Development of a Desorption Electrospray Ionization–Multiple-Reaction-Monitoring Mass Spectrometry (DESI-MRM) Workflow for Spatially Mapping Oxylipins in Pulmonary Tissue Article Swipe
Matthew J. Smith
,
Mu Nie
,
Mikael Adner
,
Jesper Säfholm
,
Craig E. Wheelock
·
YOU?
·
· 2024
· Open Access
·
· DOI: https://doi.org/10.1021/acs.analchem.4c02350
YOU?
·
· 2024
· Open Access
·
· DOI: https://doi.org/10.1021/acs.analchem.4c02350
Oxylipins are a class of low-abundance lipids formed via oxygenation of fatty acids. These compounds include potent signaling molecules (e.g., octadecanoids, eicosanoids) that can exert essential functions in the pathophysiology of inflammatory diseases including asthma. While some oxylipin signaling cascades have been unraveled using LC-MS/MS-based methods, measurements in homogenate samples do not represent the spatial heterogeneity of lipid metabolism. Mass spectrometry imaging (MSI) directly detects analytes from a surface, which enables spatial mapping of oxylipin biosynthesis and migration within the tissue. MSI has lacked the sensitivity to routinely detect low-abundance oxylipins; however, new multiple-reaction-monitoring (MRM)-based MSI technologies show increased sensitivity. In this study, we developed a workflow to apply desorption electrospray ionization coupled to a triple quadrupole mass spectrometer (DESI-MRM) to spatially map oxylipins in pulmonary tissue. The targeted MSI workflow screened guinea pig lung extracts using LC-MS/MS to filter oxylipin targets based on their detectability by DESI-MRM. A panel of 5 oxylipins was then selected for DESI-MRM imaging derived from arachidonic acid (TXB2, 11-HETE, 12-HETE), linoleic acid (12,13-DiHOME), and α-linolenic acid (16-HOTrE). To parse this new data type, a custom-built R package (quantMSImageR) was developed with functionality to label regions of interest as well as quantify and analyze lipid distributions. The spatial distributions quantified by DESI-MRM were supported by LC-MS/MS analysis, with both indicating that 16-HOTrE and 12-HETE were associated with airways, while 12,13-DiHOME and arachidonic acid were mapped to parenchyma. This study realizes the potential of targeted MSI to routinely map low-abundance oxylipins with high specificity at scale.
Related Topics
Concepts
Chemistry
Desorption electrospray ionization
Mass spectrometry
Chromatography
Extractive electrospray ionization
Electrospray
Selected reaction monitoring
Desorption
Electrospray ionization
Sample preparation in mass spectrometry
Analytical Chemistry (journal)
Chemical ionization
Ionization
Tandem mass spectrometry
Organic chemistry
Adsorption
Ion
Metadata
- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/acs.analchem.4c02350
- OA Status
- hybrid
- Cited By
- 8
- References
- 25
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4403782638
All OpenAlex metadata
Raw OpenAlex JSON
- OpenAlex ID
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https://openalex.org/W4403782638Canonical identifier for this work in OpenAlex
- DOI
-
https://doi.org/10.1021/acs.analchem.4c02350Digital Object Identifier
- Title
-
Development of a Desorption Electrospray Ionization–Multiple-Reaction-Monitoring Mass Spectrometry (DESI-MRM) Workflow for Spatially Mapping Oxylipins in Pulmonary TissueWork title
- Type
-
articleOpenAlex work type
- Language
-
enPrimary language
- Publication year
-
2024Year of publication
- Publication date
-
2024-10-26Full publication date if available
- Authors
-
Matthew J. Smith, Mu Nie, Mikael Adner, Jesper Säfholm, Craig E. WheelockList of authors in order
- Landing page
-
https://doi.org/10.1021/acs.analchem.4c02350Publisher landing page
- Open access
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YesWhether a free full text is available
- OA status
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hybridOpen access status per OpenAlex
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https://doi.org/10.1021/acs.analchem.4c02350Direct OA link when available
- Concepts
