Title: Large-Scale Metabolite Analysis of Standards and Human Serum by Laser Desorption Ionization Mass Spectrometry from Silicon Nanopost Arrays

Abstract

The unique challenges presented by metabolomics have driven the development of new mass spectrometry (MS)-based techniques for small molecule analysis. We have previously demonstrated silicon nanopost arrays (NAPA) to be an effective substrate for laser desorption ionization (LDI) of small molecules for MS. However, the utility of NAPA-LDI-MS for a wide range of metabolite classes has not been investigated. Here we apply NAPA-LDI-MS to the large-scale acquisition of high-resolution mass spectra and tandem mass spectra from a collection of metabolite standards covering a range of compound classes including amino acids, nucleotides, carbohydrates, xenobiotics, lipids, and other classes. In untargeted analysis of metabolite standard mixtures, detection was achieved for 374 compounds and useful MS/MS spectra were obtained for 287 compounds, without individual optimization of ionization or fragmentation conditions. Metabolite detection was evaluated in the context of 31 metabolic pathways, and NAPA-LDI-MS was found to provide detection for 63% of investigated pathway metabolites. Individual, targeted analysis of the 20 common amino acids provided detection of 100% of the investigated compounds, demonstrating that improved coverage is possible through optimization and targeting of individual analytes or analyte classes. In direct analysis of aqueous and organic extracts from human serum samples, spectral features were assignedmore » to a total of 108 small metabolites and lipids. Glucose and amino acids were quantitated within their physiological concentration ranges. Finally, the broad coverage demonstrated by this large-scale screening experiment opens the door for use of NAPA-LDI-MS in numerous metabolite analysis applications« less

Authors:

Korte, Andrew R. ^[1]; Stopka, Sylwia A. ^[1]; Morris, Nicholas ^[2]; Razunguzwa, Trust ^[2]; Vertes, Akos ^[1]

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+ Show Author Affiliations

1. Department of Chemistry, George Washington University, 800 22nd Street, North West, Washington, District of Columbia 20052, United States
2. Protea Biosciences, Inc., Morgantown, West Virginia 26505, United States

Publication Date:

Fri Jul 22 00:00:00 EDT 2016

Research Org.:

George Washington Univ., Washington, DC (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1315834

Alternate Identifier(s):

OSTI ID: 1326648

Grant/Contract Number:  

FG02-01ER15129; W911NF-14-2-0020

Resource Type:

Published Article

Journal Name:

Analytical Chemistry

Additional Journal Information:

Journal Name: Analytical Chemistry Journal Volume: 88 Journal Issue: 18; Journal ID: ISSN 0003-2700

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE