title: Facile synthesis of zwitterionic polymer-coated core-shell magnetic nanoparticles for highly specific capture of N-linked glycopeptides.
abstract: Highly selective and efficient capture of glycosylated proteins and peptides from complex biological samples is of profound significance for the discovery of disease biomarkers in biological systems. Recently, hydrophilic interaction liquid chromatography (HILIC)-based functional materials have been extensively utilized for glycopeptide enrichment. However, the low amount of immobilized hydrophilic groups on the affinity material has limited its specificity, detection sensitivity and binding capacity in the capture of glycopeptides. Herein, a novel affinity material was synthesized to improve the binding capacity and detection sensitivity for glycopeptides by coating a poly(2-(methacryloyloxy)ethyl)-dimethyl-(3-sulfopropyl) ammonium hydroxide (PMSA) shell onto Fe3O4@SiO2 nanoparticles, taking advantage of reflux-precipitation polymerization for the first time (denoted as Fe3O4@SiO2@PMSA). The thick polymer shell endows the nanoparticles with excellent hydrophilic property and several functional groups on the polymer chains. The resulting Fe3O4@SiO2@PMSA demonstrated an outstanding ability for glycopeptide enrichment with high selectivity, extremely high detection sensitivity (0.1 fmol), large binding capacity (100 mg g(-1)), high enrichment recovery (above 73.6%) and rapid magnetic separation. Furthermore, in the analysis of real complicated biological samples, 905 unique N-glycosylation sites from 458 N-glycosylated proteins were reliably identified in three replicate analyses of a 65 μg protein sample extracted from mouse liver, showing the great potential of Fe3O4@SiO2@PMSA in the detection and identification of low-abundance N-linked glycopeptides in biological samples.
authors.affiliation: Shanghai Key Laboratory of Functional Materials Chemistry, East China University of Science and Technology, Shanghai 200237, China. weibingzhang@ecust.edu.cn.
authors.forename: Yajing
authors.initials: Y
authors.lastname: Chen
authors.forename: Zhichao
authors.initials: Z
authors.lastname: Xiong
authors.forename: Lingyi
authors.initials: L
authors.lastname: Zhang
authors.forename: Jiaying
authors.initials: J
authors.lastname: Zhao
authors.forename: Quanqing
authors.initials: Q
authors.lastname: Zhang
authors.forename: Li
authors.initials: L
authors.lastname: Peng
authors.forename: Weibing
authors.initials: W
authors.lastname: Zhang
authors.forename: Mingliang
authors.initials: M
authors.lastname: Ye
authors.forename: Hanfa
authors.initials: H
authors.lastname: Zou
mesh_terms: D000818:Animals; D002853:Chromatography, Liquid; D016503:Drug Delivery Systems; D015195:Drug Design; D006020:Glycopeptides / Q000737:chemistry; D006031:Glycosylation; D006801:Humans; D008099:Liver / Q000378:metabolism; D008280:Magnetics; D053768:Metal Nanoparticles / Q000737:chemistry*; D051379:Mice; D036103:Nanotechnology / Q000379:methods*; D043524:Peptide-N4-(N-acetyl-beta-glucosaminyl) Asparagine Amidase / Q000737:chemistry; D010455:Peptides / Q000737:chemistry; D011108:Polymers / Q000737:chemistry*; D040901:Proteomics; D011759:Pyrrolidines / Q000737:chemistry; D012822:Silicon Dioxide / Q000737:chemistry; D019032:Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization; D017550:Spectroscopy, Fourier Transform Infrared; D014357:Trypsin / Q000737:chemistry
chemical_list: D006020:Glycopeptides; D010455:Peptides; D011108:Polymers; D011759:Pyrrolidines; D012822:Silicon Dioxide; C043250:pyrrolidin-3-yl-methanesulfonic acid; D014357:Trypsin; D043524:Peptide-N4-(N-acetyl-beta-glucosaminyl) Asparagine Amidase