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Chemistry, Desorption electrospray ionization, Mass spectrometry, Chromatography, Extractive electrospray ionization, Electrospray, Selected reaction monitoring, Desorption, Electrospray ionization, Sample preparation in mass spectrometry, Analytical Chemistry (journal), Chemical ionization, Ionization, Tandem mass spectrometry, Organic chemistry, Adsorption, IonTop concepts (fields/topics) attached by OpenAlex
- Cited by
-
8Total citation count in OpenAlex
- Citations by year (recent)
-
2025: 7, 2024: 1Per-year citation counts (last 5 years)
- References (count)
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25Number of works referenced by this work
- Related works (count)
-
10Other works algorithmically related by OpenAlex
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| abstract_inverted_index.workflow | 106, 130 |
| abstract_inverted_index.12-HETE), | 165 |
| abstract_inverted_index.DESI-MRM. | 147 |
| abstract_inverted_index.Oxylipins | 0 |
| abstract_inverted_index.analysis, | 211 |
| abstract_inverted_index.compounds | 14 |
| abstract_inverted_index.developed | 104, 185 |
| abstract_inverted_index.essential | 25 |
| abstract_inverted_index.functions | 26 |
| abstract_inverted_index.including | 33 |
| abstract_inverted_index.increased | 98 |
| abstract_inverted_index.migration | 77 |
| abstract_inverted_index.molecules | 18 |
| abstract_inverted_index.oxylipins | 123, 152, 244 |
| abstract_inverted_index.potential | 236 |
| abstract_inverted_index.pulmonary | 125 |
| abstract_inverted_index.represent | 52 |
| abstract_inverted_index.routinely | 87, 241 |
| abstract_inverted_index.signaling | 17, 38 |
| abstract_inverted_index.spatially | 121 |
| abstract_inverted_index.supported | 208 |
| abstract_inverted_index.unraveled | 42 |
| abstract_inverted_index.(DESI-MRM) | 119 |
| abstract_inverted_index.associated | 220 |
| abstract_inverted_index.desorption | 109 |
| abstract_inverted_index.homogenate | 48 |
| abstract_inverted_index.indicating | 214 |
| abstract_inverted_index.ionization | 111 |
| abstract_inverted_index.oxylipins; | 90 |
| abstract_inverted_index.quadrupole | 116 |
| abstract_inverted_index.quantified | 204 |
| abstract_inverted_index.(16-HOTrE). | 172 |
| abstract_inverted_index.(MRM)-based | 94 |
| abstract_inverted_index.arachidonic | 161, 226 |
| abstract_inverted_index.metabolism. | 58 |
| abstract_inverted_index.oxygenation | 9 |
| abstract_inverted_index.parenchyma. | 231 |
| abstract_inverted_index.sensitivity | 85 |
| abstract_inverted_index.specificity | 247 |
| abstract_inverted_index.12,13-DiHOME | 224 |
| abstract_inverted_index.biosynthesis | 75 |
| abstract_inverted_index.custom-built | 180 |
| abstract_inverted_index.eicosanoids) | 21 |
| abstract_inverted_index.electrospray | 110 |
| abstract_inverted_index.inflammatory | 31 |
| abstract_inverted_index.measurements | 46 |
| abstract_inverted_index.sensitivity. | 99 |
| abstract_inverted_index.spectrometer | 118 |
| abstract_inverted_index.spectrometry | 60 |
| abstract_inverted_index.technologies | 96 |
| abstract_inverted_index.α-linolenic | 170 |
| abstract_inverted_index.detectability | 145 |
| abstract_inverted_index.distributions | 203 |
| abstract_inverted_index.functionality | 187 |
| abstract_inverted_index.heterogeneity | 55 |
| abstract_inverted_index.low-abundance | 5, 89, 243 |
| abstract_inverted_index.LC-MS/MS-based | 44 |
| abstract_inverted_index.distributions. | 200 |
| abstract_inverted_index.octadecanoids, | 20 |
| abstract_inverted_index.(12,13-DiHOME), | 168 |
| abstract_inverted_index.(quantMSImageR) | 183 |
| abstract_inverted_index.pathophysiology | 29 |
| abstract_inverted_index.(TXB<sub>2</sub>, | 163 |
| abstract_inverted_index.multiple-reaction-monitoring | 93 |
| cited_by_percentile_year.max | 99 |
| cited_by_percentile_year.min | 90 |
| countries_distinct_count | 1 |
| institutions_distinct_count | 5 |
| citation_normalized_percentile.value | 0.90389092 |
| citation_normalized_percentile.is_in_top_1_percent | False |
| citation_normalized_percentile.is_in_top_10_percent | True |