您的位置：山东大学 -> 科技期刊社 -> 《山东大学学报（工学版）》

山东大学学报(工学版) ›› 2017, Vol. 47 ›› Issue (4): 117-123.doi: 10.6040/j.issn.1672-3961.0.2017.002

• • 上一篇    下一篇

Fe3O4磁性石墨烯分散固相萃取水中的有机氯污染物

王明雨1,苏丽清2*,张少君1,汪昱3   

  1. 1. 山东交通学院船舶与轮机工程学院, 山东 威海 264310;2. 威海市立医院内分泌科, 山东 威海 264200;3. 山东省地方病防治研究所碘缺乏病科, 山东 济南 250014
  • 收稿日期:2017-01-03 出版日期:2017-08-20 发布日期:2017-01-03
  • 通讯作者: 苏丽清(1968— ),女,山东威海人,硕士,主要研究方向为内分泌干扰物. E-mail: ytu102@163.com E-mail:vicsee@163.com
  • 作者简介:王明雨(1974— ),男,辽宁朝阳人,教授,硕导,博士,主要研究方向为水污染控制.E-mail: vicsee@163.com
  • 基金资助:
    国家自然科学基金资助项目(51609131);山东省自然科学基金资助项目(ZR2014JL038);山东省高等学校科技计划资助项目(J14LD04;J16LA61);威海市科技发展计划资助项目(2016GGX003-1)

Fe3O4 magnetic dispersive solid-phase extraction with graphene for determination of organochlorine pesticides contaminants in water

WANG Mingyu1, SU Liqing2*, ZHANG Shaojun1, WANG Yu3   

  1. 1. Naval Architecture &
    Marine Engineering College, Shandong Jiaotong University, Weihai 264310, Shandong, China;
    2. Department of Endocrinology, Weihai Municipal Hospital, Weihai 264200, Shandong, China;
    3. Iodine Deficiency Disorders, Institute of Endemic Disease Control, Shandong Province, Jinan 250014, Shandong, China
  • Received:2017-01-03 Online:2017-08-20 Published:2017-01-03

PDF (PC)

644

摘要： 开发负载胶束的磁性Fe3O4纳米微粒修饰的石墨烯作为新型分散固相萃取材料,并用于水中有机氯的检测。磁性石墨烯由氧化石墨烯和Fe2+通过氧化还原法一步合成,负载阳离子表面活性剂CTAB形成纳米混合胶束作为提取系统。应用本方法分析水中的29种有机氯,检测限达到1.5~5.0 ng/L,样品加标回收率范围在75.22%~97.15%。复重性的相对标准偏差小于9.995%,与传统的固相萃取法相比,方法的灵敏度提高了50~113倍。该方法快速、灵敏、准确,可以同时测定水中多种有机氯农残,适合于大批量样品的测定。

关键词: 农药残留, 胶束提取, 分散固相萃取, 有机氯, 石墨烯, 磁性Fe3O4纳米微粒

Abstract: A novel dispersive solid-phase extraction(DSPE)analysis method was established by combining Fe3O4magnetic nanoparticles modified graphene as absorption material for determination of organochlorine pesticides(OCPs)in water. Magnetic nanoparticles modified graphene(MNG)was prepared by graphene oxide and Fe2+ through redox reaction in one step. Cationic surfactant CTAB was added as micelle forming agent, in which MNG was carrier of mixed micelles extraction system. Mixed micelle modified MNG had higher loading capacity than pure Fe3O4magnetic graphene. This method was applied to detect 29 kinds of OCPs in water. The detection limit was in the range of 1.5~5.0 ng/L. The recovery was ranged from 75.22% to 97.15%. The relative standard deviation(RSD)of repeatability was lower than 9.995%. As compared with ordinary solid-phase extraction, the sensitivity of new method increased 50~113 times. The method was suitable for simultneous determination of OCPs pesticide residues in water with high accuracy, sensitivity and less pre-treatment time, which was suitable for batch analysis of samples.

