金属有机骨架纳米材料-固相萃取环境水样中亚硝胺类消毒副产物
Determination of N-nitrosamines in water samples based on the solid-phase extraction with metal-organic framework
-
摘要: 将通过水热合成法制备的金属有机骨架材料[MIL-101(Cr)]作为吸附剂应用于吸附环境水样中的亚硝胺类消毒副产物,采用超高效液相色谱-串联质谱法(UHPLC-MS/MS)进行测定.通过SEM、TEM和FT-IR技术对MIL-101(Cr)的表面形态和特征基团进行表征,并对影响萃取效率的主要因素,如MIL-101(Cr)的用量、萃取时间、水样的pH值和解吸条件等进行考察.研究表明,当MIL-101(Cr)用量为6.0 mg,pH=9.0,30℃下9 min内可达吸附平衡,回收率高于63.5%,3种亚硝胺的检出限为0.029-0.283 μg·L-1.将方法应用于环境水样的测定,加标回收率在77.9%-107.2%范围内,相对标准偏差低于5.4%.该方法操作简单快速、准确可靠、检出限低,可用于水样中痕量亚硝胺类消毒副产物的检测.Abstract: The metal-organic frameworks[MIL-101(Cr)] was synthesized by hydrothermal method and applied to the absorption of N-nitrosamines (NAs) in environmental water coupled with ultra high performance liquid chromatography-tandem mass spectrometry(UHPLC-MS/MS). The surface morphology was characterized by SEM, TEM and FT-IR. The experimental parameters of solid phase extraction were investigated including the amount of MIL-101(Cr), extraction time, sample pH and desorption conditions. The recoveries of NAs were over 63.5% within 9.0 min when the mass concentration of MIL-101(Cr) was 6.0 mg, the pH value of water sample was 9.0, the desorption temperature was 30℃. The detection limits were in the range of 0.029-0.238 μg·L-1. The developed method was successfully applied to the analysis of NAs in environmental water samples, the recoveries were in the range from 77.9% to 107.2% and the RSDs was within 5.4%. The proposed method was simple, rapid and accurate, which could be applied to the analysis of the trace amount NAs in environmental water samples.
-
-
[1] 张馨怡, 魏东斌, 杜宇国. 紫外-氯联合消毒处理及副产物生成特征研究进展[J]. 环境化学, 2018, 37(9):71-81. ZHANG X Y, WEI D B, DU Y G. Ultraviolet-chlorine combination disinfection and formation of disinfection by-products:A review[J]. Environmental chemistry, 2018, 37(9):71-81(in Chinese).
[2] KESZEI A P, GOLDBOHM R A, SCHOUTEN L J, et al. Dietary N-nitroso compounds, endogenous nitrosation, and the risk of esophageal and gastric cancer subtypes in the Netherlands Cohort Study[J]. American Journal of Clinical Nutrition, 2013, 97(1):135-146. [3] 彭俏容,唐涛,于淑新,等. 基于冷冻熔炼的液-液萃取/气相色谱法测定啤酒中的N-二甲基亚硝胺[J].色谱, 2014,32(4):433-437. PENG Q R, TANG T, YU S X, et al. Determination of N-nitrosodimethylamine in beer by frozen zone melting liquid-liquid extraction/gas chromatography[J]. Chromatography, 2014, 32(4):433-437(in Chinese).
[4] 陈文文, 张原, 李小水, 等. 水中N-亚硝胺的富集及色谱分析测试技术[J]. 环境化学, 2016, 35(10):2117-2126. CHEN W W, ZHANG Y, LI X S, et al. Preconcentration and chromatographic technologies for the analysis of N-nitrosamines in water[J]. Environmental Chemistry, 2016, 35(10):2117-2126(in Chinese).
[5] 陈嘉彬,孙海峰,游金清,等.磁固相萃取技术应用于主流烟气中烟草特有N-亚硝胺的测定[J].分析测试学报,2018,37(5):588-593. CHEN J B, SHUN H Y, YOU J Q, et al. A magnetic solid phase extraction technique for determination of tobacco-specific N-Nitrosamines in mainstream cigarette smoke[J]. Journal of Instrumental Analysis, 2018, 37(5):588-593(in Chinese).
[6] 赵庄,许杨彪,刘向红,等.改进的QuEChERS结合气象色谱-三重四极杆质谱法快速测定酸肉中10种挥发性N-亚硝胺类化合物[J].色谱,2017,35(10):1086-1093. ZHAO Z, XU Y B, LIU X H, et al. Rapid determination of 10 volatile N-nitrosamines in sour meats by modified QuEChERS and gas chromatography-triple quadrupole mass spectrometry[J]. Chromatography, 2017, 35(10):1086-1093(in Chinese).
