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Title: Rare earth element behavior during groundwater–seawater mixing along the Kona Coast of Hawaii

Abstract

Groundwater and seawater samples were collected from nearshore wells and offshore along the Kona Coast of the Big Island of Hawaii to investigate rare earth element (REE) behavior in local subterranean estuaries. Previously we saw that submarine groundwater discharge (SGD) is the predominant flux of terrestrial waters to the coastal ocean along the arid Kona Coast of Hawaii. Groundwater and seawater samples were filtered through 0.45 μm and 0.02 μm pore-size filters to evaluate the importance of colloidal and soluble (i.e., truly dissolved ionic species and/or low molecular weight [LMW] colloids) fractions of the REEs in the local subterranean estuaries. Mixing experiments using groundwater collected immediately down gradient from a wastewater treatment facility (WWTF) proximal to the Kaloko-Hanokohau National Historic Park, and more “pristine” groundwater from a well constructed in a lava tube at Kiholo Bay, were conducted with local seawater to study the effect of solution composition (i.e., pH, salinity) on the concentrations and fractionation behavior of the REEs as groundwater mixes with seawater in Kona Coast subterranean estuaries. The mixed waters were also filtered through 0.45 or 0.02 μm filters to ascertain the behavior of colloidal and soluble fractions of the REEs across the salinity gradient in eachmore » mixing experiment. Concentrations of the REEs were statistically identical (two-tailed Student t-test, 95% confidence) between the sequentially filtered sample aliquots, indicating that the REEs occur as dissolved ionic species and/or LMW colloids in Kona Coast groundwaters. The mixing experiments revealed that the REEs are released to solution from suspended particles or colloids when Kona Coast groundwater waters mix with local seawater. The order of release that accompanies increasing pH and salinity follows light REE (LREE) > middle REE (MREE) > heavy REE (HREE). Release of REEs in the mixing experiments is driven by decreases in the free metal ion activity in solution and the concomitant increase in the amount of each REE that occurs in solution as dicarbonato complexes [i.e., Ln(CO3)2-] as pH increases across the salinity gradient. Input-normalized REE patterns of Kona Coast groundwater and coastal seawater are nearly identical and relatively flat compared to North Pacific seawater, indicating that SGD is the chief source of these trace elements to the ocean along the Kona Coast. Additionally, REE concentrations of the coastal seawater are between 10 and 50 times higher than previously reported open-ocean seawater values from the North Pacific, further demonstrating the importance of SGD fluxes of REEs to these coastal waters. Altogether, these observations indicate that large-scale removal of REEs, which characterizes the behavior of REEs in the low salinity reaches of many surface estuaries, is not a feature of the subterranean estuary along the Kona Coast. A large positive gadolinium (Gd) anomaly characterizes groundwater from the vicinity of the WWTF. The positive Gd anomaly can be traced to the coastal ocean, providing further evidence of the impact of SGD on the coastal waters. Estimates of the SGD fluxes of the REEs to the coastal ocean along the Kona Coast (i.e., 1.3–2.6 mmol Nd day-1) are similar to recent estimates of SGD fluxes of REEs along Florida’s east coast and to Rhode Island Sound, all of which points to the importance of SGD as significant flux of REEs to the coastal ocean.« less

Authors:
 [1];  [1];  [2];  [3];  [4];  [1];  [5];  [1];  [6]
+ Show Author Affiliations
  1. Tulane Univ., New Orleans, LA (United States). Dept. of Earth and Environmental Sciences
  2. Univ. of Hawaii, Honolulu, HI (United States). Dept. of Geology and Geophysics
  3. U.S. Geological Survey, Santa Cruz, CA (United States). Pacific Coastal and Marine Science Center
  4. U.S. Geological Survey, Santa Cruz, CA (United States). Pacific Coastal and Marine Science Center; International Atmoic Energy Agency, Vienna (Austria)
  5. Tulane Univ., New Orleans, LA (United States). Dept. of Earth and Environmental Sciences; Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  6. Old Dominion Univ., Norfolk, VA (United States). Dept. of Ocean, Earth and Atmospheric Sciences
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
National Science Foundation (NSF)
OSTI Identifier:
1416299
Report Number(s):
LA-UR-17-27500
Journal ID: ISSN 0016-7037; TRN: US1800907
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 198; Journal Issue: C; Journal ID: ISSN 0016-7037
Publisher:
The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; rare earth elements; submarine groundwater discharge; coastal ocean; subterranean estuary; hawaii

