金纳米颗粒修饰的共价有机框架材料用于基质辅助激光解析/电离质谱分析小分子

引用本文: 梁倩, 李书茗, 管西良, 党福全, 张志琪, 张静. 金纳米颗粒修饰的共价有机框架材料用于基质辅助激光解析/电离质谱分析小分子[J]. 分析化学, 2021, 49(10): 1713-1721. doi: 10.19756/j.issn.0253-3820.211162 shu

Citation: LIANG Qian, LI Shu-Ming, GUAN Xi-Liang, DANG Fu-Quan, ZHANG Zhi-Qi, ZHANG Jing. A Covalent Organic Framework Material Decorated with Gold Nanoparticles as Novel Matrix for Matrix-assisted Laser Desorption/Ionization Mass Spectrometry Analysis of Small Organic Molecules[J]. Chinese Journal of Analytical Chemistry, 2021, 49(10): 1713-1721. doi: 10.19756/j.issn.0253-3820.211162 shu

金纳米颗粒修饰的共价有机框架材料用于基质辅助激光解析/电离质谱分析小分子

陕西师范大学化学化工学院陕西省生命分析化学重点实验室, 西安 710119

通讯作者: 张静,E-mail:zhangjing8902@snnu.edu.cn

基金项目:
国家自然科学基金项目（No.22074086）、中央高校基本科研业务费专项资金项目（No.gk202005003）和西安市科技计划项目（No.GXYD5.3）资助。

摘要: 利用金硫键相互作用将金纳米颗粒固定在带有硫醚悬臂的二维共价有机框架（TTB-COF）上，制备了一种金属有机复合材料（Au-TTB-COF），用于基质辅助激光解吸/电离质谱（MALDI-MS）分析小分子物质。与前期报道的基质相比，Au-TTB-COF将COF材料对紫外光的吸收和金纳米颗粒所具有的促进激光能量转移作用相结合，提高了分析物的电离效率，显著提高了小分子MALDI-MS分析的灵敏度。同时，Au—S键的稳定性有效降低了基质背景干扰，提高了分析的重现性和耐盐能力。实际样品的分析结果表明，对富含大分子物质组分的血清和牛奶样品以及富含电解质的果汁，以Au-TTB-COF为基质均可实现样品中小分子的MALDI-MS分析。

关键词:

English

A Covalent Organic Framework Material Decorated with Gold Nanoparticles as Novel Matrix for Matrix-assisted Laser Desorption/Ionization Mass Spectrometry Analysis of Small Organic Molecules

Key Laboratory of Bioanalytical Chemistry of Shaanxi Province, School of Chemistry & Chemical Engineering, Shaanxi Normal University, Xi'an 710119, China

Corresponding author: ZHANG Jing, zhangjing8902@snnu.edu.cn

Received Date: 04 March 2021
Revised Date: 17 July 2021
Fund Project:
Supported by the National Natural Science Foundation of China (No.22074086), the Fundamental Research Funds for the Central Universities, China (No.gk202005003) and the Science and Technology Plan of Xi'an, China (No.GXYD5.3).

Abstract: Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) has become a promising analytical technology for large molecular weight molecules compounds, however, the interference of matrix-related ion peaks from the conventional matrix restricts the application of MALDI-MS in low molecular weight (LMW) organs (<500 Da). Although multiple exploration has been conducted in this region, it is still difficult to directly detect some molecules, such as low-molecular carbohydrate, which is a challenge to direct analysis without any enrichment because of its neutral property and difficulty in ionization. Herein, the in-situ Au nanoparticles (AuNPs) covalently embedded covalent organic frameworks (COFs) with sulfide cantilever (TTB-COF) were applied as a novel kind of matrix for direct analysis of various small organic molecules by MALDI-MS. The advantages of COFs such as abundant π-π periodic structure, suitable pore distribution, and increasing strong adsorption in the near UV region enable COFs be employed for various LMW organic analytes in cimprison with conventional matrix α-cyano-4-hydroxycinnamic acid (CHCA). Secondly, the addition of AuNPs not only facilitated the energy adsorption and desorption/ionization efficiency, but also provided an enrichment detection of sulfide molecules (LODs of thiabendazole as 5.0 nmol/L). Additionally, the synergistic effect between spatial confined COFs with sulfide cantilever and in-situ homogeneously distributed AuNPs solved the aggregation problem of inorganic nanoparticles during the evaporation preparation, which guaranteed the low background signals and improved the desorption/ionization efficiency. Therefore, after optimization of the synthetic conditions, Au-TTB-COF as a new matrix had an extremely low detection limit for small saccharides molecules as 11.0 nmol/L. Furthermore, Au-TTB-COF with strong salt tolerance and good reproducibility was applied to direct analysis of LMW molecules in the complex samples, such as glucose in serum samples, lactose in milk and thiabendazole in soft drinks. These results indicated that this metal-organic composites as MALDI-MS matrix had great potential in sensitive and specific detection of LMW organic chemicals in complex samples.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

金纳米颗粒修饰的共价有机框架材料用于基质辅助激光解析/电离质谱分析小分子

通讯作者: 张静,E-mail:zhangjing8902@snnu.edu.cn

English

A Covalent Organic Framework Material Decorated with Gold Nanoparticles as Novel Matrix for Matrix-assisted Laser Desorption/Ionization Mass Spectrometry Analysis of Small Organic Molecules

Corresponding author: ZHANG Jing, zhangjing8902@snnu.edu.cn

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

金纳米颗粒修饰的共价有机框架材料用于基质辅助激光解析/电离质谱分析小分子

通讯作者: 张静,E-mail:zhangjing8902@snnu.edu.cn

English

A Covalent Organic Framework Material Decorated with Gold Nanoparticles as Novel Matrix for Matrix-assisted Laser Desorption/Ionization Mass Spectrometry Analysis of Small Organic Molecules

Corresponding author: ZHANG Jing, zhangjing8902@snnu.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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