Shi Peiyu, Xia Bing, Qin Yongping, Zhou Yan
Chengdu Institute of Biology, Chinese Academy of Sciences, Chengdu, 610041, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Mikrochim Acta. 2023 May 15;190(6):222. doi: 10.1007/s00604-023-05770-7.
A hydroxyl-functionalized covalent organic framework aerogel COF-aerogel was designed and prepared as an adsorbent for the removal of multiple lipids from human plasma. The applications of 1,3,5-tris(4'-hydroxy-5'-formylphenyl)benzene (THB) and 1,3,5-tris(4-aminophenyl)benzene (TAPB) as monomers, DMSO/mesitylene (v/v, 4/1) as reaction solvent, and n-propylamine as reaction regulator endow COF-aerogel with good adsorption performance for multiple lipids. The morphology, phase purity, specific surface area, pore size, surface charge, and stability of COF-aerogel were characterized. Adsorption thermodynamics and adsorption kinetics studies showed that COF-aerogel had high equilibrium adsorption capacities (> 15913 mg g) and fast adsorption equilibrium (≤ 10 s) for the four model lipids tested. COF-aerogel had good reusability with the removal of the model lipids being still more than 91% after 10 use cycles. The sample pretreatment conditions and adsorbent amounts used in lipids removal experiments were optimized. Under the optimized conditions, the method of ultra-high performance liquid chromatography-high-resolution mass spectrometry (UHPLC-HRMS) using COF-aerogel as solid-phase extraction sorbent was validated with negligible matrix effects (0.4-3.0%) and good accuracy (86.7-110%) and was applied to determine 20 amino acids in human plasma samples from healthy individuals and gastric adenocarcinoma (GA) patients. The established method has been proved to have good application potential for the removal of multiple lipids in human plasma to reduce the matrix effects and improve the accuracy of clinical LC-MS analysis.
设计并制备了一种羟基官能化的共价有机框架气凝胶COF-气凝胶，作为从人血浆中去除多种脂质的吸附剂。以1,3,5-三（4'-羟基-5'-甲酰基苯基）苯（THB）和1,3,5-三（4-氨基苯基）苯（TAPB）作为单体，二甲基亚砜/均三甲苯（体积比，4/1）作为反应溶剂，正丙胺作为反应调节剂，赋予了COF-气凝胶对多种脂质良好的吸附性能。对COF-气凝胶的形貌、相纯度、比表面积、孔径、表面电荷和稳定性进行了表征。吸附热力学和吸附动力学研究表明，COF-气凝胶对所测试的四种模型脂质具有高平衡吸附容量（>15913 mg g）和快速吸附平衡（≤10 s）。COF-气凝胶具有良好的可重复使用性，在10次使用循环后，对模型脂质的去除率仍超过91%。优化了脂质去除实验中使用的样品预处理条件和吸附剂用量。在优化条件下，以COF-气凝胶作为固相萃取吸附剂的超高效液相色谱-高分辨质谱（UHPLC-HRMS）方法得到验证，基质效应可忽略不计（0.4-3.0%），准确度良好（86.7-110%），并应用于测定健康个体和胃腺癌（GA）患者人血浆样品中的20种氨基酸。已证明所建立的方法在去除人血浆中多种脂质以减少基质效应和提高临床LC-MS分析准确度方面具有良好的应用潜力。
