基于纳米材料的食品安全与品质快速检测方法的研究
发布时间：2018-08-11 20:40
【摘要】：由于食品安全事件的频繁曝光,人们对于食品安全与品质的关注程度与日俱增。传统的实验室检测方法,虽然具有灵敏度高、检测结果准确可靠等优点,但是同样存在着检测周期长,样品前处理过程复杂繁琐,检测通量较低,仪器设备维护成本高,需要专业人员操作等不足,已无法满足目前食品安全与品质的检测需求。电化学分析技术具有成本低廉、方便、易于操作、仪器易于自动化和小型化、灵敏度高、选择性好等特点。酶联免疫分析技术具有特异性好,简单方便,易于实现自动化等优势。 本论文综合使用了纳米技术、电化学分析技术、酶联免疫分析技术、磁分离技术等诸多领域的知识,开发了针对不同检测对象的食品安全与品质的快速检测方法。使用功能性材料离子液体作为粘合剂替代传统的石蜡油来构建碳糊(carbon paste, CP)电极,并将其应用于茶叶中抗氧化剂表没食子儿茶素没食子酸酯(epigallocatechin gallate, EGCG)的快速检测；在碳糊离子液体(ionic liquid carbon paste, ILCP)电极的基础之上,使用本体改性的方法在碳糊中掺杂金纳米颗粒(Au nanoparticle, Au NP),制备出金纳米颗粒修饰的碳糊离子液体(Au NP-ILCP)电极,该电极被用于快速检测肉制品中的亚硝酸盐残留；成功使用丝网印刷技术制备了碳纳米管与离子液体修饰的丝网印刷电极,并研究了该电极在重金属离子快速检测方面的性能；制备了磁珠微纳颗粒,并通过化学修饰与生物结合的方式制备了免疫磁珠,引入了核酸纯化系统,并使用竞争免疫的原理,实现了对肉制品中瘦肉精克伦特罗(clenbuterol, CLB)的快速检测。本文为电化学分析检测技术中电极的制备和修饰方法提供了数据支持,为酶联免疫分析技术的应用提供了一种新的思路,对于研发具有自主知识产权的食品安全与品质快速检测仪器具有借鉴意义。 本文主要研究内容、结果和结论如下： (1)使用本体改性的方法制备了以功能材料离子液体为原料的CP电极,并将该电极用于茶叶中主要抗氧化剂EGCG的快速检测。ILCP电极在最优条件下对于EGCG的检测性能如下所示：1)对EGCG的检测范围为5×10-7～1.25×10-5mol/L,检测下限为1.32×10-7mol/L;2) ILCP电极能连续检测EGCG浓度的变化,具有显著的抗钝化效果；3)ILCP电极对于的常见EGCG类似物具有抗干扰特性；4)ILCP电极对EGCG的检测具有一致性、重现性和稳定性；5) ILCP电极能成功用于实际样本茶汤中EGCG的检测。 (2)使用本体改性的方法将纳米材料Au NP引入到ILCP电极中,成功制备了AuNP-ILCP电极,并使用Au NP-ILCP电极对实际样本中的亚硝酸盐残留实现了快速检测。Au NP-ILCP电极在最优的条件下对于亚硝酸盐的检测性能如下所示：1)检测范围分别为1.0×10-4～1.0×10-3mol/L(循环伏安法(cyclic voltommetry, CV))、1.0×10-6～2.0×10-4mol/L(差分脉冲伏安法(differential pulse voltommetry, DPV))以及7.6×10-6～1.4×10-4mol/L(电流时间曲线法(chronoamperometry, CA));2) Au-ILCP电极具备较强的抗干扰能力；3) Au NP-ILCP电极具备一致性、重现性和稳定性以及抗钝化能力。 (3)使用免疫磁珠结合核酸分离纯化系统的磁珠自动运输的功能,实现了对肉类实际样本(猪肉、猪肝)中瘦肉精CLB的快速检测分析。实验结果表明：1)磁珠形貌为球形,且粒径均一、单分散性较好,平均粒径为509nm；2)修饰后的磁珠仍然保持很强的磁性,在外界磁场的作用下,在1-2s内迅速完成磁分离；3)整个检测过程共耗时25min,线性检测范围为0.14～45.5ppb；4)将该检测体系用于肉类实际样品(猪肉、猪肝)的回收率测试,猪肉和猪肝中盐酸克伦特罗的回收率分别为98.1%-106.1%,94.2%-109.0%。 (4)使用碳纳米管以及离子液体作为功能材料制备了一种新型的丝网印刷(screen printed, SP)电极,并将其用于肉制品中的重金属离子Pb2+和Cd2+残留的快速检测。SP电极对于重金属离子Pb2+和Cd2+的检测性能如下：1)Pb2+的线性响应范围为1.0～100.0ppb,Cd2+的线性响应范围为1.0～100.0ppb;2)干扰实验的结果表明当溶液中的常见离子浓度200倍于Pb2+和Cd2+时,Pb2+和Cd2+离子的电流响应变化小于5%。同时新型的SP电极还具有较好的一致性和稳定性。3)使用新型的SP电极对午餐肉以及火腿肠中的Pb2+和Cd2+成分进行回收率测试,午餐肉中Pb2+和Cd2+的回收率为97.1%-102.9%,98.8%-103.0%,火腿肠中Pb2+和Cd2+的回收率为98.5%～106.5%,96.0%-103.5%。
[Abstract]:Because of the frequent exposure of food safety incidents, people pay more and more attention to food safety and quality. Although traditional laboratory testing methods have the advantages of high sensitivity, accurate and reliable detection results, they also have the advantages of long detection cycle, complex sample pretreatment process, low detection flux, instrument and equipment maintenance. The electrochemical analysis technology has the characteristics of low cost, convenience, easy operation, easy automation and miniaturization of the instrument, high sensitivity and good selectivity. The enzyme-linked immunoassay technology has good specificity, simple and convenient, easy to realize. Automation and other advantages.
