A Review of Rapid Detections for Emerging Contaminants in Groundwater
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摘要:
国内外广泛关注的新污染物主要包括抗生素、内分泌干扰物、全氟或多氟化合物等污染物质，这些污染物通过径流、扩散、渗透等多种途径进入水体环境。由于新污染物多具有生物累积性、生物毒性及环境持久性等特征，对水生生物、人体健康和生态安全构成潜在威胁，存在环境风险，因此，国家对其污染现状开始进行调查。随着中国新污染物污染状况调查评价工作的开展，快速、灵敏的检测方法成为研究热点。本文基于近年文献重点评述了水环境中新污染物的检测方法，并对方法的性能和优缺点作了对比。结果表明：①目前新污染物的检测方法以大型仪器检测方法为主。仪器检测方法的检测浓度低、精度高，对设备的要求高，从采样到测试分析得到结果的周期长，不适用于新污染物的现场快速检测。②传感检测技术和免疫分析技术逐步应用于新污染物的快速检测。其中电化学传感器和酶联免疫分析法相对成熟，应用较多，具有设备简单、检测时间短，灵敏度和精确度良好等优点，可开展现场快速检测。本文认为，①快速检测技术多针对单一污染物进行检测，而实现同时检测多种污染物质还需进一步研究；②多种检测技术相结合可以达到更好的检测效果，是未来新污染物检测的发展方向；③利用新型材料改良检测方法、降低检出限、提高灵敏度和精确度实现新污染物快速检测是未来研究的难点和重点。
Abstract:In recent years, emerging contaminants, such as antibiotics, endocrine disruptors, perfluorinated and polyfluoroalkyl substances, are of great worldwide concern. These contaminants enter the water environment through runoff, diffusion, infiltration and other ways. Due to their bioaccumulation, biological toxicity, and environmental sustainability, emerging contaminants pose a potential threat to aquatic organisms, human health, and ecological safety[1]. Therefore, it is urgent to detect and investigate the pollution status of emerging contaminants in the water environment. Many investigations and evaluations have been carried out, making rapid detection methods a research hotspot. The detection methods of emerging contaminants in the water environment based on recent literature is reviewed, comparing the advantages and disadvantages of the emerging contaminants detection methods, summarizing the research progress of rapid detection technology for emerging contaminants in water, and prospecting its development trend. Emerging contaminants were widely detected in the water environment. For instance, antibiotics have been detected in groundwater in cities such as Harbin[2] and Shijiazhuang[3], in surface rivers such as the Fuyang River and Qin River[4], and in the source water such as Yichang City[5] and the Tuojiang River Basin[6], as well as in groundwater from major urban-rural settings of Pakistan[8]. Similarly, endocrine disruptors have been detected in different types of water in China, such as the Minjiang River Basin[11], as well as in groundwater of the Wuxi—Changzhou region[9] and Xuzhou region[10]. Some endocrine disruptor pollutants have been detected in seawater along the Romanian Black Sea coast[12]. In addition, perfluorinated and polyfluoroalkyl substances have been detected in the surface water of Beijing’s reclaimed groundwater irrigation area[13] and in Hongze Lake[15]. There is perfluoroalkyl acid pollution in the groundwater environment of farmland in some regions of Hainan Province[14]. Perfluorinated compounds have also been detected in major Southern Indian rivers[16]. There are emerging contaminants in the water environment both domestically and internationally. The concentrations and detection rates are high in some areas, posing a serious threat to groundwater and surface water resources. Nowadays, the emerging contaminants are mainly detected in the laboratory using advanced instruments. The emerging contaminants are widely present in the environment, but their concentrations are quite low, of which the content is in the nanogram to microgram level. In order to reduce the detection limits, the emerging contaminants samples will be concentrated and then tested using high-resolution instruments. Instrument