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| Formato: | Artículo científico |
| Lenguaje: | en |
| Publicado: |
Environmental science & technology
2024
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| Acceso en línea: | https://pubmed.ncbi.nlm.nih.gov/39413296/ |
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| author | Papadopoulos Lambidis, Stilianos Schramm, Tilman Steuer-Lodd, Karoline Farrell, Shane Stincone, Paolo Schmid, Robin Koester, Irina Torres, Ralph Dittmar, Thorsten Aluwihare, Lihini Simon, Carsten Petras, Daniel |
| author_facet | Papadopoulos Lambidis, Stilianos Schramm, Tilman Steuer-Lodd, Karoline Farrell, Shane Stincone, Paolo Schmid, Robin Koester, Irina Torres, Ralph Dittmar, Thorsten Aluwihare, Lihini Simon, Carsten Petras, Daniel Papadopoulos Lambidis, Stilianos Schramm, Tilman Steuer-Lodd, Karoline Farrell, Shane Stincone, Paolo Schmid, Robin Koester, Irina Torres, Ralph Dittmar, Thorsten Aluwihare, Lihini Simon, Carsten Petras, Daniel |
| collection | PubMed - marine biology |
| contents | Two-Dimensional Liquid Chromatography Tandem Mass Spectrometry Untangles the Deep Metabolome of Marine Dissolved Organic Matter. Papadopoulos Lambidis, Stilianos Schramm, Tilman Steuer-Lodd, Karoline Farrell, Shane Stincone, Paolo Schmid, Robin Koester, Irina Torres, Ralph Dittmar, Thorsten Aluwihare, Lihini Simon, Carsten Petras, Daniel Tandem Mass Spectrometry Chromatography, Liquid Metabolome Seawater Organic Chemicals Dissolved organic matter (DOM) is an ultracomplex mixture that plays a central role in global biogeochemical cycles. Despite its importance, DOM remains poorly understood at the molecular level. Over the last decades, significant efforts have been made to decipher the chemical composition of DOM by high-resolution mass spectrometry (HR-MS) and liquid chromatography (LC) coupled with tandem mass spectrometry (MS/MS). Yet, the complexity and high degree of nonresolved isomers still hamper the full structural analysis of DOM. To address this challenge, we developed an offline two-dimensional (2D) LC approach using two reversed-phase dimensions with orthogonal pH levels, followed by MS/MS data acquisition and molecular networking. 2D-LC-MS/MS reduced the complexity of DOM, enhancing the quality of MS/MS spectra and increasing spectral annotation rates. Applying our approach to analyze coastal-surface DOM from Southern California (USA) and open-ocean DOM from the central North Pacific (Hawaii), we annotated in total more than 600 structures via MS/MS spectrum matching, which was up to 90% more than that in iterative 1D LC-MS/MS analysis with the same total run time. Our data offer unprecedented insights into the molecular composition of marine DOM and highlight the potential of 2D-LC-MS/MS approaches to decipher the chemical composition of ultracomplex samples. |
| format | Artículo científico |
| id | pubmed_39413296 |
| institution | PubMed |
| language | en |
| publishDate | 2024 |
| publisher | Environmental science & technology |
| record_format | pubmed |
| spellingShingle | Two-Dimensional Liquid Chromatography Tandem Mass Spectrometry Untangles the Deep Metabolome of Marine Dissolved Organic Matter. Papadopoulos Lambidis, Stilianos Schramm, Tilman Steuer-Lodd, Karoline Farrell, Shane Stincone, Paolo Schmid, Robin Koester, Irina Torres, Ralph Dittmar, Thorsten Aluwihare, Lihini Simon, Carsten Petras, Daniel Tandem Mass Spectrometry Chromatography, Liquid Metabolome Seawater Organic Chemicals Two-Dimensional Liquid Chromatography Tandem Mass Spectrometry Untangles the Deep Metabolome of Marine Dissolved Organic Matter. Papadopoulos Lambidis, Stilianos Schramm, Tilman Steuer-Lodd, Karoline Farrell, Shane Stincone, Paolo Schmid, Robin Koester, Irina Torres, Ralph Dittmar, Thorsten Aluwihare, Lihini Simon, Carsten Petras, Daniel Tandem Mass Spectrometry Chromatography, Liquid Metabolome Seawater Organic Chemicals Dissolved organic matter (DOM) is an ultracomplex mixture that plays a central role in global biogeochemical cycles. Despite its importance, DOM remains poorly understood at the molecular level. Over the last decades, significant efforts have been made to decipher the chemical composition of DOM by high-resolution mass spectrometry (HR-MS) and liquid chromatography (LC) coupled with tandem mass spectrometry (MS/MS). Yet, the complexity and high degree of nonresolved isomers still hamper the full structural analysis of DOM. To address this challenge, we developed an offline two-dimensional (2D) LC approach using two reversed-phase dimensions with orthogonal pH levels, followed by MS/MS data acquisition and molecular networking. 2D-LC-MS/MS reduced the complexity of DOM, enhancing the quality of MS/MS spectra and increasing spectral annotation rates. Applying our approach to analyze coastal-surface DOM from Southern California (USA) and open-ocean DOM from the central North Pacific (Hawaii), we annotated in total more than 600 structures via MS/MS spectrum matching, which was up to 90% more than that in iterative 1D LC-MS/MS analysis with the same total run time. Our data offer unprecedented insights into the molecular composition of marine DOM and highlight the potential of 2D-LC-MS/MS approaches to decipher the chemical composition of ultracomplex samples. |
| title | Two-Dimensional Liquid Chromatography Tandem Mass Spectrometry Untangles the Deep Metabolome of Marine Dissolved Organic Matter. |
| topic | Tandem Mass Spectrometry Chromatography, Liquid Metabolome Seawater Organic Chemicals |
| url | https://pubmed.ncbi.nlm.nih.gov/39413296/ |