Abstract

Developing an effective strategy for endogenous phosphopeptides enrichment and separation is necessary in phosphopeptidomics analysis due to the serious inference caused by chaotic biological environment. In this work, a size-exclusive magnetic binary metal mesoporous nanocomposites were synthesized to capture phosphorylated peptides for mass spectrometry analysis. The novel Fe3O4@TiO2–ZrO2@mSiO2 nanocomposites possessed the merits of ordered mesoporous channels, superparamagnetism and the integration of dual affinity of Zr–O and Ti–O. Compared with single-metal centered nanocomposites (Fe3O4@TiO2@mSiO2 and Fe3O4@ZrO2@mSiO2), Fe3O4@TiO2–ZrO2@mSiO2 showing much enhanced enrichment performance towards mono- and multi-phospho-peptides with better sensitivity. With all the advances, the Fe3O4@TiO2–ZrO2@mSiO2 was also successfully applied to capture endogenous phosphorylated peptides from human saliva. And consequently, a total of 30 phosphopeptides containing 2 multi- and 28 mono-phosphopeptides were identified efficiently. These results show that the novel materials have the great potential in peptidome analysis.

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