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高度水分散性羟基官能化共价有机框架作为基质,用于增强 MALDI-TOF MS 对水中和水果中季铵盐的鉴定和定量。

Highly water-dispersible hydroxyl functionalized covalent organic frameworks as matrix for enhanced MALDI-TOF MS identification and quantification of quaternary ammonium salts in water and fruits.

机构信息

Research Center for Analytical Science, State Key Laboratory of Medicinal Chemical Biology and Tianjin Key Laboratory of Biosensing and Molecular Recognition, College of Chemistry, Nankai University, Tianjin, 300071, China.

Research Center for Analytical Science, State Key Laboratory of Medicinal Chemical Biology and Tianjin Key Laboratory of Biosensing and Molecular Recognition, College of Chemistry, Nankai University, Tianjin, 300071, China; Central Laboratory, Nankai University, 300071, China.

出版信息

Anal Chim Acta. 2022 Sep 22;1227:340269. doi: 10.1016/j.aca.2022.340269. Epub 2022 Aug 19.

DOI:10.1016/j.aca.2022.340269
PMID:36089308
Abstract

A composite matrix of sodium alginate (SA) and COF (Tp-DHBD) was designed and prepared for the detection of quaternary ammonium salts (QAs) containing heteroatoms. SA@Tp-DHBD self-assembled by the hydrogen bonding interaction between SA and COF has abundant hydroxyl and carboxylate anion sites, which makes for the excellent enrichment of the QAs through multiple interactions. Besides, the abundant hydroxyl groups can enhance laser absorption and energy transfer to achieve sensitive detection. The introduction of hydrophilic SA greatly promotes the dispersion of COFs to obtain good detection repeatability. Under the optimized experimental conditions, SA@Tp-DHBD was added to the solution of analytes and vortexed evenly, then directly analyzed by MALDI-TOF-MS. The detection limit of choline chloride, chlormequat chloride, and mepiquat chloride is 0.001 mg L; the detection limit of acetylcholine is 0.005 mg L. The relative standard deviations of target-target and sample-sample are below 6.0% and 7.0%, respectively. Moreover, the satisfactory recoveries in complex lake water and fruits meet the needs of practical applications. Comparative experiments were performed with the reported representative matrices, including ZIF-8 (MOF), TpBD (COF), UiO@TapbTp (MOF@COF), and α-cyano-4-hydroxycinnamic acid (organic matrix, CHCA). SA@Tp-DHBD exhibits the best matrix performance for QAs.

摘要

设计并制备了一种藻酸钠(SA)和 COF(Tp-DHBD)的复合基质,用于检测含杂原子的季铵盐(QAs)。SA@Tp-DHBD 通过 SA 和 COF 之间的氢键相互作用自组装,具有丰富的羟基和羧酸盐阴离子位点,通过多种相互作用实现了对 QAs 的优异富集。此外,丰富的羟基基团可以增强激光吸收和能量转移,实现灵敏检测。亲水 SA 的引入极大地促进了 COFs 的分散,从而获得了良好的检测重现性。在优化的实验条件下,将 SA@Tp-DHBD 加入到分析物溶液中,涡旋均匀,然后直接通过 MALDI-TOF-MS 进行分析。氯化胆碱、矮壮素和甲哌𬭩的检测限为 0.001 mg/L;乙酰胆碱的检测限为 0.005 mg/L。目标-目标和样品-样品的相对标准偏差分别低于 6.0%和 7.0%。此外,在复杂湖水和水果中的令人满意的回收率满足实际应用的需要。与报道的代表性基质(包括 ZIF-8(MOF)、TpBD(COF)、UiO@TapbTp(MOF@COF)和α-氰基-4-羟基肉桂酸(有机基质,CHCA))进行了比较实验。SA@Tp-DHBD 对 QAs 表现出最佳的基质性能。

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