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Selective Metabolite and Peptide Capture/Mass Detection Using Fluorous Affinity Tags
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文摘
A new and general methodology is described for the targeted enrichment and subsequent direct massspectrometric characterization of sample subsets bearing various chemical functionalities from highlycomplex mixtures of biological origin. Specifically, sample components containing a chemical moietyof interest are first selectively labeled with perfluoroalkyl groups, and the entire sample is then appliedto a perfluoroalkyl-silylated porous silicon (pSi) surface. Due to the unique hydrophobic and lipophobicnature of the perfluorinated tags, unlabeled sample components are readily removed using simplesurface washes, and the enriched sample fraction can then directly be analyzed by desorption/ionizationon silicon mass spectrometry (DIOS-MS). Importantly, this fluorous-based enrichment methodologyprovides a single platform that is equally applicable to both peptide as well as small molecule focusedapplications. The utility of this technique is demonstrated by the enrichment and mass spectrometricanalysis of both various peptide subsets from protein digests as well as amino acids from serum.

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