In this paper, nanotechnology, electrochemical analysis technology, enzyme-linked immunoassay technology, magnetic separation technology and many other fields of knowledge were used to develop a rapid detection method for food safety and quality of different detection objects. Ase (CP) electrode was applied to the rapid detection of epigallocatechin gallate (EGCG) in tea, and Au nanoparticles (Au N) were doped into the carbon paste by bulk modification on the basis of ionic liquid carbon paste (ILCP) electrode. Carbon paste ionic liquid (Au NP-ILCP) electrode modified with gold nanoparticles was prepared, which was used for rapid detection of nitrite residues in meat products. Silk screen printing electrode modified with carbon nanotubes and ionic liquids was successfully prepared by silk screen printing technology, and its performance in rapid detection of heavy metal ions was studied. In this paper, the preparation and modification of electrodes for electrochemical analysis of clenbuterol (CLB) in meat products were studied. The method provides data support and provides a new idea for the application of enzyme-linked immunoassay (ELISA), which can be used for reference in the research and development of food safety and quality rapid detection instrument with independent intellectual property rights.
The main contents, results and conclusions are as follows:
(1) The CP electrode based on ionic liquids was prepared by bulk modification and used for the rapid detection of EGCG in tea. Under the optimal conditions, the detection performance of ILCP electrode for EGCG was as follows: 1) The detection range of EGCG was 5 - 7 mol / L; 2) ILCP electrode can continuously detect the concentration of EGCG changes, has a significant anti-passivation effect; 3) ILCP electrode for common EGCG analogues has anti-interference characteristics; 4) ILCP electrode detection of EGCG has consistency, reproducibility and stability; 5) ILCP electrode can be successfully used in the actual sample of tea soup EGCG detection.
(2) AuNP-ILCP electrode was successfully prepared by introducing nano-AuNP into ILCP electrode by bulk modification method, and nitrite residue in real samples was rapidly detected by AuNP-ILCP electrode. The detection performance of AuNP-ILCP electrode for nitrite under the optimal conditions was as follows: 1) The detection range was 1. 0 6550 Very consistent, reproducible and stable, and anti passivation capability.
(3) Immunomagnetic beads combined with magnetic beads of nucleic acid separation and purification system were used to detect and analyze leptin CLB in meat samples (pork, pork liver). The results showed that: 1) the morphology of the magnetic beads was spherical, and the particle size was uniform, monodispersity was good, the average particle size was 509 nm; 2) the modified magnetic beads remained unchanged. Strong magnetism, under the action of external magnetic field, magnetic separation can be completed quickly within 1-2 seconds; 3) the whole detection process takes 25 minutes, the linear detection range is 0.14-45.5 ppb; 4) the detection system is applied to the actual meat samples (pork, pork liver) recovery test, the recovery of clenbuterol hydrochloride in pork and pork liver is 98.1% - 106.1%, respectively. 94.2%-109.0%.
(4) Using carbon nanotubes and ionic liquids as functional materials, a novel screen printed (SP) electrode was prepared and applied to the rapid detection of Pb2+ and Cd2+ residues in meat products. The linear response range of Cd2+ was 1.0-100.0 ppb at 0.0 ppb. 2) The results of interference experiments showed that the current response of Pb2+ and Cd2+ ions was less than 5% when the concentration of common ions in the solution was 200 times that of Pb2+ and Cd2 +. The new SP electrode also had good consistency and stability. 3) The new SP electrode was used for lunch meat and ham sausage. The recoveries of Pb2+ and Cd2+ in lunch meat were 97.1% - 102.9%, 98.8% - 103.0%, and those in ham sausage were 98.5% - 106.5%, 96.0% - 103.5%.
