共价有机骨架磁固相萃取-气相色谱法测定15种邻苯二甲酸酯
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摘要
目的建立磁共价有机骨架材料TpPa-1/Fe304固相萃取与气相色谱法(gas chromatography, GC)联用技术测定样品中15种邻苯二甲酸酯(phthalate esters, PAEs)的分析方法。方法将TpPa-1与Fe~(2+)、Fe~(3+)在碱性条件下合成TpPa-1/Fe_3O_4,经过磁固相萃取过程将PAEs吸附,并使用甲醇洗脱,上机检测,外标法定量。结果15种PAEs的检出限为0.313～5.198μg/L(S/N=3)。PAEs的日内和日间相对标准偏差(relative standard deviations,RSDs)值分别小于6.6%和7.8%。该方法已成功应用于碳酸饮料和环境水样中痕量PAEs的测定,回收率在89.1%～103.6%之间,RSD小于7.9%。结论本研究提供了一种简单快速的共价有机骨架(covalent organic frameworks, COFs)材料的磁化方法,可应用于食品样品前处理中富集和分离PAEs。
Objective To establish a method for the determination of 15 kinds of phthalate esters(PAEs) in samples by solid phase extraction of covalent organic framework magnetic solid TpPa-1/Fe_3O_4 and gas chromatography(GC). Methods TpPa-1/Fe_3O_4 was synthesized with Fe~(2+), Fe~(3+) and TpPa-1 under alkaline conditions. The PAEs were adsorbed by magnetic solid phase extraction and eluted with methanol, quantified by external standard method and then detected by GC. Results The limit of detections of 15 PAEs were 0.313-5.198 μg/L(S/N=3). The intra-day and inter-day relative standard deviations(RSDs) of the PAEs were less than 6.6% and 7.8%, respectively. The developed method was successfully applied for the determination of trace PAEs in carbonated drinks and tap water with recoveries ranging from 89.1% to 103.6% and RSDs were less than 7.9%. Conclusions This is a simple and rapid magnetization method for covalent organic frameworks(COFs) materials, which is expected to be used to enrich and separate PAEs in food sample pretreatment.
Objective To establish a method for the determination of 15 kinds of phthalate esters(PAEs) in samples by solid phase extraction of covalent organic framework magnetic solid TpPa-1/Fe_3O_4 and gas chromatography(GC). Methods TpPa-1/Fe_3O_4 was synthesized with Fe~(2+), Fe~(3+) and TpPa-1 under alkaline conditions. The PAEs were adsorbed by magnetic solid phase extraction and eluted with methanol, quantified by external standard method and then detected by GC. Results The limit of detections of 15 PAEs were 0.313-5.198 μg/L(S/N=3). The intra-day and inter-day relative standard deviations(RSDs) of the PAEs were less than 6.6% and 7.8%, respectively. The developed method was successfully applied for the determination of trace PAEs in carbonated drinks and tap water with recoveries ranging from 89.1% to 103.6% and RSDs were less than 7.9%. Conclusions This is a simple and rapid magnetization method for covalent organic frameworks(COFs) materials, which is expected to be used to enrich and separate PAEs in food sample pretreatment.
引文
[1] Yang J, Li Y, Wang Y, et al. Recent advances in analysis of phthalate estersin foods[J]. Trends Anal Chem, 2015,(72):10-26.
[2]张续,邱天,付慧,等.超高效液相色谱—三重四极杆质谱法测定人尿中9种邻苯二甲酸酯代谢物[J].色谱,2018,36(9):895-903.Zhang X, Qiu T, Fu H, et al. Determination of nine phthalate ester metabolites in human urine using ultra high performance liquid chromatography-tandem triple quadrupole mass spectrometry[J]. Chin J Chromatogr, 2018, 36(9):895-903.
[3] Wang W, Craig ZR, Basavarajappa MS, et al. Di(2-ethylhexyl)phthalate inhibits growth of mouse ovarian antral follicles through an oxidative stress pathway[J]. Toxicol Appl Pharmacol, 2012, 258(2):288-295.
[4] Montevecchi G, Masino F, Di Pascale N, et al. Study of the repartition ofphthalate esters during distillation of wine for spirit production[J]. Food Chem, 2017,(237):46-52.
[5] Ji Y, Wang F, Zhang L, et al. A comprehensive assessment of human exposure to phthalates from environmental media and food in Tianjin,China[J]. J Hazard Mater, 2014,(279):133-40.