Key words: micelles extraction, Fe3O4 magnetic nanoparticles, pesticide residues, dispersive solid-phase extraction, organochlorine pesticide, graphene

中图分类号: 

  • X832
[1] RANI M, SHANKER U, JASSAL V. Recent strategies for removal and degradation of persistent & toxic organochlorine pesticides using nanoparticles: a review[J]. Journal of Environmental Management, 2017, 190(1): 208-222.
[2] 薛海全, 崔兆杰, 杜世勇. ASE萃取-GPC净化-GC/ECD测定小麦中有机氯农残和多氯联苯[J]. 山东大学学报(理学版), 2011, 46(1):11-15. XUE Haiquan, CUI Zhaojie, DU Shiyong. Determination of organochlorine pesticides and polychlorinated biphenyls in wheat by gas chromatography with accelerated solvent extraction and gel permeation chromatography cleanup[J]. Journal of Shandong University(Natural Science), 2011, 46(1): 11-15.
[3] RODRÍGUEZ A, LÓPEZ M, CASILLAS T. Monitoring of organochlorine pesticides in blood of women with uterine cervix cancer[J]. Environmental Pollution, 2017, 220(1): 853-862.
[4] YUAN H Z, LIU E F, ZHANG E L, et al. Historical records and sources of polycyclic aromatic hydrocarbons(PAHs)and organochlorine pesticides(OCPs)in sediment from a representative plateau lake, China[J]. Chemosphere, 2017, 173(1): 78-88.
[5] LIU Y X, GAO Z J, WU R, et al. Magnetic porous carbon derived from a bimetallic metal—organic framework for magnetic solid-phase extraction of organochlorine pesticides from drinking and environmental water samples[J]. Journal of Chromatography A, 2017, 1479(1): 55-61.
[6] LIU J, QI S H, YAO J, et al. Contamination characteristics of organochlorine pesticides in multimatrix sampling of the Hanjiang River Basin, southeast China[J]. Chemosphere, 2016, 163(1): 35-43.
[7] 邵阳, 杨国胜, 刘韦华, 等. 北京地区地表水中OCPs和PCBs的污染分析[J]. 中国环境科学, 2016,36(9): 2606-2613. SHAO Yang, YANG Guosheng, LIU Weihua, et al. The study of organochlorine pesticides and polychlorinated biphenyls in surface water around Beijing[J]. China Environmental Science, 2016, 36(9): 2606-2613.
[8] YANG D, QI S H, ZHANG J Q, et al. Organochlorine pesticides in soil, water and sediment along the Jinjiang River mainstream to Quanzhou Bay, south east China[J]. Ecotoxicology and Environmental Safety, 2013, 89(1):59-65.
[9] 暴志蕾, 赵兴茹, 耿梦娇, 等. 长三角地区饮用水源地沉积物中有机氯农药污染特征[J]. 环境化学, 2016, 35(6):1237-1245. BAO Zhilei, ZHAO Xingru, GENG Mengjiao, et al. Characteristics of organochlorine pesticides in the sediments from the drinking water source of the Yangtze River delta region[J].Environmental Chemistry, 2016, 35(6):1237-1245.
[10] 刘静, 崔兆杰, 许宏宇, 等. 类二噁英类多氯联苯的双柱气相色谱分析方法研究[J]. 山东大学学报(工学版), 2008, 38(4):116-122. LIU Jing, CUI Zhaojie, XU Hongyu, et al. A method study of dual capillary column gas chromatography with electron capture detection for the determination of dioxin-like polychlorinated biphenyls[J]. Journal of Shandong University(Engineering Science), 2008, 38(4):116-122.
[11] YOUSEFI S, SHEMIRANI F, GHORBANIAN S, et al. Deep eutectic solvent magnetic bucky gels in developing dispersive solid phase extraction: application for ultra trace analysis of organochlorine pesticides by GC-micro ECD using a large-volume injection technique[J]. Talanta, 2017, 168:73-81.
[12] 申中兰, 袁东, 王茂森, 等. 稳定性同位素稀释气相色谱-质谱法测定金枪鱼中多氯联苯的不确定度评定[J]. 山东大学学报(理学版), 2013, 48(5):34-38. SHEN Zhonglan, YUAN Dong, WANG Maosen, et al. Uncertainty estimation in determination of polychlorinated biphenyls in tuna by stable isotope dilution gas chromatography-mass spectrometry[J]. Journal of Shandong University(Natural Science), 2013, 48(5):34-38.