detection technology has the advantages of high throughput, high accuracy, low detection limit, and low false positive rate. While the pre-treatment of samples is very complex, and the analytical instruments used are costly, this is not something that all laboratories can afford. Therefore, the analysis of emerging contaminants takes a long time from sampling to getting analysis results. Sensor detection technology is a commonly used on-site detection method in the field of environmental monitoring. It mainly includes electrochemical, optical, and biological sensing. The field rapid detection of emerging contaminants in water environment is a promising research direction. Electrochemical sensing has been extensively studied. Sensor detection technology can give results in minutes for emerging contaminants. However, most of the work was focused on detecting a single contaminant; significant progress has been made in the laboratory, but it has not yet been promoted for field testing; there were fewer examples of field rapid detection of emerging contaminants. Further research is needed on the technology for simultaneously determining multiple emerging contaminants in the meantime. Immunoassay detection technology is suitable for on-site rapid screening of emerging contaminants in the water environment. Enzyme linked immunosorbent assay can preliminarily screen for the emerging contaminants in the water environment, while immunochromatography can perform qualitative or semi-quantitative detection of emerging contaminants. Immunoassay technology has high specificity, strong sensitivity, simplicity, convenience, and no need for expensive instruments. It has great advantages in rapid detection of large amounts of samples and on-site detection. However, it is prone to false negatives and positives[89]. There are various types of rapid detection methods for emerging contaminants. Further, the focus of research should be on utilizing new materials to improve traditional detection methods to meet the needs of rapid and on-site detection of contaminants. Besides, researchers could combine multiple detection techniques to make detection methods simpler, faster, and more cost-effective, and with high sensitivity and accuracy to achieve rapid detection of multiple pollutants simultaneously.
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Keywords:
- emerging contaminants /
- rapid detection /
- instrument detection /
- sensor /
- immunoassay
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表 1 仪器检测技术可检测抗生素种类及其性能
Table 1 The antibiotics types and performance of instrument detection technology that can be detected.
检测方法 仪器设备 可检测抗生素种类 检出限 RSD(%) 参考文献 毛细管电泳
(CE)高效毛细管电泳仪 磺胺类、喹诺酮类、四环素类等 0.4～1.0μg/L − ［17−18］ 高效液相色谱法
(HPLC)高效液相色谱-
串联质谱仪磺胺类、喹诺酮类、大环内酯类、四环素类、
氯霉素类等七大类0.06～2.28ng/L − ［19］ 高效液相色谱-串联
紫外／荧光检测器磺胺类、喹诺酮类、氯霉素类等 4.2～22.8μg/L − ［20］ 液相色谱-质谱联用法
(LC-MS)液相色谱-串联质谱仪 磺胺类、喹诺酮类、大环内酯类、
四环素类等0.15～0.9ng/L 0.36～2.25 ［21−22］ 液相色谱仪；
三重四极杆质谱仪磺胺类、喹诺酮类、大环内酯类、
四环素类等1.2～15ng/L ＜22 ［23］ 高效液相色谱-串联质谱法
(HPLC-MS/MS)三重四级杆质谱仪；
高效液相色谱仪磺胺类、喹诺酮类、大环内酯类、
头孢霉素类等0.0056～3.9675ng/L ＜11 ［24−25］ 高效液相色谱-
串联质谱仪喹诺酮类 0.1μg/L 0.71～12.80 ［26］ 超高效液相色谱-
串联质谱法
(UPLC-MS/MS)超高效液相色谱仪；
三重四极杆质谱仪磺胺类、喹诺酮类、大环内酯类、
四环素类、氯霉素类等七大类0.01～10.6ng/L ≤16 ［27−30］ 
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表 2 仪器检测技术可检测内分泌干扰物种类及其性能
Table 2 The environmental endocrine disruptors types and performance of instrument detection technology that can be detected.
