化工新型材料

化工新型材料 ›› 2023, Vol. 51 ›› Issue (4) : 208-213. DOI: 10.19817/j.cnki.issn1006-3536.2023.04.037

科学研究

磺酸化铁酸镍磁性石墨烯复合材料活化过硫酸盐降解水中2-氨基苯并噻唑的研究

^1*

作者信息 +

Magnetic graphene modified by sulfonic acid ionic liquid surfactant to degrade 2-aminobenzothiazole in water by activated PMS

Ma Sen¹, Gao Shiqian¹, Wang Zhenfeng², Zhang Zhanen¹

Author information +

文章历史 +

Received		Published
2021-12-16		2023-04-20
Issue Date	Revised Date
2023-04-27	2021-12-16

PDF

摘要

采用微波法在水-离子液体表面活性剂的体系,制备了磺酸化铁酸镍磁性石墨烯(GS/NiFe₂O₄)复合材料,通过扫描电镜(SEM)、透射电镜(TEM)、X射线衍射(XRD)、振动样品磁强计(VSM)、X射线光电子能谱(XPS)、BET/BJH的方法分析材料的表观结构。使用GS/NiFe₂O₄活化过硫酸盐(PMS)降解水中的2-氨基苯并噻唑(ABT),并通过超高效液相色谱-串联质谱法对降解率进行定量分析。经条件优化得出,在pH=3、PMS浓度为4mmol/L,投加15mg GS/NiFe₂O₄的条件下,30min内可完全降解20mg/L的2-氨基苯并噻唑。考察了阴阳离子对ABT的降解过程影响:Cl^-对ABT的降解有促进作用,HCO^-₃具有抑制作用,而Cu²⁺具有双重作用。通过自由基猝灭实验发现SO^-₄·为主导自由基、·OH为辅。最后对ABT的降解过程进行了产物分析且证明了GS/NiFe₂O₄具有良好的循环利用性能。

Abstract

The sulfonated nickel ferrite magnetic graphene (GS/NiFe₂O₄) composite was prepared by microwave method in the system of water-ionic liquid surfactant.The surface structure of the composite was analyzed by SEM,TEM,XRD,VSM,XPS and BET/BJH.GS/NiFe₂O₄ activated persulfate (PMS) was used to degrade 2-aminobenzothiazole (ABT) in water,and the degradation rate was quantitatively analyzed by ultra high performance liquid chromatography tandem mass spectrometry.The optimized conditions showed that it could completely degrade 20mg/L of 2-aminobenzothiazole within 30 minutes at pH=3,PMS concentration of 4mmol/L and 15mg GS/NiFe₂O₄ addition.The effects of anions and cations on the degradation process of ABT were investigated:Cl^- promoted the degradation of ABT,while HCO^-₃ inhibited it,and Cu²⁺ had a dual effect.The radical quenching experiment revealed that SO^-₄· was the dominant radical and ·OH was the auxiliary.Finally,the degradation process of ABT was analyzed,which demonstrated that GS/NiFe₂O₄ had good recycling performance.

关键词

磺酸化 / 铁酸镍磁性石墨烯 / 2-氨基苯并噻唑 / 过硫酸盐 / 降解

Key words

sulfonation / nickel ferrite magnetic graphene / 2-aminobenzothiazole / persulfate / degradation

引用本文

引用格式 ▾

磺酸化铁酸镍磁性石墨烯复合材料活化过硫酸盐降解水中2-氨基苯并噻唑的研究[J]. 化工新型材料, 2023, 51(4): 208-213 DOI:10.19817/j.cnki.issn1006-3536.2023.04.037