Citation Formats

Johannesson, Karen H., Palmore, C. Dianne, Fackrell, Joseph, Prouty, Nancy G., Swarzenski, Peter W., Chevis, Darren A., Telfeyan, Katherine, White, Christopher D., and Burdige, David J. Rare earth element behavior during groundwater–seawater mixing along the Kona Coast of Hawaii. United States: N. p., 2016. Web. doi:10.1016/j.gca.2016.11.009.
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Johannesson, Karen H., Palmore, C. Dianne, Fackrell, Joseph, Prouty, Nancy G., Swarzenski, Peter W., Chevis, Darren A., Telfeyan, Katherine, White, Christopher D., & Burdige, David J. Rare earth element behavior during groundwater–seawater mixing along the Kona Coast of Hawaii. United States. https://doi.org/10.1016/j.gca.2016.11.009
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Johannesson, Karen H., Palmore, C. Dianne, Fackrell, Joseph, Prouty, Nancy G., Swarzenski, Peter W., Chevis, Darren A., Telfeyan, Katherine, White, Christopher D., and Burdige, David J. Mon . "Rare earth element behavior during groundwater–seawater mixing along the Kona Coast of Hawaii". United States. https://doi.org/10.1016/j.gca.2016.11.009. https://www.osti.gov/servlets/purl/1416299.
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@article{osti_1416299,
title = {Rare earth element behavior during groundwater–seawater mixing along the Kona Coast of Hawaii},
author = {Johannesson, Karen H. and Palmore, C. Dianne and Fackrell, Joseph and Prouty, Nancy G. and Swarzenski, Peter W. and Chevis, Darren A. and Telfeyan, Katherine and White, Christopher D. and Burdige, David J.},
abstractNote = {Groundwater and seawater samples were collected from nearshore wells and offshore along the Kona Coast of the Big Island of Hawaii to investigate rare earth element (REE) behavior in local subterranean estuaries. Previously we saw that submarine groundwater discharge (SGD) is the predominant flux of terrestrial waters to the coastal ocean along the arid Kona Coast of Hawaii. Groundwater and seawater samples were filtered through 0.45 μm and 0.02 μm pore-size filters to evaluate the importance of colloidal and soluble (i.e., truly dissolved ionic species and/or low molecular weight [LMW] colloids) fractions of the REEs in the local subterranean estuaries. Mixing experiments using groundwater collected immediately down gradient from a wastewater treatment facility (WWTF) proximal to the Kaloko-Hanokohau National Historic Park, and more “pristine” groundwater from a well constructed in a lava tube at Kiholo Bay, were conducted with local seawater to study the effect of solution composition (i.e., pH, salinity) on the concentrations and fractionation behavior of the REEs as groundwater mixes with seawater in Kona Coast subterranean estuaries. The mixed waters were also filtered through 0.45 or 0.02 μm filters to ascertain the behavior of colloidal and soluble fractions of the REEs across the salinity gradient in each mixing experiment. Concentrations of the REEs were statistically identical (two-tailed Student t-test, 95% confidence) between the sequentially filtered sample aliquots, indicating that the REEs occur as dissolved ionic species and/or LMW colloids in Kona Coast groundwaters. The mixing experiments revealed that the REEs are released to solution from suspended particles or colloids when Kona Coast groundwater waters mix with local seawater. The order of release that accompanies increasing pH and salinity follows light REE (LREE) > middle REE (MREE) > heavy REE (HREE). Release of REEs in the mixing experiments is driven by decreases in the free metal ion activity in solution and the concomitant increase in the amount of each REE that occurs in solution as dicarbonato complexes [i.e., Ln(CO3)2-] as pH increases across the salinity gradient. Input-normalized REE patterns of Kona Coast groundwater and coastal seawater are nearly identical and relatively flat compared to North Pacific seawater, indicating that SGD is the chief source of these trace elements to the ocean along the Kona Coast. Additionally, REE concentrations of the coastal seawater are between 10 and 50 times higher than previously reported open-ocean seawater values from the North Pacific, further demonstrating the importance of SGD fluxes of REEs to these coastal waters. Altogether, these observations indicate that large-scale removal of REEs, which characterizes the behavior of REEs in the low salinity reaches of many surface estuaries, is not a feature of the subterranean estuary along the Kona Coast. A large positive gadolinium (Gd) anomaly characterizes groundwater from the vicinity of the WWTF. The positive Gd anomaly can be traced to the coastal ocean, providing further evidence of the impact of SGD on the coastal waters. Estimates of the SGD fluxes of the REEs to the coastal ocean along the Kona Coast (i.e., 1.3–2.6 mmol Nd day-1) are similar to recent estimates of SGD fluxes of REEs along Florida’s east coast and to Rhode Island Sound, all of which points to the importance of SGD as significant flux of REEs to the coastal ocean.},
doi = {10.1016/j.gca.2016.11.009},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 198,
place = {United States},
year = {Mon Nov 14 00:00:00 EST 2016},
month = {Mon Nov 14 00:00:00 EST 2016}
}
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Chemical evolution of rare earth elements: fractionation between colloidal and solution phases of filtered river water
journal, December 1992

The geochemistry of rare earth elements in the Amazon River estuary
journal, May 1993

The aquatic chemistry of rare earth elements in rivers and estuaries
journal, January 1995

The coagulation, solubility and adsorption properties of Fe, Mn, Cu, Ni, Cd, Co and humic acids in a river water
journal, February 1981

