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双响应MWCNTs分离介质结构调控及对污染物快速程序释放机理研究
结题报告
批准号:
21677115
项目类别:
面上项目
资助金额:
65.0 万元
负责人:
赵景婵
依托单位:
学科分类:
B0602.环境分析化学
结题年份:
2020
批准年份:
2016
项目状态:
已结题
项目参与者:
王怡、徐飞、卜春苗、王改玲、武玲敏、潘欣悦、辛拉弟
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中文摘要
样品前处理吸附介质的记忆效应、解离速度慢是导致大气有机污染物在线监测时间分辨率差、误差大的重要原因。本项目提出利用PNIPAM、PMMA-PEG的温敏性及双亲性,结合β-CD超分子的可逆转换特性,通过ATRP、Click手段,功能化MWCNTs,构筑具有双开-关性能的程序控制分离介质。重点探讨MWCNTs表面功能膜CD-PNIPAM/Ad-PMMA-PEG的双重敏感性。揭示各组成结构单元对MWCNTs-CD-PNIPAM/Ad-PMMA-PEG微观结构与LCST的影响规律;阐明功能化MWCNTs的分配-包结双作用模式在不同极性溶剂中的程序释放机制。通过调整CD取代基位点及聚合物分子量,实现CD-PNIPAM与PMMA-PEG的协同作用,提高MWCNTs-CD-PNIPAM/Ad-PMMA-PEG的响应速度。为功能化MWCNTs在大气有机污染物在线分析中的应用提供理论基础和技术支撑。
英文摘要
In recent years, many environments organic matter significantly contributes to the compound of atmosphere and aerosol particles, and the problem of atmospheric environment pollution is becoming more serious. Detailed chemical characterization is crucial to help us to understand the formation process, source identification and properties of organic compounds in the atmosphere. The composition of organic compounds in the atmosphere is very complex, and the content is very low, therefore, air pollutants sample requires to be pretreated by various methods to reduce matrix interference and increase the concentration of the target substance. However, current off-line analytical methods are time-consuming and also subjected to artifacts during compounds collection and storage. Above all, it is an urgent affair to establish a rapid, sensitive and accurate on-line atmospheric environmental monitoring methods, and it is critical to construct a kind of multi-functional adsorption material.. In the present project, we propose a MWCNTs functional adsorption materials, which combines the thermo-responsive properties of PNIPAM and amphiphilicity of PMMA-PEG with the reversible properties of β-CD supramolecular self-assembly system. The MWCNTs surface is functionalized by a type of non-covalently connected block polymer, in which the polymer chains of β-CD-PNIPAM and Ad-PMMA-PEG are prepared via click chemistry and ATRP method, and they are connected by inclusion interaction between β-CD and ADA. The LCST and microstructures of MWCNTs-β-CD-PNIPAM/Ad-PMMA-PEG can be tuned by controlling the substituents sites of β-CD and the composition of PNIPAM and PMMA-PEG. We expect the β-CD-PNIPAM/Ad-PMMA-PEG complexes will respond to the external stimulation of apolar solvent or temperature via different mechanisms: (1) at temperatures below the LCST, the hydrophobic PNIPAM becomes hydrophilic. (2) The block polymer chain of PMMA-PEG exhibits reversible conformation transition and the complexes of β-CD-PNIPAM/Ad-PMMA-PEG exhibits reversible assembly behavior in different polar solvent. The constructed MWCNTs functional adsorption materials should achieve the acceleration effect of dual-responsive of β-CD-PNIPAM and PMMA-PEG.. Fabrication of multi-sensitive systems with fine-tunable release properties is considered to be a very important future direction. This study will provides the theoretical basis and technical support for the application of MWCNTs-β-CD-PNIPAM/PMMA-PEG on organic pollutants on-line analysis system.
