基于三维碳纳米网络的环境样品萃取新方法与器件研究

Sample preparation is still the bottleneck of environmental analytical chemistry. In our preliminary study, we have found that carbon nanomaterials keep tremendous application potentials as adsorbent in sample preparation. However, some disadvantage, such as aggregation and adsorbent loss, still need to be overcome. Therefore, in this application, we focus on the development of new environmental sample preparation methods based on novel three-dimensional carbon nanostructured network, which is constructed by using conventional carbon nanomaterials such as graphene and carbon nanotubes as building blocks. The obtained material is free-standing porous monolith of carbon nanomaterials, and thus can effectively avoid the problems associating with the existing methods. The new materials will be used to fabricate solid-phase microextraction coatings, solid-phase extraction adsorbents, magnetic extraction probes and extraction membranes for enrichment and analysis of some typical pollutants from diverse environmental matrices, such as environmental endocrine disruptors (EEDs), perfluorinated chemicals (PFCs), pharmaceuticals and personal care products (PPCPs), and heavy metal ions. The in situ and in vivo sampling techniques will also be developed. The 3D carbon nanostructured network is expected to provide higher extraction efficiency, higher selectivity, better stability, and better tolerance to matrix interference than conventional materials. After completion of the project, new environmental sample preparation methods will be obtained, and new progress in analytical devices and water purification materials will also be achieved.

环境样品前处理目前仍然是环境分析化学的瓶颈问题。在前期研究中，我们发现碳纳米材料作为一种新型的吸附材料在样品前处理中具有重要的应用价值，但是也还存在着一些明显的不足，如填料流失、团聚、堵塞等问题。为了克服这些问题，同时弥补现有样品前处理技术的缺陷与不足，在本项目中，拟开发基于新型三维碳纳米网络的环境样品萃取新方法，以常规碳纳米材料（如石墨烯、碳纳米管）作为单体构建具有独立三维纳米网络结构的宏观碳材料，将其作为固相微萃取纤维涂层、固相萃取吸附填料、磁性萃取探针及纳米萃取膜，研制新型萃取器件，提高萃取效率、选择性、稳定性和抗基质干扰能力，用于富集和分析多种环境介质中的环境内分泌干扰物、全氟化合物、医药和个人护理品（PPCPs）、重金属离子等几类典型的环境污染物，并应用于生物样品的原位与活体采样。项目完成后将获得新的环境样品前处理方法，同时有望在分析器件及污染物净化材料等方面取得进展。

本项目按照计划书内容，开展了基于三维碳纳米网络的环境样品萃取新方法与器件研究。开发了一系列针对实际环境介质中痕量新型污染物的功能化石墨烯萃取材料及功能化3D碳纳米材料质谱探针，可适用于多种环境与生物样品分析，且分析性能显著优于传统方法。在此基础上，获得了一系列新型的污染物前处理及分析器件，形成了较为系统的环境健康分析方法学。此外，在污染物鉴定表征及来源解析方面还开展了一系列探索性研究，为后续的深入研究打下了良好的基础。已在Nat. Nanotechnol.、Angew. Chem. Int. Ed.、Anal. Chem.、Environ. Sci. Technol.、Chem. Commun.等期刊发表SCI论文17篇（其中IF>5的11篇，最高IF 38.99），中文核心期刊论文1篇，申请国家发明专利4项，已授权1项，在国内外学术会议上做大会或特邀报告12次。以本项目研究为主体的成果获中国分析测试协会科学技术奖（CAIA奖）特等奖1项（本项目负责人排名第一），项目负责人入选国家“万人计划”青年拔尖人才。已培养（含联合培养）硕士研究生4人，参与项目的研究生获中科院优秀博士学位论文1项、中科院院长优秀奖1项、国家奖学金2人次、宝钢优秀学生奖特等奖1项。总之，本项目研究取得了一系列重要的研究成果，达到了预期目标。