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  • 1.
    Bergman, Hilde-Marlene
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Duncan, Kyle D.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Lanekoff, Ingela
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Single‐Cell Mass Spectrometry2018Inngår i: Encyclopedia of Analytical Chemistry: Applications, Theory and Instrumentation / [ed] Editor-in-Chief Robert A. Meyers, Wiley-VCH Verlagsgesellschaft, 2018Kapittel i bok, del av antologi (Fagfellevurdert)
    Abstract [en]

    Over the past few decades, the chemical characterization of single cells has improved immensely. In particular, mass spectrometry (MS) has pioneered direct analysis of metabolites, lipids, and peptides from single cells. This progress has been enabled by new and improved strategies for ionization and sampling, where a multitude of techniques for single‐cell MS has contributed unique insights to many different disciplines. Here, an overview of the main three techniques secondary ion mass spectrometry (SIMS), matrix‐assisted laser desorption ionization (MALDI), and ambient ionization for direct single‐cell MS analysis are presented, including some example studies detailing the use of single‐cell MS.

  • 2.
    Duncan, Kyle D.
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Andersson, Ingela
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Oversampling To Improve Spatial Resolution for Liquid Extraction Mass Spectrometry Imaging2018Inngår i: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 90, nr 4, s. 2451-2455Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Liquid extraction mass spectrometry imaging (MSI) experiments provide users with direct analysis of biological surfaces with minimal sample preparation. Until now, much of the effort to increase spatial resolution for MSI with liquid extraction techniques has focused on reducing the size of the sampling area. However, this can be experimentally challenging. Here, we present oversampling as a simple alternative to increase the spatial resolution using nanospray desorption electrospray ionization (nano-DESI) MSI. By imaging partial rat spinal cord tissue sections, two major concerns with oversampling are addressed: whether endogenous molecules are significantly depleted from repeated sampling events and whether analytes are redistributed as a result of oversampling. In depth examination of ion images for representative analytes show that depletion and redistribution do not affect analyte localization in the tissue sample. Nano-DESI MSI experiments using three times oversampling provided higher spatial resolution, allowing the observation of features not visible with undersampling. Although proper care must be taken to ensure that oversampling will work in specific applications, we envision oversampling as a simple approach to increase image quality for liquid extraction MSI techniques.

  • 3.
    Duncan, Kyle D.
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Bergman, Hilde-Marlene
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Andersson, Ingela
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    A pneumatically assisted nanospray desorption electrospray ionization source for increased solvent versatility and enhanced metabolite detection from tissue2017Inngår i: The Analyst, ISSN 0003-2654, E-ISSN 1364-5528, Vol. 142, nr 18, s. 3424-3431Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Nanospray desorption electrospray ionization (nano-DESI) has been established as a powerful technique for mass spectrometry imaging (MSI) of biomolecules from tissue samples. The direct liquid extraction of analytes from a surface at ambient pressure negates the need for significant sample preparation or matrix application. Although many recent studies have applied nano-DESI to new and exciting applications, there has not been much work in the development and improvement of the nano-DESI source. Here, we incorporate a nebulizer to replace the self-aspirating secondary capillary in the conventional nano-DESI setup, and characterize the device by use of rat kidney tissue sections. We find that the pneumatically assisted nano-DESI device offers improved sensitivity for metabolite species by 1-3 orders of magnitude through more complete desolvation and reduced ionization suppression. Further, the pneumatically assisted nano-DESI device reduces the dependence on probe-to-surface distance and enables sampling and imaging using pure water as the nano-DESI solvent. This provides exclusive detection and imaging of many highly polar endogenous species. Overall, the developed pneumatically assisted nano-DESI device provides more versatile solvent selection and an increased sensitivity for metabolites, which generates ion images of higher contrast - allowing for more intricate studies of metabolite distribution.