Cycling of dissolved rare earth elements in Chesapeake Bay
journal, June 1988

The estuarine chemistry of rare earth elements: comparison of the Amazon, Fly, Sepik and the Gulf of Papua systems
journal, June 2000

The pore water chemistry of rare earth elements in Buzzards Bay sediments
journal, November 1989

  • Sholkovitz, Edward R.; Piepgras, Donald J.; Jacobsen, Stein B.
  • Geochimica et Cosmochimica Acta, Vol. 53, Issue 11
  • DOI: 10.1016/0016-7037(89)90162-2

The geochemistry of rare earth elements in the seasonally anoxic water column and porewaters of Chesapeake Bay
journal, September 1992

Towards explaining the Nd paradox using reversible scavenging in an ocean general circulation model
journal, October 2008

  • Siddall, Mark; Khatiwala, Samar; van de Flierdt, Tina
  • Earth and Planetary Science Letters, Vol. 274, Issue 3-4
  • DOI: 10.1016/j.epsl.2008.07.044

Nutrient inputs to the coastal ocean through submarine groundwater discharge: controls and potential impact
journal, August 2004

Submarine groundwater discharge and nutrient addition to the coastal zone and coral reefs of leeward Hawai'i
journal, April 2008

Uranium geochemistry on the Amazon shelf: Chemical phase partitioning and cycling across a salinity gradient
journal, January 1995

Distribution of rare earth elements and neodymium isotopes in settling particulate material of the tropical Atlantic Ocean (EUMELI site)
journal, November 1997

  • Tachikawa, K.; Handel, C.; Dupré, B.
  • Deep Sea Research Part I: Oceanographic Research Papers, Vol. 44, Issue 11
  • DOI: 10.1016/S0967-0637(97)00057-5

A new approach to the Nd residence time in the ocean: the role of atmospheric inputs
journal, July 1999

Distribution of rare earth elements and neodymium isotopes in suspended particles of the tropical Atlantic Ocean (EUMELI site)
journal, May 1999

  • Tachikawa, K.; Jeandel, C.; Vangriesheim, A.
  • Deep Sea Research Part I: Oceanographic Research Papers, Vol. 46, Issue 5
  • DOI: 10.1016/S0967-0637(98)00089-2

Neodymium budget in the modern ocean and paleo-oceanographic implications
journal, January 2003

Hawaiian double volcanic chain triggered by an episodic involvement of recycled material: Constraints from temporal Sr–Nd–Hf–Pb isotopic trend of the Loa-type volcanoes
journal, January 2008

  • Tanaka, Ryoji; Makishima, Akio; Nakamura, Eizo
  • Earth and Planetary Science Letters, Vol. 265, Issue 3-4
  • DOI: 10.1016/j.epsl.2007.10.035

Adsorption of rare earth elements onto Carrizo sand: Experimental investigations and modeling with surface complexation
journal, November 2005

Ligand extraction of rare earth elements from aquifer sediments: Implications for rare earth element complexation with organic matter in natural waters
journal, December 2010

Rare earth elements adsorption onto Carrizo sand: Influence of strong solution complexation
journal, December 2010

Investigation of submarine groundwater discharge
journal, January 2002

  • Taniguchi, Makoto; Burnett, William C.; Cable, Jaye E.
  • Hydrological Processes, Vol. 16, Issue 11
  • DOI: 10.1002/hyp.1145

Aqueous Stability of Gadolinium in Surface Waters Receiving Sewage Treatment Plant Effluent, Boulder Creek, Colorado
journal, September 2005

  • Verplanck, Philip L.; Taylor, Howard E.; Nordstrom, D. Kirk
  • Environmental Science & Technology, Vol. 39, Issue 18
  • DOI: 10.1021/es048456u

Controls on the geochemistry of rare earth elements in sediments and groundwaters of the Aquia aquifer, Maryland, USA
journal, June 2011

Submarine groundwater discharge: A large, previously unrecognized source of dissolved iron to the South Atlantic Ocean
journal, December 2006

Halloysite as a kinetically controlled end product of arid-zone basalt weathering
journal, December 2003

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    Works referencing / citing this record:

    Gadolinium as an Emerging Microcontaminant in Water Resources: Threats and Opportunities
    journal, February 2019

    The Influence of Basaltic Islands on the Oceanic REE Distribution: A Case Study From the Tropical South Pacific
    journal, March 2018

    • Molina-Kescher, Mario; Hathorne, Ed C.; Osborne, Anne H.
    • Frontiers in Marine Science, Vol. 5
    • DOI: 10.3389/fmars.2018.00050

    Gadolinium as a new emerging contaminant of aquatic environments: Gadolinium as a new emerging contaminant
    journal, April 2018

    • Rogowska, Justyna; Olkowska, Ewa; Ratajczyk, Wojciech
    • Environmental Toxicology and Chemistry, Vol. 37, Issue 6
    • DOI: 10.1002/etc.4116

    Rare earth element geochemistry characteristics of seawater and porewater from deep sea in western Pacific
    journal, November 2017

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