表面增强拉曼光谱检测二噁英类化合物研究进展

doi:10.6023/A19040139

化学学报 ›› 2019, Vol. 77 ›› Issue (10): 977-983.DOI: 10.6023/A19040139 上一篇下一篇

综述

表面增强拉曼光谱检测二噁英类化合物研究进展

程劼, 王培龙^*(), 苏晓鸥^*()

中国农业科学院农业质量标准与检测技术研究所北京 100081

投稿日期:2019-04-22 发布日期:2019-06-05
通讯作者: 王培龙,苏晓鸥 E-mail:wplcon99@163.com;suxiaoou@caas.cn
作者简介:程劼, 博士, 副研究员, 中国农业科学院农业质量标准与检测技术研究所, 二噁英污染研究室. 主要从事SERS快速分析技术、POPs迁移转化规律等研究. 发表SCI论文20余篇, 授权发明专利6项, 省部级奖励3项.|王培龙, 博士, 研究员, 中国农业科学院农业质量标准与检测技术研究所, 二噁英污染研究室. 主要从事饲料及畜产品质量安全及POPs分析毒理研究. 近年来发表SCI论文30余篇, 授权发明专利4项, 省部级奖励5项.|苏晓鸥, 博士, 二级研究员, 中国农业科学院农业质量标准与检测技术研究所. 主要从事饲料及畜产品质量安全检测技术研究. 发表SCI论文80余篇, 授权国家发明专利10项, 制定国家和农业行业标准10余项, 出版专著8部.
基金资助:
项目受国家十三五重点研发计划(2017YFC1600301);中国农业科学院基本科研业务费资助(1610072017006)

Recent Progress on the Detection of Dioxins Based on Surface-enhanced Raman Spectroscopy

Cheng, Jie, Wang, Peilong^*(), Su, Xiaoou^*()

Institute of Quality Standards and Testing Technologies for Agro-products, Chinese Academy of Agricultural Sciences,Beijing 100081

Received:2019-04-22 Published:2019-06-05
Contact: Wang, Peilong,Su, Xiaoou E-mail:wplcon99@163.com;suxiaoou@caas.cn
Supported by:
Project supported by the 13th five-year development plan of China by the National Key Research and Development Program(2017YFC1600301);the Fundamental Research Funds for Central Non-profit Scientific Institution, Chinese Academy of Agricultural Sciences(1610072017006)

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摘要/Abstract

以二噁英及二噁英类多氯联苯为代表的持久性有机污染物(POPs), 具有致畸、致癌、致突变的性质, 被国际癌症研究中心列为人类一级致癌物. POPs通过环境进入食物链对食品安全造成威胁和影响. 以表面增强拉曼光谱(SERS)为代表的新型快速检测技术具有高灵敏分析的特点. 本综述总结了近年来基于SERS技术分析POPs的研究进展, 归纳了不同类型增强基底, 提出了SERS分析POPs的若干关键技术难点, 并对未来SERS技术在POPs分析方面的发展进行了展望.

关键词: 表面增强拉曼光谱, 二噁英, 增强基底, 检测

Persistent Organic Pollutants (POPs), represented by dioxins and dioxin-like polychlorinated biphenyls have the property of teratogenic, carcinogenic and mutagenic, which have been classified as Group A human carcinogen by the international agency for research on cancer (IARC) and put into the initial list of Stockholm Convention managed by the United Nations Environment Program. POPs have posed a threat and impact on food security through the food chain from environment. The conventional detection methods, such as liquid chromatography-tandem mass spectrometry, high resolution gas chromatography-mass spectrometry and two-dimensional gas chromatography with time-of-flight mass spectrometry are sufficiently accurate, but fail to meet the requirements of on-site detection. Meanwhile, the rapid testing technologies for PCBs mainly included fluorescence detection, electrochemical sensors, and so on. As a new type of rapid detection technology, Surface-enhanced Raman Spectroscopy (SERS) has attracted significant attention as a promising analytical technique. With its ultra-sensitivity, high speed detection, ease of operation, SERS is particularly well-suited for the rapid detection of POPs. However, the multiple molecules in matrices may generate interfering Raman signals via competitive adsorption with the target compound on the substrate surface in the SERS detection of real samples. In addition, reproducibility represents a major bottleneck for the widespread application of SERS. Metal nanoparticle colloids are widely used as SERS substrates due to the hot spots formed between the nanoparticles. However, metal nanoparticle aggregation in colloidal solutions is difficult to control, leading to the random formation of hot spots. When the target POPs exist near the hot spots, the intensities of the enhanced Raman signals were unstable. Other factors influenced by the chemical adsorption such as vibration, charge transfer, and the deformation or distortion of molecules also affect the Raman signals. In the review, we provide an overview of the recent advances in SERS for POPs determination, especially the different types of enhanced substrates. And several key technical points of SERS detection including sensitivity, selectivity, and reproducibility have been summarized. Finally, the development of SERS for POPs detection in the future are proposed.

