Facile Synthesis of Boronate-Decorated Polyethyleneimine-Grafted Hybrid Magnetic Nanoparticles for the Highly Selective Enrichment of Modified Nucleosides and Ribosylated Metabolites

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• 作者：Hua Li ; Yuanhong Shan ; Lizhen Qiao ; Abo Dou ; Xianzhe Shi ; Guowang Xu
• 刊名：Analytical Chemistry
• 出版年：2013
• 出版时间：December 3, 2013
• 年：2013
• 卷：85
• 期：23
• 页码：11585-11592
• 全文大小：438K
• 年卷期：v.85,no.23(December 3, 2013)
• ISSN：1520-6882

文摘

Ribosylated metabolites, especially modified nucleosides, have been extensively evaluated as cancer-related biomarkers. Boronate adsorbents are considered to be promising materials for extracting them from complex matrices. However, the enrichment of ribosylated metabolites in low abundance is still a challenge due to the limited capacity and selectivity of the existing boronate adsorbents. In this study, a novel type of magnetic nanoparticles named Fe₃O₄@SiO₂@PEI-FPBA was synthesized by grafting polyethyleneimine (PEI) onto the surface of Fe₃O₄@SiO₂ before modification by boronate groups. The high density of the amino groups on the PEI chains supplied a large number of binding sites for boronate groups. Thus, the adsorption capacity (1.34 卤 0.024 mg/g) of the nanoparticles, which is 6- to 7-fold higher than that of analogous materials, was greatly improved. The unreacted secondary amines and tertiary amines of the PEI enhanced the aqueous solubility of the nanoparticles, which could efficiently reduce nonspecific adsorption. The nanoparticles were able to capture 1,2 cis-diol nucleosides from 1000-fold interferences. Moreover, the flexible chains of PEI were favorable for effective enrichment and quick equilibration (<2 min). Finally, 60 ribose conjugates were enriched from human urine using the nanoparticles. Among them, 43 were identified to be nucleosides and other ribosylated metabolites. Nine low abundance modified nucleosides were detected for the first time. In conclusion, Fe₃O₄@SiO₂@PEI-FPBA is an attractive candidate material for the highly selective enrichment of 1,2-cis-diol compounds.