[6] Huo SH, Yan XP. Facile magnetization of metal-organic framework MIL-101 for magnetic solid-phase extraction of polycyclic aromatic hydrocarbons in environmental water samples[J]. Analyst, 2012, 137(15):3445-3451.
[7] Russo MV, Notardonato I, Cinelli G, et al. Evaluation of an analytical method for determining phthalate esters in wine samples by solid-phase extraction and gas chromatography coupled with ion-trap mass spectrometer detector[J]. Anal Bioanal Chem, 2012,402(3):1373-1381.
[8]杨成雄,严秀平.共价-有机骨架材料在色谱及样品预处理中的应用[J].色谱,2018,36(11):1075-1080.Yang CX, Yan XP. Application of covalent-organic frameworks in chromatography and sample pretreatment[J]. Chin J Chromatogr, 2018,36(11):1075-1080.
[9] Luo YB, Yu QW, Yuan BF, et al. Fast microextraction of phthalate acid esters from beverage, environmental water and perfume samples by magnetic multi-walled carbon nanotubes[J]. Talanta, 2012,(90):123-131.
[10] Biswal BP, Chandra S, Kandambeth S, et al. Mechanochemical synthesis of chemically stable isoreticular covalent organic frameworks[J]. J AmChem Soc, 2013, 135(14):5328-5331.
[11] Chandra S, Kandambeth S, Biswal BP, et al. Chemically stable multilayered covalent organic nanosheets from covalent organic frameworks via mechanical delamination[J]. J Am Chem Soc, 2013,135(47):17853-17861.
[12] Segura JL, Mancheno MJ, Zamora F. Covalent organic frameworks based on Schiff-base chemistry:Synthesis, properties and potential applications[J]. Chem Soc Rev, 2016,45(20):5635-5671.
[2]张续,邱天,付慧,等.超高效液相色谱—三重四极杆质谱法测定人尿中9种邻苯二甲酸酯代谢物[J].色谱,2018,36(9):895-903.Zhang X, Qiu T, Fu H, et al. Determination of nine phthalate ester metabolites in human urine using ultra high performance liquid chromatography-tandem triple quadrupole mass spectrometry[J]. Chin J Chromatogr, 2018, 36(9):895-903.
[3] Wang W, Craig ZR, Basavarajappa MS, et al. Di(2-ethylhexyl)phthalate inhibits growth of mouse ovarian antral follicles through an oxidative stress pathway[J]. Toxicol Appl Pharmacol, 2012, 258(2):288-295.
[4] Montevecchi G, Masino F, Di Pascale N, et al. Study of the repartition ofphthalate esters during distillation of wine for spirit production[J]. Food Chem, 2017,(237):46-52.
[5] Ji Y, Wang F, Zhang L, et al. A comprehensive assessment of human exposure to phthalates from environmental media and food in Tianjin,China[J]. J Hazard Mater, 2014,(279):133-40.
[6] Huo SH, Yan XP. Facile magnetization of metal-organic framework MIL-101 for magnetic solid-phase extraction of polycyclic aromatic hydrocarbons in environmental water samples[J]. Analyst, 2012, 137(15):3445-3451.
[7] Russo MV, Notardonato I, Cinelli G, et al. Evaluation of an analytical method for determining phthalate esters in wine samples by solid-phase extraction and gas chromatography coupled with ion-trap mass spectrometer detector[J]. Anal Bioanal Chem, 2012,402(3):1373-1381.
[8]杨成雄,严秀平.共价-有机骨架材料在色谱及样品预处理中的应用[J].色谱,2018,36(11):1075-1080.Yang CX, Yan XP. Application of covalent-organic frameworks in chromatography and sample pretreatment[J]. Chin J Chromatogr, 2018,36(11):1075-1080.
[9] Luo YB, Yu QW, Yuan BF, et al. Fast microextraction of phthalate acid esters from beverage, environmental water and perfume samples by magnetic multi-walled carbon nanotubes[J]. Talanta, 2012,(90):123-131.
[10] Biswal BP, Chandra S, Kandambeth S, et al. Mechanochemical synthesis of chemically stable isoreticular covalent organic frameworks[J]. J AmChem Soc, 2013, 135(14):5328-5331.
[11] Chandra S, Kandambeth S, Biswal BP, et al. Chemically stable multilayered covalent organic nanosheets from covalent organic frameworks via mechanical delamination[J]. J Am Chem Soc, 2013,135(47):17853-17861.
[12] Segura JL, Mancheno MJ, Zamora F. Covalent organic frameworks based on Schiff-base chemistry:Synthesis, properties and potential applications[J]. Chem Soc Rev, 2016,45(20):5635-5671.