【学位授予单位】：浙江大学
【学位级别】：博士
【学位授予年份】：2014
【分类号】：TS207.3
本文编号：2178179
[Abstract]:Because of the frequent exposure of food safety incidents, people pay more and more attention to food safety and quality. Although traditional laboratory testing methods have the advantages of high sensitivity, accurate and reliable detection results, they also have the advantages of long detection cycle, complex sample pretreatment process, low detection flux, instrument and equipment maintenance. The electrochemical analysis technology has the characteristics of low cost, convenience, easy operation, easy automation and miniaturization of the instrument, high sensitivity and good selectivity. The enzyme-linked immunoassay technology has good specificity, simple and convenient, easy to realize. Automation and other advantages.
In this paper, nanotechnology, electrochemical analysis technology, enzyme-linked immunoassay technology, magnetic separation technology and many other fields of knowledge were used to develop a rapid detection method for food safety and quality of different detection objects. Ase (CP) electrode was applied to the rapid detection of epigallocatechin gallate (EGCG) in tea, and Au nanoparticles (Au N) were doped into the carbon paste by bulk modification on the basis of ionic liquid carbon paste (ILCP) electrode. Carbon paste ionic liquid (Au NP-ILCP) electrode modified with gold nanoparticles was prepared, which was used for rapid detection of nitrite residues in meat products. Silk screen printing electrode modified with carbon nanotubes and ionic liquids was successfully prepared by silk screen printing technology, and its performance in rapid detection of heavy metal ions was studied. In this paper, the preparation and modification of electrodes for electrochemical analysis of clenbuterol (CLB) in meat products were studied. The method provides data support and provides a new idea for the application of enzyme-linked immunoassay (ELISA), which can be used for reference in the research and development of food safety and quality rapid detection instrument with independent intellectual property rights.
The main contents, results and conclusions are as follows:
(1) The CP electrode based on ionic liquids was prepared by bulk modification and used for the rapid detection of EGCG in tea. Under the optimal conditions, the detection performance of ILCP electrode for EGCG was as follows: 1) The detection range of EGCG was 5 - 7 mol / L; 2) ILCP electrode can continuously detect the concentration of EGCG changes, has a significant anti-passivation effect; 3) ILCP electrode for common EGCG analogues has anti-interference characteristics; 4) ILCP electrode detection of EGCG has consistency, reproducibility and stability; 5) ILCP electrode can be successfully used in the actual sample of tea soup EGCG detection.
(2) AuNP-ILCP electrode was successfully prepared by introducing nano-AuNP into ILCP electrode by bulk modification method, and nitrite residue in real samples was rapidly detected by AuNP-ILCP electrode. The detection performance of AuNP-ILCP electrode for nitrite under the optimal conditions was as follows: 1) The detection range was 1. 0 6550 Very consistent, reproducible and stable, and anti passivation capability.
(3) Immunomagnetic beads combined with magnetic beads of nucleic acid separation and purification system were used to detect and analyze leptin CLB in meat samples (pork, pork liver). The results showed that: 1) the morphology of the magnetic beads was spherical, and the particle size was uniform, monodispersity was good, the average particle size was 509 nm; 2) the modified magnetic beads remained unchanged. Strong magnetism, under the action of external magnetic field, magnetic separation can be completed quickly within 1-2 seconds; 3) the whole detection process takes 25 minutes, the linear detection range is 0.14-45.5 ppb; 4) the detection system is applied to the actual meat samples (pork, pork liver) recovery test, the recovery of clenbuterol hydrochloride in pork and pork liver is 98.1% - 106.1%, respectively. 94.2%-109.0%.
(4) Using carbon nanotubes and ionic liquids as functional materials, a novel screen printed (SP) electrode was prepared and applied to the rapid detection of Pb2+ and Cd2+ residues in meat products. The linear response range of Cd2+ was 1.0-100.0 ppb at 0.0 ppb. 2) The results of interference experiments showed that the current response of Pb2+ and Cd2+ ions was less than 5% when the concentration of common ions in the solution was 200 times that of Pb2+ and Cd2 +. The new SP electrode also had good consistency and stability. 3) The new SP electrode was used for lunch meat and ham sausage. The recoveries of Pb2+ and Cd2+ in lunch meat were 97.1% - 102.9%, 98.8% - 103.0%, and those in ham sausage were 98.5% - 106.5%, 96.0% - 103.5%.
【学位授予单位】：浙江大学
【学位级别】：博士
【学位授予年份】：2014
【分类号】：TS207.3
【参考文献】
相关期刊论文 前1条
1 程启坤,阮宇成,王月根,刘维华,朱珩;绿茶滋味化学鉴定法[J];茶叶科学;1985年01期
，本文编号：2178179
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