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化学进展 2019, Vol. 31 Issue (1): 191-200 DOI: 10.7536/PC180527 前一篇   后一篇

• 综述 •

金属-有机骨架及其功能材料在食品和水有害物质预处理中的应用

白蕾1,2, 王艳凤1,2, 霍淑慧1,2,**(), 卢小泉1,2,**()   

  1. 1. 西北师范大学化学化工学院 兰州 730070
    2. 甘肃省生物电化学与环境分析重点实验室 兰州 730070
  • 收稿日期:2018-05-21 修回日期:2018-07-01 出版日期:2019-01-15 发布日期:2018-10-20
  • 通讯作者: 霍淑慧, 卢小泉
  • 基金资助:
    国家自然科学基金项目(21305112); 甘肃省自然科学基金项目(No.)(18JR3RA085); 国家自然科学基金项目(No.21305112)、甘肃省自然科学基金项目(No.18JR3RA085)和甘肃省高等学校科研项目资助(2015A-027)
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Application of Food and Water Samples Pretreatment Using Functional Metal-Organic Frameworks Materials

Lei Bai1,2, Yanfeng Wang1,2, Shuhui Huo1,2,**(), Xiaoquan Lu1,2,**()   

  1. 1. College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070, China
    2. Key Laboratory of Bioelectrochemistry & Environmental Analysis of Gansu Province, Lanzhou 730070, China;
  • Received:2018-05-21 Revised:2018-07-01 Online:2019-01-15 Published:2018-10-20
  • Contact: Shuhui Huo, Xiaoquan Lu
  • About author:
    ** Corresponding author e-mail: (Shuhui Huo);
    (Xiaoquan Lu)
  • Supported by:
    The work was supported by the National Natural Science Foundation of China(21305112); The Natural Science Foundation of Gansu Province(18JR3RA085); The Research Projects of Gansu Universities(2015A-027)

食品安全问题是关系人民生命健康和经济社会和谐发展的重大问题。食品类样品残存的痕量有毒有害物质对人体健康产生潜在危害。因此,需要高效的吸附材料用于食品类样品预处理及检测。金属-有机骨架材料(metal-organic frameworks, MOFs) 是一类新型的多孔功能材料,具有高孔隙度、高比表面积、结构可设计与调控、孔径可调及良好的化学和热稳定性等优点。MOFs的早期研究主要集中在结构及功能化设计方面,近年来MOFs及其功能材料在各领域的潜在应用逐渐成为新的研究热点。MOFs具有高度发达的孔隙结构,易通过功能化改变材料表面性质,不同的金属元素和配体种类,以及配位方式的多样化特性,极大地丰富固相萃取的固定相材料种类。尤其是在复杂基质样品预处理中,MOFs及其功能材料表现出强富集能力、强抗基质干扰能力、优异的选择性以及环境友好等优势。本文综述了近几年MOFs及其功能材料在食品和水样品中有害物质预处理方面的研究进展,并对这类材料应用在食品安全分析方面的发展进行了展望。

关键词： 金属-有机骨架, 功能材料, 样品预处理, 食品安全检测

Food safety has received great attention due to its close connectivity with people’s health and the harmonious development of national economy and society. Trace amount of toxic and harmful compounds in food and water are potentially harmful to human health. Excellent adsorbent and efficient extraction have received more and more attention in food safety detection. Metal-organic frameworks (MOFs) are an emerging class of porous functional materials with high porosity, large surface area, easy structural design, adjustable pore size, as well as acceptable chemical and thermal stability. In the past, the research on MOFs mainly focused on the structural design. Recently, more and more attention has been focused on applications of MOFs in food safety analysis. Meanwhile, their high porosity, tunable surface functionalities, various metal and ligands, as well as diverse coordination modes make MOFs promising as adsorption material for SPE. The merits of MOFs and their functional materials, in particular, are high enrichment, excellent matrix interference resistance, good selectivity, and environmentally-friendly development. Interesting research of MOFs and their functional materials in the pretreatment of food and water samples are summarized.