  • 4.
    Duncan, Kyle D.
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Fang, Ru
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC.
    Yuan, Jia
    Cincinnati Childrens Hosp Med Ctr, Div Reprod Sci, Cincinnati, OH 45229 USA.
    Chu, Rosalie K.
    Pacific Northwest Natl Lab, Biol Sci Div, Richland, WA 99352 USA.
    Dey, Sudhansu K.
    Cincinnati Childrens Hosp Med Ctr, Div Reprod Sci, Cincinnati, OH 45229 USA.
    Burnum-Johnson, Kristin E.
    Pacific Northwest Natl Lab, Biol Sci Div, Richland, WA 99352 USA.
    Lanekoff, Ingela
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Quantitative Mass Spectrometry Imaging of Prostaglandins as Silver Ion Adducts with Nanospray Desorption Electrospray Ionization2018Inngår i: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 90, nr 12, s. 7246-7252Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Prostaglandins (PG) are an important class of lipid biomolecules that are essential in many biological processes, including inflammation and successful pregnancy. Despite a high bioactivity, physiological concentrations are typically low, which makes direct mass spectrometric analysis of endogenous PG species challenging. Consequently, there have not been any studies investigating PG localization to specific morphological regions in tissue sections using mass spectrometry imaging (MSI) techniques. Herein, we show that silver ions, added to the solvent used for nanospray desorption electrospray ionization (nano-DESI) MSI, enhances the ionization of PGs and enables nano-DESI MSI of several species in uterine tissue from day 4 pregnant mice. It was found that detection of [PG + Ag](+) ions increased the sensitivity by similar to 30 times, when compared to [PG - H](-) ions. Further, the addition of isotopically labeled internal standards enabled generation of quantitative ion images for the detected PG species. Increased sensitivity and quantitative MSI enabled the first proof-of-principle results detailing PG localization in mouse uterus tissue sections. These results show that PG species primarily localized to cellular regions of the luminal epithelium and glandular epithelium in uterine tissue. Further, this study provides a unique scaffold for future studies investigating the PG distribution within biological tissue samples.

  • 5.
    Duncan, Kyle D.
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Fyrestam, Jonas
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Lanekoff, Ingela
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Advances in mass spectrometry based single-cell metabolomics2019Inngår i: The Analyst, ISSN 0003-2654, E-ISSN 1364-5528, Vol. 144, nr 3, s. 782-793Artikkel, forskningsoversikt (Fagfellevurdert)
    Abstract [en]

    Metabolomics has grown into a prominent field contributing to the molecular understanding of complex biological processes in both health and disease. Furthermore, single-cells are known to display metabolic differences between seemingly homogeneous populations of cells. Single-cell metabolomics attempts to analyze many cellular metabolites from single cells to understand phenotypic heterogeneity, which is a significant challenge due to the low analyte abundances and limited sample volumes. Label-free metabolite detection can be achieved with mass spectrometry, which is capable of simultaneously analyzing hundreds of metabolites. Herein, we review the recent advances in mass spectrometry based single-cell metabolomics, highlighting the current state-of-the-art within the last three years, and identify the challenges to move the field forward.

  • 6.
    Duncan, Kyle D.
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Lanekoff, Ingela
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
    Spatially Defined Surface Sampling Capillary Electrophoresis Mass Spectrometry2019Inngår i: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 91, nr 12, s. 7819-7827Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Capillary electrophoresis mass spectrometry (CE-MS) is an established technique for targeted and untargeted analysis of metabolites from complex biological samples. However, current CE-MS devices rely on liquid sample extracts, which restricts acquisition of spatially defined chemical information from tissue samples. The ability to chemically profile distinct cellular regions in tissue can contribute better understanding to molecular foundations in health and disease. Therefore, we describe the first CE-MS device capable of untargeted metabolite profiling directly from defined morphological regions of solid tissue sections. With surface sampling capillary electrophoresis mass spectrometry (SS-CE-MS), endogenous molecules are sampled and detected from a single defined tissue location. Characterization of SS-CE MS from different locations of the outer epidermal layer of A. Cepa demonstrated reproducible relative migration times and a peak area RSD of 20% (n = 5). Further, relative migration times were conserved for endogenous metabolites in tissues with varying complexities, including brain, spinal cord, and kidney. Results from proof-of-principle experiments from distinct morphological tissue regions reveal simultaneous analysis of small and large biomolecules, confident metabolite annotation, identification of in-source fragmentation interferences, and discrete isomeric abundances related to biological function. We envision that this new tool will provide in-depth chemical profiling and annotation of molecules in distinct cellular regions of tissue for improved biological understanding.