与分析仪器的飞速发展相比,样品前处理技术发展相对滞后,其决定着分析过程的速度及准确性,也是制约在线分析仪器应用的瓶颈。复杂样品前处理介质的界面分子设计是其分离富集性能的关键。本项目设计了具有超分子性能及环境敏感性的聚合物,用ATRP及点击化学方法合成了几种环境响应性嵌段聚合物。.(1)探讨了环境敏感聚合物的溶剂效应、霍夫斯曼效应,环境敏感聚合物与目标物之间的相互作用机理,考察了聚合物分子量、组成对LCST、MWCNTs微观结构的影响规律。(2)在此理论研究基础上,基于温敏聚合物相转变性质,首次提出一种绿色的液-液微萃取方法,该方法无需加入分散剂、无需离心、冷冻,萃取过程快速、简单。并成功用于环境、食品中有机污染物(增塑剂、稠环芳烃、酚类)的测定;建立了温敏聚合物协调多臂碳纳米管固相微萃取-HPLC测定食品包装材料中的抗生素。(3)设计出一种适用于在线固相微萃取的螺母型不锈钢微柱,可消除预处理柱对分析柱性能的影响。以此搭建了在线固相微萃取-HPLC系统。建立了环境水样、食品中有机污染物的分析方法。通过“Grafting from”法将β-CD和NIPAM接枝到SiO2表面,合成了一系列表面具有温敏性的填料(SiO2@P-β-CD/NIPAM),在固相萃取柱部分控制温度,增强洗脱能力,提高方法的精密度。以SiO2@ P-β-CD/ NIPAM为吸附介质,建立了在线固相微萃取-HPLC监测酚类污染物的新方法;(4)利用本项目合成的吸附介质,对大气中羰基化合物及有机酸的含量及分布进行研究,结果表明该方法可以准确地测定大气中污染物的浓度水平。含氧有机物的含量水平与雾霾、温度成正相关,与相对湿度呈现负相关。阐明了以环境敏感材料为核心的样品前处理材料具有分子设计的多样性,在环境分析、食品分析及现场检测等领域具有很高的应用价值。
期刊论文列表
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DOI:10.1016/j.chroma.2019.01.052
发表时间:2019
期刊:Journal of Chromatography A
影响因子:4.1
作者:Chen Xiaomei;Guo Zhian;Wang Yi;Liu Yufeng;Xu Yidong;Liu Jie;Li Zhiqiang;Zhao Jingchan
通讯作者:Zhao Jingchan
DOI:10.1002/jssc.201900410
发表时间:2019
期刊:Journal of Separation Science
影响因子:3.1
作者:Chen Xiaomei;Xin Ladi;Xu Yidong;Liu Jie;Li Zhiqiang;Wang Yi;Zhao Jingchan
通讯作者:Zhao Jingchan
Quantitative Monitoring of Rutin in Human Urine by Flow Injection-Chemiluminescence Analysis
流动注射-化学发光分析法定量监测人尿液中的芦丁
DOI:10.1002/jccs.201600884
发表时间:2017
期刊:Journal of the Chinese Chemical Society
影响因子:1.8
作者:Xin Ladi;Li Yajuan;Wu Lingmin;Zhao Jingchan;Song Zhenghua
通讯作者:Song Zhenghua
DOI:10.1016/j.foodchem.2020.128960
发表时间:2020-12
期刊:Food chemistry
影响因子:8.8
作者:Yidong Xu;Liulin Wei;Xiaomei Chen;Jingchan Zhao;Yi Wang
通讯作者:Yidong Xu;Liulin Wei;Xiaomei Chen;Jingchan Zhao;Yi Wang
Effects and mechanisms of calcium peroxide on purification of severely eutrophic water
过氧化钙净化严重富营养化水体的效果及机制
DOI:10.1016/j.scitotenv.2018.10.040
发表时间:2019
期刊:Science of the Total Environment
影响因子:9.8
作者:Wang Yi;Wang Wen Huai;Yan Fei Long;Ding Zhuo;Feng Lin Lin;Zhao Jing Chan
通讯作者:Zhao Jing Chan
国内基金
海外基金