检测方法 仪器设备 可检测内分泌干扰物种类 检出限 RSD(%) 参考文献 气相色谱-质谱
联用法
(GC-MS)气相色谱-质谱仪 类固醇类、酚类等 0.5～140ng/L 2.54～5.36 ［31］ 高效液相色谱法
(HPLC)高效液相色谱仪-串联荧光检测器 三氯生、β-雌二醇、壬基酚和4-辛基酚 1.1～1.9ng/L − ［32−33］ 高效液相色谱仪 邻苯二甲酸二丁(辛)酯 0.1μg/L ＜4.47 ［34］ 高效液相色谱仪-串联二极管阵列检测器 三氯生、三氯卡班和甲基三氯生 0.05～0.2μg/L ＜10 ［35］ 高效液相色谱-
串联质谱法
(HPLC-MS/MS)高效液相色谱仪；质谱仪 对乙酰氨基酚等17种 0.07～1.88ng/L − ［36］ 高效液相色谱系统；
三重四极杆质谱仪黄体酮代谢物、类固醇类、酚类等 0.02～50ng/L ＜15 ［37−39］ 超高效液相色谱
串联质谱法
(UPLC-MS/MS)超高效液相色谱-串联质谱仪 雌激素类、雄激素类、肾上腺皮质激素类、
酚类和非甾类激素类等0.05～2.00ng/L 0.99～12.0 ［40−41］ 超高效液相色谱系统；三重四极杆质谱仪 酚类、黄体酮等 0.03ng/L～5.0μg/L ≤11.6 ［42−44］
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表 3 仪器检测技术可检测全氟化合物种类及其性能
Table 3 The perfluorinated and polyfluoroalkyl substances types and performance of instrument detection technology that can be detected.
检测方法 仪器设备 可检测全氟化合物种类 检出限 RSD(%) 参考文献 气相色谱-质谱
联用法
(GC-MS)气相色谱-质谱仪 中性全氟烷基化合物、
全氟羧酸化合物等0.02ng/L～1.5μg/L ＜14.5 ［46-47］ 液相色谱-质谱联用法
(LC-MS/MS)液相色谱仪；
三重四极杆质谱仪全氟辛烷磺酸等22种以上
全氟烷基化合物0.16～5.13ng/L 3～18 ［48-49］ 高效液相色谱-串联质谱法
(HPLC-MS/MS)高效液相色谱仪；质谱仪 全氟辛烷磺酸等21种全氟化合物 0.01～0.08ng/L 1.1～11.2 ［50］ 超高效液相色谱-串联质谱法
(UPLC-MS/MS)超高效液相色谱-串联四极杆
质谱仪全氟羧酸、全氟磺酸、全氟醚羧酸等
57种以上全氟化合物0.01ng/L～0.1μg/L 0.4～23.0 ［51-53］ 超高效液相色谱-质谱仪 全氟丁烷磺酸、全氟辛酸和全氟
辛烷磺酸等16种以上全氟化合物0.06ng/L～0.25μg/L 2.1～9.19 ［54-56］
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表 4 水中新污染物传感检测技术优缺点对比
Table 4 Comparison of advantages and disadvantages of emerging contaminants sensor detection methods for water samples.
传感检测技术 优点 缺点 电化学传感 操作简单，成本低廉，分析速度快，仪器体积小，
易携带，适用于现场检测检出限较高，电极构造耗时、繁琐，电极易被污染，
需定期更换电极光学传感 操作简单，成本低，可实时检测 灵敏度一般，容易受环境干扰，使用寿命较短，
大多只能对特定污染物进行检测生物传感 操作简单，费用低，适用于批量样品快速筛选 易受到水样中其他物质干扰，专一性和精确度不足
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表 5 不同类别新污染物可选择的快速检测方法总结
Table 5 Summary of emerging contaminants that can be detected by rapid detection methods.
快速检测技术分类 方法名称 抗生素类 全氟化合物类 内分泌干扰物类 传感检测技术 电化学传感 √ √ √ 光学传感 √ √ √ 生物传感 √ √ √ 免疫检测技术 酶联免疫分析法 √ √ √ 免疫层析法 − − √ 其他快速检测技术 平面波导免疫传感器 √ − √ 荧光免疫生物传感器 − − √ 阵列倏逝波荧光传感器 − − √ 单扫描极谱 − √ − 原位显色反应 − − √ 注：“−”表示该类新污染物不涉及。
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