基于稳定同位素质谱探针标记的食品污染物检测新技术及膳食暴露评估研究

HPLC-MS/MS technology is the most effective tool for food safety monitoring. However, the low efficiency of ionization and matrix effects have become the serious factors, affecting accurate analysis of this technology. The use of stable isotope internal standard can overcome the influence of matrix effects, but the available isotope internal standards are very limited, the preparation of isotope internal standards for all analytes is very expensive and unrealistic. And, this problem can be solved by employing stable isotope probe to label the analytes. In this project, we tend to develop the multifunctional isotope-coded mass spectrum probes with the merits of economy, practicability, high sensitivity, facile chromatographic separation and isotope-coded, which can be employed to label food contaminants with the functional groups of amines, phenols and carboxylic acids. After labeling by new probes, the complex contaminants in food can be simplified, and matrix effect could be overcome, and ionization efficiency can also be improved. Ultimately, the rapid, accurate and sensitive detection technologies are established for the determination of multi-category contaminants by HPLC-MS/MS. The new methods are also used for food sample analysis and dietary exposure assessment. This study will provide new ideas for the development of novel methods for food security analysis, offer the theoretical basis and technical support for food safety supervision, and also provide the basic data for the analysis of the status of dietary pollutants and dietary exposure. Thus, the presented project has important theoretical and practical significance.

HPLC-MS/MS技术是目前最有效的食品安全检测手段。然而，离子化效率低和基质效应已成为影响该技术准确分析的重要因素。利用稳定同位素内标物可克服基质效应影响，但现有同位素内标物非常有限，制备所有分析物的同位素内标造价高且不现实。借助稳定同位素探针标记能够解决诸多污染物难以找到同位素内标的难题。本项目从功能集成思路出发，开发经济实用、兼备质谱增敏、色谱改性和同位素编码的多功能质谱探针，可实现对食品中胺类、酚类和羧酸类污染物标记。通过标记，既能实现对食品污染物分类简化，又能克服基质效应，提高目标化合物离子化效率，最终构建快速、准确、高灵敏的多类别痕量食品污染物HPLC-MS/MS检测技术，并将新检测技术用于膳食样品检测及膳食暴露评估。本研究将为食品安全检测提供新思路、新方法，为食品安全监管提供理论依据与技术支持，为分析研究我国膳食污染及膳食暴露现状提供基础数据，具有重要的理论意义和现实意义。

食品安全已经成为全社会关注的焦点，食品污染物的快速精准检测技术对于保障我国食品安全意义重大。本项目围绕复杂食品基质中痕量污染物成分样品前处理及精准检测技术开展研究，开发了经济实用、兼备质谱增敏、色谱改性和同位素标记的多功能质谱探针，对食品中多类别污染物进行标记，从而克服基质效应，简化污染物分类，提高目标化合物离子化效率，构建了快速、准确的痕量污染物检测技术。样品前处理技术决定了分析方法的准确度及分析通量，本项目针对食品中痕量污染物的化学结构特征，合成系列磁性功能化的共价有机框架材料，开发了选择性好、富集效率高的食品样品前处理技术，实现复杂基质样品的净化和富集目标物，很好的克服了基质效应干扰。最终，借助探针标记结合磁性固相萃取技术，构建了食品中的甾醇、硫化氢、N-亚硝胺、氟喹诺酮、磺胺类、多环芳烃、内分泌干扰物、植物生长调节剂等系列新兴及热点污染物快速精准检测技术，可以很好的克服复杂样品的基质效应干扰，提升了检测的准确度及灵敏度，同时极大缩短样品检测时间，提升了分析通量，最后将构建的方法用于多类别食品及环境样品的分析。相关研究为食品安全检测提供新思路、新方法，为食品安全监管提供理论依据与技术支持，为食品污染物检测和分析研究我国膳食污染及膳食暴露现状提供基础数据。