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Sulfur isotope fractionations constrain the biological cycling of dimethylsulfoniopropionate in the upper ocean

Osorio‐Rodriguez, Daniela and Razo-Mejia, Manuel and Dalleska, Nathan F. and Sessions, Alex L. and Orphan, Victoria J. and Adkins, Jess F. (2021) Sulfur isotope fractionations constrain the biological cycling of dimethylsulfoniopropionate in the upper ocean. Limnology and Oceanography, 66 (10). pp. 3607-3618. ISSN 0024-3590. doi:10.1002/lno.11901. https://resolver.caltech.edu/CaltechAUTHORS:20210817-204334443

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Abstract

The rapid turnover of dimethylsulfoniopropionate (DMSP), likely the most relevant dissolved organic sulfur compound in the surface ocean, makes it pivotal to understand the cycling of organic sulfur. Dimethylsulfoniopropionate is mainly synthesized by phytoplankton, and it can be utilized as carbon and sulfur sources by marine bacteria or cleaved by bacteria or algae to produce the volatile compound dimethylsulfide (DMS), involved in the formation of sulfate aerosols. The fluxes between the consumption (i.e., demethylation) and cleavage pathways are thought to depend on community interactions and their sulfur demand. However, a quantitative assessment of the sulfur partitioning between each of these pathways is still missing. Here, we report for the first time the sulfur isotope fractionations by enzymes involved in DMSP degradation with different catalytic mechanisms, expressed heterologously in Escherichia coli. We show that the residual DMSP from the demethylation pathway is 2.7‰ enriched in δ ³⁴S relative to the initial DMSP, and that the fractionation factor (³⁴ε) of the cleavage pathways varies between −1 and −9‰. The incorporation of these fractionation factors into mass balance calculations constrains the biological fates of DMSP in seawater, supports the notion that demethylation dominates over cleavage in marine environments, and could be used as a proxy for the dominant pathways of degradation of DMSP by marine microbial communities.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1002/lno.11901DOIArticle
ORCID:
AuthorORCID
Osorio‐Rodriguez, Daniela0000-0001-6676-4124
Razo-Mejia, Manuel0000-0002-9510-0527
Dalleska, Nathan F.0000-0002-2059-1587
Sessions, Alex L.0000-0001-6120-2763
Orphan, Victoria J.0000-0002-5374-6178
Adkins, Jess F.0000-0002-3174-5190
Additional Information:© 2021 The Authors. Limnology and Oceanography published by Wiley Periodicals LLC on behalf of Association for the Sciences of Limnology and Oceanography. This is an open access article under the terms of the Creative Commons Attribution-NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes. Issue Online: 09 October 2021; Version of Record online: 24 July 2021; Manuscript accepted: 05 July 2021; Manuscript revised: 22 March 2021; Manuscript received: 27 November 2020. We thank Dan Tawfik and Lei Lei (Weizmann Institute of Science), and William Whitman and Joe Wirth (University of Georgia, Athens), who kindly provided us the recombinant E. coli strains with DMSP lyases and DmdA, respectively. Guillem Salazar helped with the arrangement of the transcriptomic data. We also thank Reto Wijker, Elliot Mueller, and Thomas Hanson for useful discussions, as well as John Crounse, Fenfang Wu, and Alex Phillips for both input and technical assistance. UPLC/Q-TOF-MS was performed in the Caltech Environmental Analysis Center, which is supported by the Caltech Environmental Science and Engineering program and the Beckman Institute at Caltech. This work was supported by the Caltech Center for Environmental Microbial Interactions (CEMI) Training Grant to DOR and the National Science Foundation Grant 53994-ND2 to all authors. Conflict of Interest: None declared.
Group:Caltech Center for Environmental Microbial Interactions (CEMI)
Funders:
Funding AgencyGrant Number
Caltech Center for Environmental Microbial Interactions (CEMI)UNSPECIFIED
Caltech Beckman InstituteUNSPECIFIED
NSF53994-ND2
Issue or Number:10
DOI:10.1002/lno.11901
Record Number:CaltechAUTHORS:20210817-204334443
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210817-204334443
Official Citation:Osorio-Rodriguez, D., Razo-Mejia, M., Dalleska, N.F., Sessions, A.L., Orphan, V.J. and Adkins, J.F. (2021), Sulfur isotope fractionations constrain the biological cycling of dimethylsulfoniopropionate in the upper ocean. Limnol Oceanogr, 66: 3607-3618. https://doi.org/10.1002/lno.11901
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:110297
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:18 Aug 2021 21:47
Last Modified:12 Oct 2021 22:05

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