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ACS Nano. 2018 Jul 24;12(7):6938-6948. doi: 10.1021/acsnano.8b02376. Epub 2018 Jul 6.

Fluorinated Gold Nanoparticles for Nanostructure Imaging Mass Spectrometry.

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Scripps Center for Metabolomics , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.
Department of Chemistry and Biochemistry , San Diego State University , 5500 Campanile Drive , San Diego , California 92182 , United States.
Department of Food Chemistry and Toxicology, Faculty of Chemistry and Vienna Metabolomics Center (VIME) , University of Vienna , Währingerstraße 38 , 1090 Vienna , Austria.
Department of Microbiology and Ecosystem Science, Division of Microbial Ecology, Research Network Chemistry Meets Microbiology , University of Vienna , Althanstraße 14 , 1090 Vienna , Austria.
Department of Chemistry, Molecular and Computational Biology , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.


Nanostructure imaging mass spectrometry (NIMS) with fluorinated gold nanoparticles (f-AuNPs) is a nanoparticle assisted laser desorption/ionization approach that requires low laser energy and has demonstrated high sensitivity. Here we describe NIMS with f-AuNPs for the comprehensive analysis of metabolites in biological tissues. F-AuNPs assist in desorption/ionization by laser-induced release of the fluorocarbon chains with minimal background noise. Since the energy barrier required to release the fluorocarbons from the AuNPs is minimal, the energy of the laser is maintained in the low μJ/pulse range, thus limiting metabolite in-source fragmentation. Electron microscopy analysis of tissue samples after f-AuNP NIMS shows a distinct "raising" of the surface as compared to matrix assisted laser desorption ionization ablation, indicative of a gentle desorption mechanism aiding in the generation of intact molecular ions. Moreover, the use of perfluorohexane to distribute the f-AuNPs on the tissue creates a hydrophobic environment minimizing metabolite solubilization and spatial dislocation. The transfer of the energy from the incident laser to the analytes through the release of the fluorocarbon chains similarly enhances the desorption/ionization of metabolites of different chemical nature, resulting in heterogeneous metabolome coverage. We performed the approach in a comparative study of the colon of mice exposed to three different diets. F-AuNP NIMS allows the direct detection of carbohydrates, lipids, bile acids, sulfur metabolites, amino acids, nucleotide precursors as well as other small molecules of varied biological origins. Ultimately, the diversified molecular coverage obtained provides a broad picture of a tissue's metabolic organization.


fiber free diet; gut microbiome; mass spectrometry imaging; metabolomics; mice; nanostructure imaging mass spectrometry; perfluorinated gold nanoparticles


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