Key words: surface-enhanced Raman spectroscopy, dioxins, enhanced substrates, detection

引用此文

程劼, 王培龙, 苏晓鸥. 表面增强拉曼光谱检测二噁英类化合物研究进展[J]. 化学学报, 2019, 77(10): 977-983.

Cheng, Jie, Wang, Peilong, Su, Xiaoou. Recent Progress on the Detection of Dioxins Based on Surface-enhanced Raman Spectroscopy[J]. Acta Chimica Sinica, 2019, 77(10): 977-983.

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图/表 7

同系物	毒性当量	同系物	毒性当量
二噁英及呋喃 (PCDD/Fs)		二噁英类多氯联苯 (DL-PCBs)
2,3,7,8-TCDD	1
1,2,3,7,8-PeCDD	1	Non-ortho PCBs
1,2,3,4,7,8-HxCDD	0.1	PCB-77	0.0001
1,2,3,6,7,8-HxCDD	0.1	PCB-81	0.0003
1,2,3,7,8,9-HxCDD	0.1	PCB-126	0.1
1,2,3,4,6,7,8-HpCDD	0.01	PCB-169	0.03
OCDD	0.0003
		Mono-ortho PCBs
2,3,7,8-TCDF	0.1	PCB-105	0.00003
1,2,3,7,8-PeCDF	0.03	PCB-114	0.00003
2,3,4,7,8-PeCDF	0.3	PCB-118	0.00003
1,2,3,4,7,8-HxCDF	0.1	PCB-123	0.00003
1,2,3,6,7,8-HxCDF	0.1	PCB-156	0.00003
1,2,3,7,8,9-HxCDF	0.1	PCB-157	0.00003
2,3,4,6,7,8-HxCDF	0.1	PCB-167	0.00003
1,2,3,4,6,7,8-HpCDF	0.01	PCB-189	0.00003
1,2,3,4,7,8,9-HpCDF	0.01
OCDF	0.0003

表1. 29种二噁英类化合物及TEF值

Table 1. TEF for 29 dioxin-like compounds (dioxin, furans and DL-PCBs)

图1. 二噁英类POPs化合物迁移途径

Figure 1. Carry-over of dioxins

图2. SERS增强示意图

Figure 2. Schematic diagram of SERS

图3. 3D热点纳米结构组装

Figure 3. Schematic image of the fabrication of 3D hotspots SERS substrate

目标物	修饰官能团	基质	灵敏度(mol?L^–1)	文献
PCB-47, -77	alkanethiol	标液	10^–11	[45]
PCB-40, -54, -65, -80	β-CD	土壤	—^a	[50]
PCB-77	β-CD	标液	10^–10	[51]
PCB-3, -29, -77	β-CD	标液	10^–6	[46]
PCB-77	HS-β-CD	标液	10^–7	[47]
PCB-47	GSH	土壤	—	[48]
PCB-77	aptamer	标液	10^–8	[36]
PCB-77	aptamer	标液	3.3×10^–8	[37]
PCB-77	aptamer	标液	10^–6	[52]
PCB-47, -52, -77	rGO	标液	10^–7	[49]
PCB-3, -77	GO	标液	10^–4	[53]

表2. 基底表面修饰类型

Table 2. Kinds of modification on the surface of SERS substrates

图4. (a) 烷硫醇修饰; (b) 环糊精修饰

Figure 4. (a) Alkanethiol modification; (b) β-CD modification

图5. (a) PCB-77在基底表面吸附; (b) PCB-77-SCH3在基底表面吸附; (c)基底SEM图; (d) 5×10–3~5×10–6 mol?L–1浓度范围内PCB-77的SERS谱图; (e) 5×10–3~5×10–8 mol?L–1浓度范围内PCB-77-SCH3的SERS谱图

Figure 5. (a) The adsorption of PCB-77 on the base surface; (b) The adsorption of PCB-77-SCH3 on the base surface; (c) The SEM images of substrates; (d) SERS spectra of PCB-77 at concentrations of 5×10–3~5×10–6 mol?L–1. (e) SERS spectra of PCB-77-SCH3 at concentrations of 5×10–3~5×10–8 mol?L–1

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表面增强拉曼光谱检测二噁英类化合物研究进展

Recent Progress on the Detection of Dioxins Based on Surface-enhanced Raman Spectroscopy

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