Key words: metal-organic frameworks, functional materials, sample pretreatment, food safety analysis
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表1 固相萃取在食品痕量重金属检测中的应用[40,41,42,43,44,45,46,47,48,49,50,51]
Table 1 SPE for the detection of trace heavy metal in food samples[40,41,42,43,44,45,46,47,48,49,50,51]
MOFs Analyte Mode Samples LOD (μg·L-1) Recovery (%) ref
Cu3(BTC)2 Cd(Ⅱ), Pb(Ⅱ), Ni(Ⅱ), Zn(Ⅱ) MSPE-FAAS tap, river, mineral and seawater. soil, sediment and fish extracts 0.12~1.2 88.0~104.0 40
Cu3(BTC)2 Cd(Ⅱ), Zn(Ⅱ), Pb(Ⅱ) MSPE-FAAS baby food 25 93.0~106.0 41
Cu3(BTC)2 Cd(Ⅱ), Pb(Ⅱ), Zn(Ⅱ), Cr(Ⅲ) MSPE-FAAS vegetable 0.12~0.7 92.5~106.0 42
Cu3(BTC)2 Cd(Ⅱ), Pb(Ⅱ), and Ni(Ⅱ) MSPE-FAAS sea food and agri food 0.15~0.8 94.6~102.2 43
Cu3(BTC)2 Hg(Ⅱ) MSPE-CVAAS fish and canned tuna 0.06~60 95.1~102.0 44
MIL-101(Fe) Cd(Ⅱ), Pb(Ⅱ), Zn(Ⅱ), Cr(Ⅲ) MSPE-FAAS agricultural (leek, radish, basil) after microwave digestion 0.15~0.8 87.3~110 45
MIL-101(Fe) Cd(Ⅱ), Pb(Ⅱ), Co(Ⅱ), Ni(Ⅱ), MSPE-FAAS fish 0.13~0.5 88.8~108.0 46
TMU-8 Co(Ⅱ), Cu(Ⅱ), Pb(Ⅱ), Cd(Ⅱ), Ni(Ⅱ), Cr(Ⅲ), Mn(Ⅱ) MSPE-FI-ICP-AES fruit samples and tea 0.3~1 91.0~108.0 47
MOF-199 As(III)and As(V) MSPE-ETAAS rice and canned tuna 1.2 84.0~103.0 48
JUC-62 Hg(Ⅱ) SPE-AFS tea and mushroom 0.40 90.0~93.3 49
PCN-222/
MOF-545		 Hg(Ⅱ) Pipette-Tip SPE-CVAAS fish 0.020 74.3~98.7 50
MOF-545 Pb(Ⅱ) vortex assisted SPE-FAAS cereal, beverage and water 1.78 92~107 51
图1 (a)双硫腙功能化的Fe3O4合成示意图;(b)磁性MOF-DHz纳米复合材料的合成示意图[40]
Fig.1 (a) A schematic diagram of dithizone functionalized Fe3O4synthesis. (b) The schematic illustration of synthesis of magnetic MOF-DHz nanocomposite[40]
图2 PCN-222/MOF-545的结构[50]
Fig.2 Molecular representations of PCN-222/MOF-545[50]
表2 固相萃取在食物样品抗生素和激素检测中的应用[52,53,54,55]
Table 2 SPE for the detection of antibiotics and hormones in food samples[52,53,54,55]
MOF Analyte Mode Samples LOD
(μg·L-1)		 Recovery (%) ref
MIL-101(Cr), MIL-100(Cr), MIL-100 (Fe), MIL-100(Al), UIO-66(Zr), MIL-88B(Cr) penicillin SPME- CEC-UV PENG, PENV, OXA, CLOX, NAFC and DICL 1.2~4.5 63~96.2 52
MIL-53 (Al) penicillin SPME- nano Acquity UPLC river water and milk 0.06~0.26 80.8~90.9 53
MOF-5 estrogens SPME- HPLC milk 0.17~0.31 73.1~80.6 54
MOF-5 chloramphenicol,
thiamphenicol		 SPME- GC-FID milk, honey, urine and serum 0.0148~0.0195 82.3~103.2 55
