Super-hydrophilic sulfonate-modified covalent organic framework nanosheets for efficient separation and enrichment of glycopeptides.
Super-hydrophilic sulfonate-modified covalent organic framework nanosheets for efficient separation and enrichment of glycopeptides.
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DOI：
10.1016/j.chroma.2023.464020
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发表时间：
2023-04
期刊：
影响因子：
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通讯作者：
Yinjie Ji;Heming Li;Jinghan Dong;Jiashi Lin;Zian Lin
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文献类型：
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作者：
Yinjie Ji;Heming Li;Jinghan Dong;Jiashi Lin;Zian Lin
在质谱检测之前高效提取糖肽对于糖蛋白质组研究，特别是在疾病生物标志物研究中极其重要。这里报道的是首次通过应用二维（2D）共价有机骨架（COF）纳米片来高效富集糖肽。特别是，通过自下而上的策略掺入亲水单体，2D COF纳米片（表示为NUS-9）表现出超高的磺酸基接枝密度和超亲水性。此外，由于2D COF纳米片具有大表面积、低空间位阻、高化学稳定性和丰富的可及位点，NUS-9对糖肽富集表现出显着的效率，包括优异的检测灵敏度（0.01 fmol μL−1）、出色的富集能力和良好的富集选择性（1:1500，辣根过氧化物酶（HRP）胰蛋白酶消化到牛血清白蛋白（BSA）胰蛋白酶消化），以及回收率（92.2 ± 2.0%）。此外，NUS-9 能够明确检测人唾液中的 631 种内源性糖肽，展现出无与伦比的糖肽富集效率。对 NUS-9 富集的人类唾液中的蛋白质进行基因本体分析，证明了其进行全面糖蛋白组分析的潜力。
Highly efficient extraction of glycopeptides prior to mass spectrometry detection is extremely crucial for glycoproteomic research, especially in disease biomarker research. Reported here is the first time by applying two-dimensional (2D) covalent organic framework (COFs) nanosheets for highly efficient enrichment of glycopeptides. Particularly, by incorporating hydrophilic monomers through a bottom-up strategy, the 2D COF nanosheets (denoted as NUS-9) displayed an ultra-high graft density of sulfonic groups and super-hydrophilicity. In addition, because of the large surface area, low steric hindrance, high chemical stability, and abundant accessibility sites of 2D COF nanosheets, NUS-9 exhibited remarkable efficiency for glycopeptide enrichment, involving excellent detection sensitivity (0.01 fmol μL−1), outstanding enrichment capability, and good enrichment selectivity (1:1500, horseradish peroxidase (HRP) tryptic digest to bovine serum albumin (BSA) tryptic digest), and recovery (92.2 ± 2.0%). Moreover, the NUS-9 was able to unambiguously detect 631 endogenous glycopeptides from human saliva, demonstrating an unparalleled high efficiency in glycopeptide enrichment. Gene ontology analyses of proteins from human saliva enriched by NUS-9 demonstrated its potential for comprehensive glycoproteome analysis.