Facile Synthesis of Boronate-Decorated Polyethyleneimine-Grafted Hybrid Magnetic Nanoparticles for the Highly Selective Enrichment of Modified Nucleosides and Ribosylated Metabolites
Facile Synthesis of Boronate-Decorated Polyethyleneimine-Grafted Hybrid Magnetic Nanoparticles for the Highly Selective Enrichment of Modified Nucleosides and Ribosylated Metabolites
复制标题
轻松合成硼酸酯修饰的聚乙烯亚胺接枝的杂化磁性纳米粒子，用于高度选择性富集修饰核苷和核糖基化代谢物
DOI：
10.1021/ac402979w
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发表时间：
2013-12-03
影响因子：
7.4
通讯作者：
Xu, Guowang
中科院分区：
文献类型：
--
作者：
Li, Hua;Shan, Yuanhong;Xu, Guowang
核糖基化代谢物，特别是修饰核苷，已被广泛评估为癌症相关生物标志物。硼酸盐吸附剂被认为是从复杂基质中提取硼酸盐的有前途的材料。然而，由于现有硼酸盐吸附剂的容量和选择性有限，低丰度核糖基化代谢物的富集仍然是一个挑战。本研究通过在 Fe3O4@SiO2 表面接枝聚乙烯亚胺 (PEI) 并用硼酸酯基团修饰，合成了一种新型磁性纳米颗粒 Fe3O4@SiO2@PEI-FPBA。 PEI 链上的高密度氨基为硼酸酯基团提供了大量的结合位点。因此，纳米颗粒的吸附容量（1.34+/-0.024mg/g）大大提高，比同类材料高6至7倍。 PEI中未反应的仲胺和叔胺增强了纳米颗粒的水溶性，可以有效减少非特异性吸附。纳米颗粒能够从 1000 倍干扰中捕获 1,2 顺式二醇核苷。此外，PEI的柔性链有利于有效富集和快速平衡（
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 +/- 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 (