[7] WANG B, XIE L H, WANG X Q, et al. Applications of metal-organic frameworks for green energy and environment:New advances in adsorptive gas separation, storage and removal[J]. Green Energy & Environment, 2018, 3(3):191-228. [8] 赵玲, 刘恒恒, 胡晴, 等. 金属有机骨架材料MOF-5催化吸附SO2[J]. 环境化学, 2017, 36(9):1914-1922. ZHAO L, LIU H H, HU Q, et al. Synthesis of MOF-5 catalysts and their catalytic oxidation of sulfur dioxide[J]. Environmental Chemistry, 2017, 36(9):1914-1922(in Chinese).
[9] HASAN Z, CHOI E J, JHUNG S H. Adsorption of naproxen and clofibric acid over a metal-organic framework MIL-101 functionalized with acidic and basic groups[J].Chemical Engineering Journal, 2013, 219(1):537-544. [10] LAREDO G C, VEGA-MERINO P M, MORA-VALLEJO R J, et al. Comparison of the metal-organic framework MIL-101(Cr) versus four commercial adsorbents for nitrogen compounds removal in diesel feedstocks[J]. Fuel, 2016, 180:284-291. [11] 张艳梅,杨力.金属有机骨架材料在污水处理中的应用[J].农业与技术,2014,34(4):13-14. ZHANG Y M, YANG L. Application of Metal Organic Framework Materials in Wastewater Treatment[J]. Agriculture and Technology, 2014, 34(4):13-14(in Chinese).
[12] LUO X P, FU S Y, DU Y M, et al. Adsorption of methylene blue and malachite green from aqueous solution by sulfonic acid group modified MIL-101[J]. Microporous & Mesoporous Materials, 2017, 237:268-274. [13] 陶海军, 黄艳芳, 王子惠,等. 以羧酸盐为有机配体合成金属有机骨架材料MIL-101(Cr)[J]. 南京工业大学学报:自然科学版, 2018, 40(5):40-47. TAO H J, HUANG H F, WANG Z H, et al. Synthesis of MIL-101(Cr) with carboxylate as organic ligand[J]. Journal of Nanjing Tech University(Nature Science Edition), 2018, 40(5):40-47(in Chinese).
[14] 吴天斌,张鹏,马珺,等.超临界流体中制备微孔和介孔结构金属有机框架负载Ru及其催化性能[J].催化学报,2013,34(1):167-175. WU T B, ZHANG P, MA J, et al. Catalytic activity of immobilized Ru nanoparticles in a porous metal-organic framework using supercritical fluid[J]. Chinese Journal of Catalysis, 2013, 34(1):167-175(in Chinese).
[15] 黎兰馨. 亚硝胺的分析化学[J]. 分析化学, 1977, 5(4):65-73. LI L X. Analytical Chemistry of N-nitrosamines[J]. Analytical Chemistry, 1977, 5(4):65-73(in Chinese).
[16] 汤庆会,余沛芝,陆坤, 等. 固相萃取-气相色谱串联质谱测定饮用水中N-亚硝胺类消毒副产物[J]. 净水技术,2018, 37(10):28-32. TANG Q H, YU P Z, LU K, et al. Detection of N-nitrosamine disinfection by-products in drinking water by SPE-GC/MS[J]. Water Purification Technology, 2018, 37(10):28-32(in Chinese).
[17] LIU F J, XIAN Y P, CHEN J W, et al. Determination of eleven volatile N-nitrosamines in skin care cosmetics using multi-walled carbon nanotubes as a dispersive clean-up sorbent and ultrahigh-performance liquid chromatography-atmospheric pressure chemical ionization tandem mass spectrometry[J]. Analytical Methods, 2016,8:4245-4253. [18] 唐雪惠,吴艳芬,李朝晖,等. 超高效液相色谱质谱法测定饮用水中亚硝胺[J]. 化学研究与应用, 2018, 30(7):1190-1196. TANG X H, WU H F, LI C H, et al. Determination of nitrosamies in drinking water by UPLC-MS/MS[J]. Chemical Research and Application, 2018, 30(7):1190-1196(in Chinese).
-

计量
- 文章访问数: 3832
- HTML全文浏览数: 3832
- PDF下载数: 70
- 施引文献: 0