Facile fabrication of zwitterionic magnetic composites by one-step distillation-precipitation polymerization for highly specific enrichment of glycopeptides
Facile fabrication of zwitterionic magnetic composites by one-step distillation-precipitation polymerization for highly specific enrichment of glycopeptides
复制标题
通过一步蒸馏-沉淀聚合轻松制备两性离子磁性复合材料，以实现糖肽的高度特异性富集
DOI：
10.1016/j.aca.2018.12.00
复制
发表时间：
2018
影响因子：
6.2
通讯作者：
Junjie Ou
中科院分区：
文献类型：
--
作者：
Yongsheng Ji;Ruihong Lv;Shuhui Song;Junfeng Huang;Luwei Zhang;Guang Huang;Jinan Li;Junjie Ou
亲水作用色谱（HILIC）以两性离子修饰物为固相，用于糖肽的选择性富集，引起了广泛的关注。然而，糖肽的合成繁琐，特异性低，限制了其应用。本文采用一步蒸馏沉淀聚合法（DPP）制备了两性离子（2-（甲基丙烯酰氧基）乙基）-二甲基-（3-磺丙基）氢氧化铵（MSA）包覆的磁性复合材料（Fe3O4@PMSA）。设计良好的复合材料呈现出明显的ZIC-聚合物壳和上级亲水性（水接触角30.2），并且分别用标准样品和真实的样品研究了选择性富集糖肽的性能。由于Fe_3O_4@PMSA表面含有丰富的多电荷和极性基团的ZIC分子，因此对IgG消化物（鉴定出20种糖肽，S/N 20）和IgG与BSA质量比为1：230的混合物（鉴定出16种糖肽，S/N 20）表现出高选择性的糖肽富集。此外，IgG（S/N 10）的检测限低至0.67 fmol，回收率大于74%。最后，将Fe3O4@PMSA应用于人血清中N-糖肽的富集，从1 mL人血清中严格鉴定了158个糖蛋白的348个独特的N-糖基化位点和419个糖肽。实验结果表明，Fe_3O_4@PMSA在真实的生物样品的糖蛋白组学分析中具有良好的应用前景。
Hydrophilic interaction chromatography (HILIC) utilizing zwitterion-modified material as solid phase has.attracted extensive attention for selective enrichment of glycopeptides. However, a tedious synthesis and.low specificity for glycopeptides have restricted its application. Herein, a facile and effective approach.was developed to synthesize a zwitterionic (ZIC) polymer-coated magnetic composites (denoted as.Fe3O4@PMSA) with a zwitterion ((2-(methacryloyloxy)ethyl)-dimethyl-(3-sulfopropyl) ammonium hydroxide, MSA) via one-step distillation-precipitation polymerization (DPP). The well-designed composites presented clearly ZIC-polymer shell and superior hydrophilicity (water contact angle 30.2), and the.performance for selective enrichment of glycopeptides were investigated with standard and real samples, respectively. Owning to the abundant of ZIC molecules with multi-charge and polar groups on the.surface of resulting polymer coating, the Fe3O4@PMSA demonstrated high selectivity for glycopeptides.enrichment with IgG digest (twenty glycopeptides identified, S/N 20) and a mixture of IgG and BSA at.the mass ratio of 1:230 (sixteen glycopeptides identified, S/N 20). Besides, the detection limit as low as.0.67 fmol for IgG (S/N 10) and satisfied recovery yield more than 74% were achieved by the proposed.sorbents. Finally, the Fe3O4@PMSA was applied for enriching N-linked glycopeptides from human serum,and 348 unique N-glycosylation sites and 419 glycopeptides from 158 glycoproteins were strictly identified from 1 mL human serum. The results demonstrated that the proposed Fe3O4@PMSA showed a.promising potential in glycoproteomics analysis of real biological samples.