  • 7.
    Duncan, Kyle D.
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi. Vancouver Isl Univ, Chem, Appl Environm Res Labs, 900 Fifth St, Nanaimo, BC V9R 5S5, Canada.
    Richards, Larissa C.
    Vancouver Isl Univ, Chem, Appl Environm Res Labs, 900 Fifth St, Nanaimo, BC V9R 5S5, Canada;Univ Victoria, Dept Chem, Stn CSC, POB 1700, Victoria, BC V8W 2Y2, Canada.
    Monaghan, Joseph
    Vancouver Isl Univ, Chem, Appl Environm Res Labs, 900 Fifth St, Nanaimo, BC V9R 5S5, Canada;Univ Victoria, Dept Chem, Stn CSC, POB 1700, Victoria, BC V8W 2Y2, Canada.
    Simair, Monique C.
    Maven Water & Environm, 238-111 Res Dr, Saskatoon, SK S7N 3R2, Canada;Univ Saskatchewan, Dept Civil Geol & Environm Engn, 57 Campus Dr, Saskatoon, SK S7N 5A9, Canada;Univ Saskatchewan, Sch Environm & Sustainabil, 323 Kirk Hall,117 Sci Pl, Saskatoon, SK S7N 5C8, Canada;Clemson Univ, Dept Environm Engn & Earth Sci, 321 Calhoun Dr, Clemson, SC 29634 USA.
    Ajaero, Chukwuemeka
    Environm & Climate Change Canada, Sci & Technol Branch, Watershed Hydrol & Ecol Res Div, 11 Innovat Blvd, Saskatoon, SK S7N 3H5, Canada;Univ Regina, Environm Syst Engn, 3737 Wascana Pkwy, Regina, SK S4S 0A2, Canada.
    Peru, Kerry M.
    Environm & Climate Change Canada, Sci & Technol Branch, Watershed Hydrol & Ecol Res Div, 11 Innovat Blvd, Saskatoon, SK S7N 3H5, Canada.
    Friesen, Vanessa
    Contango Strategies Ltd, 104-411 Downey Rd, Saskatoon, SK S7N 4L8, Canada.
    McMartin, Dena W.
    Univ Saskatchewan, Dept Civil Geol & Environm Engn, 57 Campus Dr, Saskatoon, SK S7N 5A9, Canada;Univ Saskatchewan, Sch Environm & Sustainabil, 323 Kirk Hall,117 Sci Pl, Saskatoon, SK S7N 5C8, Canada.
    Headley, John V.
    Environm & Climate Change Canada, Sci & Technol Branch, Watershed Hydrol & Ecol Res Div, 11 Innovat Blvd, Saskatoon, SK S7N 3H5, Canada.
    Gill, Chris G.
    Vancouver Isl Univ, Chem, Appl Environm Res Labs, 900 Fifth St, Nanaimo, BC V9R 5S5, Canada;Univ Victoria, Dept Chem, Stn CSC, POB 1700, Victoria, BC V8W 2Y2, Canada.
    Krogh, Erik T.
    Vancouver Isl Univ, Chem, Appl Environm Res Labs, 900 Fifth St, Nanaimo, BC V9R 5S5, Canada;Univ Victoria, Dept Chem, Stn CSC, POB 1700, Victoria, BC V8W 2Y2, Canada.
    Direct analysis of naphthenic acids in constructed wetland samples by condensed phase membrane introduction mass spectrometry2020Inngår i: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 716, artikkel-id 137063Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The application of direct mass spectrometry techniques to the analysis of complex samples has a number of advantages including reduced sample handling, higher sample throughput, in situ process monitoring, and the potential for adaptation to on-site analysis. We report the application of a semi-permeable capillary hollow fibre membrane probe (immersed directly into an aqueous sample) coupled to a triple quadrupole mass spectrometer by a continuously flowing methanol acceptor phase for the rapid analysis of naphthenic adds with unit mass resolution. The intensity of the naphthenic add-associated peaks in the mass spectrum are normalized to an internal standard in the acceptor phase for quantitation and the relative abundance of the peaks in the mass spectrum are employed to monitor compositional changes in the naphthenic add mixture using principle component analysis. We demonstrate the direct analysis of a synthetic oil sands process-affected water for classical (CnH2n+zO2) as they are attenuated through constructed wetlands containing sedge (Carex aquatilis), cattail (Typha latifolia), or bulrush (Schoenoplectus acutus). Quantitative results for on-line membrane sampling compare favourably to those obtained by solid-phase extraction high-resolution mass spectrometry. Additionally. chemometric analysis of the mass spectra indicates a clear discrimination between naphthenic acid-influenced and natural background waters. Furthermore, the compositional changes within complex naphthenic acid mixtures track closely with the degree of attenuation. Overall, the technique is successful in following changes in both the concentration and composition of naphthenic acids from synthetic oil sands process-affected waters. with the potential for high throughput screening and environmental forensics. 

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