Cationic metal-organic framework based mixed-matrix membrane for extraction of phenoxy carboxylic acid (PCA) herbicides from water samples followed by UHPLC-MS/MS determination
Cationic metal-organic framework based mixed-matrix membrane for extraction of phenoxy carboxylic acid (PCA) herbicides from water samples followed by UHPLC-MS/MS determination
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DOI：
10.1016/j.jhazmat.2020.122556
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发表时间：
2020-07-15
影响因子：
13.6
通讯作者：
Chen, Lingxin
中科院分区：
文献类型：
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作者：
Wu, Gege;Ma, Jiping;Chen, Lingxin
首次设计了一种基于阳离子金属有机骨架(MOF)的混合基质膜(MMM)，即阳离子MOF-MMM，并将其用于同时分散膜萃取水样中6种苯氧基羧酸(PCA)除草剂，然后用超高效液相色谱串联质谱(MS)进行测定。通过在聚偏氟乙烯(PVDF)溶液中浸泡锆基MOF，并进一步用季胺基团UIO-66-NMe3+MMM进行官能化，合成了阳离子MOF-MMM。采用红外光谱、扫描电子显微镜、X射线衍射仪、X射线光电子能谱、核磁共振等手段对制备的UIO-66-NMe3+MMM进行了表征，详细考察了MOF/PVDF用量比、溶液pH、萃取时间、共存阴离子和离子强度等因素对MMM基二甲醚催化效率的影响。阴离子PCA与阳离子UIO-66-NMe3+MMM之间的吸附机理以静电作用为主，同时伴随着pi-pi共轭和阳离子-pi键，使其具有较好的吸附性能。方法的检出限为0.03~0.59 ng/L，加标回收率为80.06~117.40%，具有较高的灵敏度和适用性。结果表明，基于阳离子MOF-MMM的二甲醚可以作为一种通用的、有价值的高通量萃取技术用于不同水样的污染物提取。
A novel kind of cationic metal-organic framework(MOF) based mixed-matrix membrane(MMM) namely cationic MOF-MMM was firstly designed and used for simultaneous dispersive membrane extraction(DME) of six phenoxy carboxylic acid(PCA) herbicides from water samples followed by determination using ultrahigh-performance liquid chromatography tandem mass spectrometry. The cationic MOF-MMM was synthesized by soaking the zirconium-based MOFs in a polyvinylidene fluoride(PVDF) solution and further functionalization with quaternary amine groups, viz., UiO-66-NMe3+ MMM. The well-prepared UiO-66-NMe3+ MMM was characterized by FT-IR, SEM, XRD, XPS, NMR and etc. Several main variables influencing the MMM based DME efficiency were investigated and optimized in detail, such as dosage ratio of MOF/PVDF, solution pH, extraction time, coexistent anions and ionic strength. Electrostatic interactions dominated adsorption mechanism between anionic PCAs and cationic UiO-66-NMe3+ MMM, along with pi-pi conjugation and cation-pi bonding, leading to better adsorption performance. Low limits of detection in the range of 0.03-0.59 ng/L and satisfactory recoveries within 80.06-117.40 % for all the PCAs are a reliable witness to demonstrate supreme sensitivity and the applicability of the developed method. By relying on the obtained results, the present work implied cationic MOF-MMM based DME can be a versatile and worthy utility for extraction of pollutants from different water samples with high throughput.