Ligand-free strategy for ultrafast and highly selective enrichment of glycopeptides using Ag-coated magnetic nanoarchitectures

Abstract

Selective enrichment of glycopeptides from complicated biological samples is essential for MS-based glycoproteomics, but still remains a great challenge. In this study, we report an unprecedented ligandfree strategy for the selective enrichment of glycopeptides by simply utilizing the multivalent interaction between glycopeptides and silver nanoparticles (Ag-NPs) coated magnetic nanoarchitectures. The composite microspheres were deliberately designed to be constructed with a high-magnetic-response magnetic colloid nanocrystal cluster (MCNC) core, a poly(methacrylic acid) (PMAA) interim layer and a Ag-NPs functional shell with high coverage. Taking advantage of the reversible interaction of glycans with Ag-NPs and the high magnetic susceptibility of the magnetite core, the MCNC@PMAA@Ag-NPs microspheres possess remarkable selectivity for glycopeptides even at a low molar ratio of glycopeptides/non-glycopeptides (1 : 100) with a very rapid enrichment speed (only 1 min needed) and a simple operation procedure using magnetic separation. Applying this approach, we identified 127 unique glycopeptides mapped to 51 different glycoproteins from only 1 mL rat serum samples. These results clearly demonstrated that the MCNC@PMAA@Ag-NPs have great potential for purifying and identifying the low-abundant glycopeptides in complex biological samples.

Nanotechnology in Glycomics: Applications in Diagnostics, Therapy, Imaging, and Separation Processes

“…Another approach using particles larger than 100 nm described by Ma et al. is worth mentioning . This ligand‐free approach is based on the application of hybrid particles having a magnetic core with 22 nm AgNPs deposited on the surface.…”

“…Selective glycan enrichment by such hybrid particles was achieved by the reversible interaction between glycans and the Ag surface, and glycopeptides could be effectively separated from a mixture having a molar ratio of glycopeptides to nonglycopeptides of 1:100 within 1 min. Finally, the method was applied for MALDI‐TOF‐MS glycan analysis from just 1 μL of rat serum …”

Analysis of carbohydrates and glycoconjugates by matrix‐assisted laser desorption/ionization mass spectrometry: An update for 2011–2012

“…Silver‐coated magnetic nanoarchitectures were used by Ma et al () to enrich glycopeptides from rat serum samples. The method makes use of the reversible reaction between silver and glycans to selectively extract the glycoproteins from mixtures.…”

Magnetic Colloidal Supraparticles: Design, Fabrication and Biomedical Applications

“…To this end, Zhang and Deng's group synthesized the C 8 ‐functinoalized MCSP microspheres. The carbon‐covered MCSPs prepared by a two‐step hydrothermal process were modified with chlorodimethyloctylsilane, resulting in MCSP@Carbon‐C 8 microspheres 112. Then peptide analysis was studied using Angiotensin II as a model.…”