台人,河北大学在读硕士研究生,主要从事环境污染化学方向研究.E-mail:2317535846@qq.com 通信作者:刘芃岩(1964—),女,河北保定人,河北大学教授,博士生导师,主要从事环境中典型污染物的生成降解与迁移转化研究.E-mail:hbupyliu@163.com第5期雷源等:可见光催化降解水中邻苯二甲酸二丁酯

Key words: visible light, dibutyl phthalate, photocatalytic degradation, g-C₃N₄/Bi₄O₅I₂

CLC Number:

X703

LEI Yuan, LIU Guisui, ZHU Aixue, LI Muyuan, LIU Pengyan. Study on visible light photocatalytic degradation of dibutyl phthalate in water[J]. Journal of Hebei University(Natural Science Edition), 2022, 42(5): 474-482.

References

[1] ZENG H H, LI X Q, HAO W L, et al. Determination of phthalate esters in airborne particulates by heterogeneous photo-Fenton catalyzed aromatic hydroxylation fluorimetry[J]. Journal of Hazardous Materials, 2017, 324(Pt B): 250-257. DOI:10.1016/j.jhazmat.2016.10.055.
[2] XU Y, LIU X, ZHAO J, et al. An efficient phthalate ester-degrading Bacillus subtilis:Degradation kinetics, metabolic pathway, and catalytic mechanism of the key enzyme[J]. Environmental Pollution, 2021, 273: 116461. DOI:10.1016/j.envpol.2021.116461.
[3] DU H, HU R W, ZHAO H M, et al. Mechanistic insight into esterase-catalyzed hydrolysis of phthalate esters(PAEs)based on integrated multi-spectroscopic analyses and docking simulation[J]. Journal of Hazardous Materials, 2021, 408: 124901. DOI:10.1016/j.jhazmat.2020.124901.
[4] YANG Q, ZHAI Y, XU T, et al. Facile fabrication of Sc-BiOBr photocatalyst immobilized on palm bark with enhanced visible light photocatalytic performance for estradiol degradation[J]. Journal of Physics and Chemistry of Solids, 2019, 130:127-135. DOI:10.1016/j.jpcs.2019.02.028.
[5] AGHDAM S M, HAGHIGHI M, ALLAHYARI S, et al. Precipitation dispersion of various ratios of BiOI/BiOCl nanocomposite over g-C₃N₄ for promoted visible light nanophotocatalyst used in removal of acid orange 7 from water[J]. Journal of Photochemistry and Photobiology A:Chemistry, 2017, 338: 201-212. DOI:10.1016/j.jphotochem.2017.02.013.
[6] FENG Z, ZENG L, ZHANG Q L, et al. In situ preparation of g-C₃N₄/Bi₄O₅I₂ complex and its elevated photoactivity in Methyl Orange degradation under visible light[J]. Journal of Environmental Sciences(China), 2020, 87:149. DOI:10.1016/j.jes.2019.05.032.
[7] JIANG X D, LAI S F, XU W C, et al. Novel ternary BiOI/g-C₃N₄/CeO₂ catalysts 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] HUANG H, LIU C Y, OU H L, et al. Self-sacrifice transformation for fabrication of type-Ⅰ and type-Ⅱ heterojunctions in hierarchical BixOyIz/g-C₃N₄ for efficient visible-light photocatalysis[J]. Applied Surface Science, 2019, 470: 1101-1110. DOI:10.1016/j.apsusc.2018.11.193.
[9] TIAN N, HUANG H W, WANG S B, et al. Facet-charge-induced coupling dependent interfacial photocharge separation:A case of BiOI/g-C₃N₄ p-n junction[J]. Applied Catalysis B:Environmental, 2020, 267: 118697. DOI:10.1016/j.apcatb.2020.118697.
[10] JIANG D, CHEN L, ZHU J, et al. Novel p-n heterojunction photocatalyst constructed by porous graphite-like C₃N₄ and nanostructured BiOI:facile synthesis and enhanced photocatalytic activity[J]. Dalton Transactions, 2013, 42(44): 15726-15734. DOI:10.1039/C3DT52008K.
[11] TIAN Y L, CHANG B B, LU J L, et al. Hydrothermal synthesis of graphitic carbon nitride-Bi₂WO₆ Heterojunctions with enhanced visible light photocatalytic activities[J]. Applied Materials & Interfaces, 2013, 5(15): 7079-7085. DOI:10.1021/am4013819.
[12] FENG Z, ZENG L, ZHANG Q, et al. In situ preparation of g-C₃N₄/Bi₄O₅I₂ complex and its elevated photoactivity in Methyl Orange degradation under visible light[J]. Journal of Environmental Sciences, 2020, 87. DOI:10.1016/j.jes.2019.05.032.
[13] SAKTHIVEL T, HUANG X, Wu Y, et al. Recent progress in black phosphorus nanostructures as environmental photocatalysts[J]. Chemical Engineering Journal(Lausanne, Switzerland:1996), 2020, 379: 122297. DOI:10.1016/j.cej.2019.122297.
[14] TIAN N, HUANG H W, WANG S B, et al. Facet-charge-induced coupling dependent interfacial photocharge separation:A case of BiOI/g-C₃N₄ p-n junction[J]. Applied Catalysis B:Environmental, 2020, 267: 118697. DOI:10.1016/j.apcatb.2020.118697.
[15] TIAN N, ZHANG Y, LIU C, et al. G-C₃N₄/Bi₄O₅I22D-2D heterojunctional nanosheets with enhanced visible-light photocatalytic activity[J]. RSC Advances, 2016, 6(13): 10895-10903. DOI:10.1039/C5RA24672E.
[16] ZHAO Q, ZHAO H, QUAN X, et al. Photochemical transformation of 2, 2', 4, 4'-tetrabromodiphenyl ether(BDE-47)in surface coastal waters: Effects of chloride and ferric ions[J]. Marine Pollution Bulletin, 2014, 86(1-2): 76-83. DOI:10.1016/j.marpolbul.2014.07.040.
[17] PERSSON I. Hydrated metal ions in aqueous solution:How regular are their structures?[J]. Pure & Applied Chemistry, 2010, 82(10):1901-1917. DOI:10.1351/PAC-CON-09-10-22.
[18] LI S, LAI C, LI C, et al. Enhanced photocatalytic degradation of dimethyl phthalate by magnetic dual Z-scheme iron oxide/ mpg-C₃N₄/ BiOBr/ polythiophene heterostructure photocatalyst under visible light[J]. Journal of Molecular Liquids, 2021,324:116947. DOI:10.1016/j.molliq.2021.116947.
[19] 邹亚文,张泽明,张洪海,等.水体系中3种常见邻苯二甲酸酯的光化学降解研究[J].环境科学学报, 2018,38(8): 3012-3020. DOI:10.13671/j.hjkxxb.2018.0057.
[20] 潘水红.水环境中邻苯二甲酸酯光降解机理的研究[D].温州:温州大学, 2018.
[21] XU X R, LI S X, LI X Y, et al. Degradation of n-butyl benzyl phthalate using TiO₂/UV[J]. Journal of Hazardous Materials, 2009, 164(2-3): 527-532. DOI:10.1016/j.jhazmat.2008.08.027.
[22] 梁大鹏,聂林春,方媛萍,等.水体中邻苯二甲酸酯的光催化降解[J].吉林大学学报(理学版), 2020, 58(2): 434-440. DOI:10.13413/j.cnki.jdxblxb.2019294. (