Details zur Publikation

Kategorie Textpublikation
Referenztyp Zeitschriften
DOI 10.1021/acs.est.4c07173
Volltext Autorenversion
Titel (primär) Two-dimensional liquid chromatography tandem mass spectrometry untangles the deep metabolome of marine dissolved organic matter
Autor Papadopoulos Lambidis, S.; Schramm, T.; Steuer-Lodd, K.; Farrell, S.; Stincone, P.; Schmid, R.; Koester, I.; Torres, R.; Dittmar, T.; Aluwihare, L.; Simon, C. ORCID logo ; Petras, D.
Quelle Environmental Science & Technology
Erscheinungsjahr 2024
Department EAC
Band/Volume 58
Heft 43
Seite von 19289
Seite bis 19304
Sprache englisch
Topic T9 Healthy Planet
Supplements https://pubs.acs.org/doi/10.1021/acs.est.4c07173?goto=supporting-info
Keywords dissolved organic matter; 2D chromatography; 2D-LC-MS/MS; tandem mass spectrometry; environmental metabolomics; molecular networking
Abstract 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.
dauerhafte UFZ-Verlinkung https://www.ufz.de/index.php?en=20939&ufzPublicationIdentifier=30129
Papadopoulos Lambidis, S., Schramm, T., Steuer-Lodd, K., Farrell, S., Stincone, P., Schmid, R., Koester, I., Torres, R., Dittmar, T., Aluwihare, L., Simon, C., Petras, D. (2024):
Two-dimensional liquid chromatography tandem mass spectrometry untangles the deep metabolome of marine dissolved organic matter
Environ. Sci. Technol. 58 (43), 19289 - 19304 10.1021/acs.est.4c07173