Relating Molecular Properties to the Persistence of Marine Dissolved Organic Matter with Liquid Chromatography–Ultrahigh-Resolution Mass Spectrometry

Boiteau, Rene M.; Corilo, Yuri E.; Kew, William R.; Dewey, Christian; Alvarez Rodriguez, Maria Cristina; Carlson, Craig A.; Conway, Tim M.

doi:10.1021/acs.est.3c08245

Relating Molecular Properties to the Persistence of Marine Dissolved Organic Matter with Liquid Chromatography–Ultrahigh-Resolution Mass Spectrometry

Journal Article · Fri Feb 09 00:00:00 EST 2024 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.3c08245· OSTI ID:2405130

^[1]; Corilo, Yuri E. ^[2]; ^[2]; ^[3]; Alvarez Rodriguez, Maria Cristina ^[4]; Carlson, Craig A. ^[5]; Conway, Tim M. ^[6]

Oregon State Univ., Corvallis, OR (United States); Univ. of Minnesota, Minneapolis, MN (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)
Univ. of Minnesota, Minneapolis, MN (United States)
Oregon State Univ., Corvallis, OR (United States)
Univ. of California, Santa Barbara, CA (United States)
Univ. of South Florida, St. Petersburg, FL (United States)

Marine dissolved organic matter (DOM) contains a complex mixture of small molecules that eludes rapid biological degradation. Spatial and temporal variations in the abundance of DOM reflect the existence of fractions that are removed from the ocean over different time scales, ranging from seconds to millennia. However, it remains unknown whether the intrinsic chemical properties of these organic components relate to their persistence. Here, we elucidate and compare the molecular compositions of distinct DOM fractions with different lability along a water column in the North Atlantic Gyre. Our analysis utilized ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry at 21 T coupled to liquid chromatography and a novel data pipeline developed in CoreMS that generates molecular formula assignments and metrics of isomeric complexity. Clustering analysis binned 14 857 distinct molecular components into groups that correspond to the depth distribution of semilabile, semirefractory, and refractory fractions of DOM. The more labile fractions were concentrated near the ocean surface and contained more aliphatic, hydrophobic, and reduced molecules than the refractory fraction, which occurred uniformly throughout the water column. These findings suggest that processes that selectively remove hydrophobic compounds, such as aggregation and particle sorption, contribute to variable removal rates of marine DOM.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: Environmental Molecular Sciences Laboratory; National Science Foundation (NSF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2405130

Report Number(s):: PNNL-SA--182454

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 7 Vol. 58; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Relating Molecular Properties to the Persistence of Marine Dissolved Organic Matter with Liquid Chromatography–Ultrahigh-Resolution Mass Spectrometry

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