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Changing chemistry of particulate manganese in the near- and far-field hydrothermal plumes from 15°S East Pacific Rise and its influence on metal scavenging

Lee, Jong-Mi and Lam, Phoebe J. and Vivancos, Sebastián M. and Pavia, Frank J. and Anderson, Robert F. and Lu, Yanbin and Cheng, Hai and Zhang, Pu and Edwards, R. Lawrence and Xiang, Yang and Webb, Samuel M. (2021) Changing chemistry of particulate manganese in the near- and far-field hydrothermal plumes from 15°S East Pacific Rise and its influence on metal scavenging. Geochimica et Cosmochimica Acta, 300 . pp. 95-118. ISSN 0016-7037. https://resolver.caltech.edu/CaltechAUTHORS:20210223-075234781

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Abstract

Dissolved Mn(II) in the hydrothermal plume is known to be microbially oxidized to form Mn(III/IV) oxides, and the Mn oxides scavenge other trace elements in seawater. In the GEOTRACES GP16 cruise, dissolved Mn (dMn) and particulate Mn (pMn) were found to be transported over 4000 km westwards from the Southern Eastern Pacific Rise. Previous studies in this plume showed different removal rates of dMn and pMn as well as pMn size distribution between the near-field (<80 km from the ridge axis) and far-field (>80 km) plumes. In order to understand Mn cycling in these plumes, spatial distribution, oxidation states, and mineral structures of Mn in small size fraction (SSF; 0.8–51 μm) and large size fraction (LSF; >51 μm) particles from the near-field and far-field plumes were examined using micro X-ray fluorescence spectrometry (μ-XRF), X-ray absorption near-edge structure spectroscopy (XANES), chemical species mapping, and extended X-ray absorption fine-structure spectroscopy (EXAFS). In the near-field plume, pMn in the SSF is dominated by oxidized Mn with Mn(III) fractions of ∼30%. They are a mixture of δ-MnO₂ and triclinic birnessites that is known to be formed as a result of autocatalytic Mn(II) oxidation at the surface of freshly-formed δ-MnO₂, suggesting that both microbial and autocatalytic Mn oxidation occur in the near-field plume. The LSF pMn in the near-field plume is also oxidized and often found in large aggregates several hundreds of μm in size. These aggregates settle out in the near-field and during transport, and are not found in the far-field plume. In the far-field plume where Mn oxides are not newly formed, pMn in the SSF is oxidized, but their Mn(III) fractions are smaller than in the near-field pMn. Unlike the SSF, the far-field plume LSF pMn is dominated by reduced Mn, implying very slow aggregation of pMn in the far-field plume. The different characteristics of pMn between the near-field and far-field plumes affect its scavenging of other trace elements. In the near-field plume, Co, Mo, ²³¹Pa are associated with pMn, but not in the far-field plume. ²³¹Pa is adsorbed to pFe rather than pMn in the far-field plume, and Pb is adsorbed to pFe in the entire plume. The result shows that freshly-formed Mn oxides in the near-field plume have higher scavenging capacity than the far-field plume pMn. Our findings suggest that the mineralogical age of Mn oxides may be an important parameter that controls the scavenging of many other trace elements and isotopes.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.gca.2021.02.020DOIArticle
https://www.bco-dmo.org/dataset/668083Related ItemData
https://www.bco-dmo.org/dataset/676231Related ItemData
ORCID:
AuthorORCID
Vivancos, Sebastián M.0000-0002-8057-5685
Pavia, Frank J.0000-0003-3627-0179
Anderson, Robert F.0000-0002-8472-2494
Zhang, Pu0000-0002-7509-1694
Additional Information:© 2021 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). Received 26 August 2020, Accepted 13 February 2021, Available online 22 February 2021. We would like to thank Dan Ohnemus, Erin Black, Sarah Nicholas and S. Pike for operating in-situ pumps and processing particle samples on board during the GP16 cruise. The authors also thank Sirine Fakra and Sharon Bone for their support at the ALS and SSRL facilities and Martin Fleisher for operating the LDEO ICP-MS facility. Portions of this research were carried out at the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231, and at the Stanford Synchrotron Radiation Lightsource, supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The SSRL Structural Molecular Biology Program is supported by the DOE Office of Biological and Environmental Research, and by the National Institutes of Health, National Institute of General Medical Sciences (P30GM133894). The contents of this publication are solely the responsibility of the authors and do not necessarily represent the official views of NIGMS or NIH. This research was supported by the Chemical Oceanography program through the National Science Foundation under grant number NSF OCE-1518110 to PJL, NSF OCE-1233688 to RFA and MQF, and NSF OCE-1233903 to RLE and HC. The particulate trace elements (pTE) and ²³¹Pa (p²³¹Pa) concentrations data from the U.S. GEOTRACES EPZT cruise can be found at the Biological and Chemical Oceanography Data Management Office (BCO-DMO): https://www.bco-dmo.org/dataset/668083 for pTE and http://www.bco-dmo.org/dataset/676231 for p²³¹Pa. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-05CH11231
Department of Energy (DOE)DE-AC02-76SF00515
NIHP30GM133894
NSFOCE-1518110
NSFOCE-1233688
NSFOCE-1233903
Subject Keywords:Manganese; Particle chemistry; Hydrothermal plume particles; Scavenging; Micro X-ray fluorescence (μ-XRF) spectrometry; X-ray absorption near edge structure (XANES) spectroscopy; X-ray microprobe chemical speciation mapping; Extended X-ray absorption fine-structure (EXAFS) spectroscopy; East Pacific Rise; GEOTRACES GP16; Eastern Pacific Zonal Transect
Record Number:CaltechAUTHORS:20210223-075234781
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210223-075234781
Official Citation:Jong-Mi Lee, Phoebe J. Lam, Sebastian M. Vivancos, Frank J. Pavia, Robert F. Anderson, Yanbin Lu, Hai Cheng, Pu Zhang, R. Lawrence Edwards, Yang Xiang, Samuel M. Webb, Changing chemistry of particulate manganese in the near- and far-field hydrothermal plumes from 15°S East Pacific Rise and its influence on metal scavenging, Geochimica et Cosmochimica Acta, Volume 300, 2021, Pages 95-118, ISSN 0016-7037, https://doi.org/10.1016/j.gca.2021.02.020. (https://www.sciencedirect.com/science/article/pii/S0016703721001150)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108148
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:23 Feb 2021 18:17
Last Modified:25 Mar 2021 21:19

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