表3 固相萃取在食物样品农药检测中的应用[58,59,60,61]
Table 3 SPE for the detection of pesticides in food samples[58,59,60,61]
MOF Analyte Mode Samples LOD Recovery (%) ref
MIL-101(Cr) herbicides DSPE- HPLC peanuts 0.98~1.9 ng·g-1 89.5~102.7 58
ZIF-8 benzoylurea insecticides DSPE- HPLC water and tangerine 0.10~0.23 ng mL-1 91.7~107.9 59
MIL-101(Cr) amphenicols and their
metabolites		 vortex assisted D-μ-SPE- UPLC-MS / MS aquaculture water 0.05~0.15 ng mL-1 70.1~109.2 60
UiO-66-NH2 Chlorophenoxy acids
herbicides		 D-μ-SPE- HPLC vegetables 0.16~0.37 ng·g-1 82.3~102.0 61
图3 制备MOF-C过程(A)及固相萃取甲酰脲类杀虫剂(B)[59]
Fig.3 Procedures of the preparation of MOF-C (A) and dispersive solid-phase extraction for benzoylurea insecticides (B)[59]
表4 固相萃取在食品和水持久性有机污染物检测中的应用[63,64,65,66,67,68,69]
Table 4 SPE for the detection of persistent organic pollutants in food and water samples[63,64,65,66,67,68,69]
MOF Analyte Mode Samples LOD Recovery (%) ref
MOF-5(Fe) PCBs SBSE-GC-MS fish 0.061~0.096 ng·g-1 94.3~97.5 63
MOF-5 PCBs Aptamer-functionalized
SBSE-GC-MS		 fish 3.0~4.0 ng·L-1 89.2~97.1 64
Bio-MOF-1 PAHs SPME-GC-FID water 0.02~5.57 μg·L-1 80.0~115 65
Magnetic MIL-101 PAHs MSPE-GC-FID water 2.8~27.2 ng·L-1 83.6~105 66
Magnetic MIL-100 PAHs MSPE-GC-FID water 4.6~8.9 ng·L-1 88.5~106.6 67
HKUST-1 PAHs M-d-μ-SPE- UHPLC-FD waters and fruit tea infusions 0.8 ng·L-1 75.0~94.0 68
MIL-101 and MOF-5 PAHs MSPE- GC-MS/ MS waters, food and PM2.5 0.03~0.30 ng·L-1 71.2~109.7 69
图4 锈钢纤维丝水热法原位制备SPME双配体MOF bio-MOF-1 涂层[65]
Fig.4 锈钢纤维丝水热法原位制备SPME双配体MOF bio-MOF-1 涂层[65]
图5 扫描电镜图:不锈钢丝纤维(A); bio-MOF-1 涂层SPME纤维(B、C);bio-MOF-1纤维成分分析(D-G)的[65]
Fig.5 SEM images of (A) stainless steel wire; (B) and (C) bio-MOF-1 SPME fiber. EDS elemental mapping images for bio-MOF-1 SPME fiber (DG)[65]
图6 Fe3O4@SiO2-MIL-101 MNPs作为MSPE吸附剂的示意图[66]
Fig.6 Schematic diagram for the application of Fe3O4@SiO2-MIL-101 MNPs as sorbent for MSPE[66]
图7 (A) MIL-100的热解原位磁化的示意图; (B) MSPE的分析过程图[67]
Fig.7 Schematic diagram of pyrolytic in situ magnetization of MIL-100 (A) and analytical procedures for MSPE. (B)[67]
图8 MOF@MON的合成和固相微萃取纤维的制备[69]
Fig.8 Synthesis of MOF@MON and fabrication of solid-phase microextraction fibers[69]
图9 MIL-101(a)和MIL-101@DMIP(b)的扫描电子显微图[72]
Fig.9 Scanning electron micrographs of MIL-101(a) and MIL-101@DMIP(b)[72]
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