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用于高效吸附和检测有机磷农药的高缺陷铜基金属有机骨架:实验和计算研究。

Highly defective copper-based metal-organic frameworks for the efficient adsorption and detection of organophosphorus pesticides: An experimental and computational investigation.

机构信息

College of Food Science and Engineering, Shandong Agricultural University, Taian 271018, PR China.

Department of Nutrition and Food Science, College of Agriculture and Natural Resources, University of Maryland, College Park, MD 20742, USA.

出版信息

Food Chem. 2023 Oct 15;423:136319. doi: 10.1016/j.foodchem.2023.136319. Epub 2023 May 11.

DOI:10.1016/j.foodchem.2023.136319
PMID:37187007
Abstract

Organophosphorus pesticide (OP) residues pose a serious threat to human health, motivating the search for novel adsorbents and detection methods. Herein, defective copper-based metal organic frameworks (Cu-MOFs) were synthesized by the reaction of Cu ions and 1,3,5-benzenetricarboxylate linkers in the presence of acetic acid. As the amount of acetic acid increased, the crystallization kinetics and morphology of the Cu-MOFs changed, leading to mesoporous Cu-MOFs with many large surface pores (defects). Adsorption studies of OPs revealed the defective Cu-MOFs showed faster pesticide adsorption kinetics and higher pesticide adsorption capacities. Density functional theory calculations showed that pesticide adsorption in the Cu-MOFs was mainly electrostatic. A dispersive solid phase extraction method was developed based on a defective Cu-MOF-6 for rapidly extracting pesticides from food samples. The method allowed pesticide detection over a wide linear concentration range, low limits of detection (0.0067-0.0164 µg L) and good recoveries in pesticide-spiked samples (81.03-109.55%).

摘要

有机磷农药(OP)残留对人类健康构成严重威胁,促使人们寻求新型吸附剂和检测方法。在此,通过 Cu 离子与 1,3,5-苯三甲酸连接体在醋酸存在下的反应合成了具有缺陷的铜基金属有机骨架(Cu-MOFs)。随着醋酸用量的增加,Cu-MOFs 的结晶动力学和形态发生变化,导致具有许多大表面孔(缺陷)的介孔 Cu-MOFs。对 OP 的吸附研究表明,具有缺陷的 Cu-MOFs 表现出更快的农药吸附动力学和更高的农药吸附容量。密度泛函理论计算表明,农药在 Cu-MOFs 中的吸附主要是静电的。基于缺陷的 Cu-MOF-6 开发了一种分散固相萃取方法,用于从食品样品中快速提取农药。该方法允许在宽线性浓度范围内检测农药,检测限低(0.0067-0.0164 µg L),在加标样品中的回收率良好(81.03-109.55%)。

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