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Title: Ambient Metabolic Profiling and Imaging of Biological Samples with Ultrahigh Molecular Resolution using Laser Ablation Electrospray Ionization 21 Tesla FTICR Mass Spectrometry

Abstract

Mass spectrometry (MS) has been an indispensable analytical tool in capturing the complexity and array of biomolecules within biological systems. However, conventional MS-based analytical workflows are limited in both throughput and measuring the native molecular state these systems, due in large part to sample handling and preparation. The development of ambient ionization methods capable of sampling directly from tissues circumvent many of these issues but requires the use of high-performance MS to resolve the molecular complexity within these samples. Herein, we demonstrate the unique combination of laser ablation electrospray ionization (LAESI) coupled with a 21 Tesla Fourier transform ion cyclotron resonance (21T-FTICR-MS) for MS imaging applications. This analytical platform provides isotopic fine structure information directly from native tissues, delivering a higher degree of confidence for molecular identification. The ability to capture and visualize the complex metabolic behavior of living organisms in situ is a bioanalytical grand challenge that has yet to be fully realized. Due to their excellent sensitivity and selectivity, mass spectrometry (MS)-based platforms offer a unique opportunity to characterize an array of biomolecules from a variety of biological samples.[1] One method in particular, MS imaging (MSI), has demonstrated the ability to simultaneously determine the spatial distributions for hundredsmore » of biomolecules, e. g., metabolites, lipids, peptides, and xenobiotics, within complex biological systems simultaneously.[2-3] Matrix-assisted laser desorption/ionization (MALDI)-MSI remains the most common of these methods.[4] However, the application of an exogenous matrix, and the limited availability of commercial sources that operate under atmospheric pressure,[5] has significantly prohibited the ability of MALDI to be useful for biomolecular mapping of living systems. Ambient ionization methods that require minimal to no sample preparation, like desorption electrospray ionization (DESI and nano-DESI) and laser ablation electrospray ionization (LAESI), demonstrated the ability to spatially map biomolecule distributions within live organisms.« less

Authors:
 [1];  [1];  [2];  [2];  [2];  [3];  [3];  [2];  [4];  [2];  [2];  [5]
  1. GEORGE WASHINGTON UNIV
  2. BATTELLE (PACIFIC NW LAB)
  3. UNIVERSITY PROGRAMS
  4. University of Missouri - Columbia
  5. George Washington University
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1530571
Report Number(s):
PNNL-SA-137600
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Analytical Chemistry
Additional Journal Information:
Journal Volume: 91; Journal Issue: 8
Country of Publication:
United States
Language:
English
Subject:
Mass Spectometry, fourier transform ion cyclostron resonance, ultrahigh resolution, laser ablation electrospray ionization, Mass spectrometry imaging

Citation Formats

Stopka, Sylwia A., Samarah, Laith Z., Shaw, Jared B., Liyu, Andrey V., Velickovic, Dusan, Agtuca, Beverly J., Kukolj, Caroline, Koppenaal, David W., Stacey, Gary, Pasa Tolic, Ljiljana, Anderton, Christopher R., and Vertes, Akos. Ambient Metabolic Profiling and Imaging of Biological Samples with Ultrahigh Molecular Resolution using Laser Ablation Electrospray Ionization 21 Tesla FTICR Mass Spectrometry. United States: N. p., 2019. Web. doi:10.1021/acs.analchem.8b05084.
Stopka, Sylwia A., Samarah, Laith Z., Shaw, Jared B., Liyu, Andrey V., Velickovic, Dusan, Agtuca, Beverly J., Kukolj, Caroline, Koppenaal, David W., Stacey, Gary, Pasa Tolic, Ljiljana, Anderton, Christopher R., & Vertes, Akos. Ambient Metabolic Profiling and Imaging of Biological Samples with Ultrahigh Molecular Resolution using Laser Ablation Electrospray Ionization 21 Tesla FTICR Mass Spectrometry. United States. doi:10.1021/acs.analchem.8b05084.
Stopka, Sylwia A., Samarah, Laith Z., Shaw, Jared B., Liyu, Andrey V., Velickovic, Dusan, Agtuca, Beverly J., Kukolj, Caroline, Koppenaal, David W., Stacey, Gary, Pasa Tolic, Ljiljana, Anderton, Christopher R., and Vertes, Akos. Tue . "Ambient Metabolic Profiling and Imaging of Biological Samples with Ultrahigh Molecular Resolution using Laser Ablation Electrospray Ionization 21 Tesla FTICR Mass Spectrometry". United States. doi:10.1021/acs.analchem.8b05084.
@article{osti_1530571,
title = {Ambient Metabolic Profiling and Imaging of Biological Samples with Ultrahigh Molecular Resolution using Laser Ablation Electrospray Ionization 21 Tesla FTICR Mass Spectrometry},
author = {Stopka, Sylwia A. and Samarah, Laith Z. and Shaw, Jared B. and Liyu, Andrey V. and Velickovic, Dusan and Agtuca, Beverly J. and Kukolj, Caroline and Koppenaal, David W. and Stacey, Gary and Pasa Tolic, Ljiljana and Anderton, Christopher R. and Vertes, Akos},
abstractNote = {Mass spectrometry (MS) has been an indispensable analytical tool in capturing the complexity and array of biomolecules within biological systems. However, conventional MS-based analytical workflows are limited in both throughput and measuring the native molecular state these systems, due in large part to sample handling and preparation. The development of ambient ionization methods capable of sampling directly from tissues circumvent many of these issues but requires the use of high-performance MS to resolve the molecular complexity within these samples. Herein, we demonstrate the unique combination of laser ablation electrospray ionization (LAESI) coupled with a 21 Tesla Fourier transform ion cyclotron resonance (21T-FTICR-MS) for MS imaging applications. This analytical platform provides isotopic fine structure information directly from native tissues, delivering a higher degree of confidence for molecular identification. The ability to capture and visualize the complex metabolic behavior of living organisms in situ is a bioanalytical grand challenge that has yet to be fully realized. Due to their excellent sensitivity and selectivity, mass spectrometry (MS)-based platforms offer a unique opportunity to characterize an array of biomolecules from a variety of biological samples.[1] One method in particular, MS imaging (MSI), has demonstrated the ability to simultaneously determine the spatial distributions for hundreds of biomolecules, e. g., metabolites, lipids, peptides, and xenobiotics, within complex biological systems simultaneously.[2-3] Matrix-assisted laser desorption/ionization (MALDI)-MSI remains the most common of these methods.[4] However, the application of an exogenous matrix, and the limited availability of commercial sources that operate under atmospheric pressure,[5] has significantly prohibited the ability of MALDI to be useful for biomolecular mapping of living systems. Ambient ionization methods that require minimal to no sample preparation, like desorption electrospray ionization (DESI and nano-DESI) and laser ablation electrospray ionization (LAESI), demonstrated the ability to spatially map biomolecule distributions within live organisms.},
doi = {10.1021/acs.analchem.8b05084},
journal = {Analytical Chemistry},
number = 8,
volume = 91,
place = {United States},
year = {2019},
month = {4}
}