登录浏览全文

4963

注册一个新账户忘记密码

参考文献

原文顺序 | 出版日期 | 本文引用

[1] Dutta G K,Guha S,Patil S,et al.Synthesis of liquid crystalline benzothiazole based derivatives:a study of their optical and electrical properties[J].Organic Electronics,2010,11:1-9.
[2] Weekes A A,Westwell A D,et al.2-Arylbenzothiazole as a privileged scaffold in drug discovery[J].Current Medicinal Chemistry,2009,16:2430-2440.
[3] Hong Y P,Song B A,Wu P,et al.Research advances in synthesis and biological activity of benzothiazole derivatives[J].Journal of Anhui Agricultural Sciences,2005,33:1254-1257.
[4] De Wever H,Besse P,Verachtert H,et al.Microbial transformations of 2-substituted benzothiazoles[J].Applied Microbiology and Biotechnology,2001,57:620-625.
[5] Wen M T,Shao L W,Chen W G,et al.Research and application of bioeide containing TCMTB[J].Industrial Water Treatment,2008,28:33-35.
[6] Qi B R,Qin C Y,Dong J,et al.Occurence and mitigation of benzothiazoles in wastewater[J].Environmental Chemistry 2017,36:2498-2510.
[7] Li P Y,Li J S,Liu W D,et al.Recent advance in the synthesis of benzothiazoles[J].Fine Chemical Intermediates,2011,41:8-11.
[8] Hornung M W,Kosian P A,Haselman J T,et al.In vitro,ex vivo,and in vivo determination of thyroid hormone modulating activity of benzothiazoles[J].Toxicological Sciences,2015,146:254-264.
[9] 孙佳政.天津市土壤和典型植物中有机紫外吸收剂污染特征及环境风险[D].北京:华北电力大学,2020.
[10] Chipinda I,Zhang X D,Simoyi R H,et al.Mercaptobenzothiazole allergenicity-role of the thiol group[J].Cutaneous and Ocular Toxicology,2008,27:103-116.
[11] Wang J C,Xiong L,Zhang H J,et al.Simultaneous determination of benzotriazoles and benzothiazole in surface water by solid phase extraction and high performance liquid chromatography[J].Chinese Journal of Chromatography,2013,31:139-142.
[12] Zhong M,Li M,Lu F,et al.Mechanism of thermal-activated persulfate combined with coagulation in the treatment of microemulsion[J].China Environmental Science,2021,41:704-712.
[13] Shen Y J,Peng G M,Xu B K,et al.Degradation of BP4 by UV-activated persulfate process:kinetic,mechanism and risk[J].Research of Environmental Sciences,2019,32:174-182.
[14] Tian T T,Li Z Y,Wang Z D,et al.Research progress of transition metal activated persulfate to degrade organic wastewater[J].Chemical Industry and Engineering Progress,2021,40:3480-3488.
[15] Li X J,Ye L M,Liao F Z,et al.Research progress in the application of heteroatom-doped carbonaceous materials for persulfate activation[J].Chemical Industry and Engineering Progress,2021,40:273-281.
[16] Hu Y,Zhang Y Q,Li X Y,et al.A new imidazolium ionic liquid surfactant soft-template method for preparation of strontium carbonate nanorods[J].Chemical Research and Application,2011,23:1374-1377.
[17] Wang H X,Li X X,Tang Z W,et al.Synthesis and properties of TiO₂ hollow microspheres[J].Fine Chemicals,2017,34:1329-1333.
[18] Laokul P,Amornkitbamrung V,Seraphin S,et al.Preparation and characterization of hollow TiO₂ nanospheres:the effect of Fe³⁺ doping on their microstructure and electronic structure[J].Current Applied Physics,2011,11:101-108.
[19] Cheng Y,Zheng Y H,Wang Y H,et al.Synthesis and magnetic properties of nickel ferrite nano-octahedra[J].Journal of Soild State Chemistry,2005,178:2394-2397.
[20] Dong J,Ren L M,Chi Z F,et al.Analysis of XPS in the Removal of Cr(Ⅳ) from Groundwater with rGO-nZVI[J].Spectroscopy and Spectral Analysis,2015,37:250-255.
[21] Yan Z J,He M,Chen B B,et al.Magnetic covalent triazine framework for rapid extraction of phthalate esters in plastic packaging materiaIs followed by gas chromatography-flame ionization detection[J].Journal of Chromatography A,2017,1525:32-41.
[22] Shao Z C,Gao S Q,Zhang Z E,et al.Covalent triazine-based framework activates peroxymonosulfate to degrade sulfamethoxazole[J].China Environmental Science,2020,40:135-142.
[23] Anipsitakis G P,Dionysiou D D.Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science & Technology,2004,38:3705-3712.
[24] Yang S Y,Yang X,Shao X T,et al.Activated carbon catalyzed persulfate oxidation of Azo dye acid orange 7at ambient temperature[J].Journal of Hazardous Materials,2011,186:659-666.
[25] Wang H Z,Guo W Q,Yin R L,et al.Biochar-induced Fe(Ⅲ) reduction for persulfate activation in sulfamethoxazole degradation:insight into the electron transfer,radical oxidation and degradation pathways[J].Chemical Engineering Journal,2019,362:561-569.
[26] Liu C M,Ding J,Liu X S,et al.Study on the degradation efficiency of benzothiazole in an electrically assisted microbial reactor[J].Environmental Science,2014,35:4192-4197.
[27] Han X Y,Zhang L,Chen T M,et al.Research on treatment of benzothiazole in wastewater by Fenton process[J].Modern Chemical Industy,2017,37:117-120.