[13] KOUREAS M, KARAGKOUNI F, RAKITSKII V, et al. Serum levels of organochlorine pesticides in the general population of Thessaly, Greece, determined by HS-SPME GC—MS method[J]. Environmental Research, 2016, 148(1):318-321.
[14] BAJWA A, ALI U, MAHMOOD A, et al. Organochlorine pesticides(OCPs)in the Indus River catchment area, Pakistan: status, soil-air exchange and black carbon mediated distribution[J]. Chemosphere, 2016, 152(1): 292-300.
[15] HANAN A. Validation method of organochlorine pesticides residues in water using gas chromatography-quadruple mass[J]. Water Science, 2016, 30(2):96-107.
[16] ZHANG Z W, WU Y P, LI X W, et al. Multi-class method for the determination of nitroimidazoles, nitrofurans, and chloramphenicol in chicken muscle and egg bydispersive-solid phase extraction and ultra-high performance liquid chromatography-tandem mass spectrometry[J]. Food Chemistry, 2017, 217(1):182-190.
[17] FIROUZABADI Z, SHABANI A, DADFARNIA S, et al. Preconcentration and speciation of thallium by ferrofluid based dispersive solid phase extraction and flame atomic absorption spectrometry[J]. Microchemical Journal, 2017, 130(1):428-435.
[18] YASER P, FATEMEH G, MARYAM S. Superparamagnetic graphene oxide-based dispersive-solid phase extraction for preconcentration and determination of tamsulosin hydrochloride in human plasma by high performance liquid chromatography-ultraviolet detection[J]. Journal of Chromatography A, 2017, 1499(1):21-29.
[19] LI M H, WANG J T, JIAO C, et al. Graphene oxide framework: an adsorbent for solid phase extraction of phenylurea herbicides from water and celery samples[J]. Journal of Chromatography A, 2016, 1469:17-24.
[20] 祁振, 于淑艳, 刘璐, 等. 石墨烯对四环素的吸附热力学及动力学研究[J]. 山东大学学报(工学版), 2013,43(3):63-69. QI Zhen, YU Shuyan, LIU Lu, et al. Kinetic and thermodynamic studies on the adsorption of tetracycline onto graphene[J]. Journal of Shandong University(Engineering Science), 2013,43(3):63-69.
[21] ARMAKOVIC S, ARMAKOVIC S J. Investigation of boron modified graphene nanostructures; optoelectronic properties of graphenenanoparticles and transport properties of graphene nanosheets[J]. Journal of Physics and Chemistry of Solids, 2016, 98(1):156-166.
[22] NODEH H R, IBRAHIM W A W, KAMBOH M A, et al. New magnetic graphene-based inorganic—organic sol-gel hybrid nanocomposite for simultaneous analysis of polar and non-polar organophosphorus pesticides from water samples using solid-phase extraction[J]. Chemosphere, 2017, 166: 21-30.
[23] WANG F X, LIU S Q, YANG H, et al. Hierarchical graphene coating for highly sensitive solid phase microextraction of organochlorine pesticides[J]. Talanta, 2016, 160:217-224.
[24] 白艳艳, 曹月欣, 张宪玺, 等. SDS对香豆素在SB-16胶束增溶行为影响[J]. 山东大学学报(工学版), 2016, 46(3):99-105. BAI Yanyan, CAO Yuexin, ZHANG Xianxi, et al. The influence of SDS on C-343 solubilizing behavior in SB-16 micelle[J]. Journal of Shandong University(Engineering Science), 2016, 46(3):99-105.
[25] LIU Q, SHI J B, WANG T. Hemimicelles/admicelles supported on magnetic graphene sheets for enhanced magnetic solid-phase extraction[J]. Journal of Chromatography A, 2012, 1257(1):1-8.
[1] 祁振, 于淑艳, 刘璐, 王曙光*. 石墨烯对四环素的吸附热力学及动力学研究[J]. 山东大学学报(工学版), 2013, 43(3): 63-69.
Viewed
Full text


Abstract

Cited
  Shared   
  Discussed   
No Suggested Reading articles found!
版权所有 © 2018 《山东大学学报(工学版)》编辑部　
地址: 济南市山大南路27号（250100）　 电话: 0531-88366735　 E-mail: xbgxb@sdu.edu.cn
本系统由北京玛格泰克科技发展有限公司设计开发