Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size

Ledingham, Greg; Fang, Yihang; Catalano, Jeffrey G

doi:10.7936/6rxs-103704

Title: Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size

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Abstract

The dynamics of trace metals at mineral surfaces influence their fate and bioaccessibility in the environment. Trace metals on iron (oxyhydr)oxide surfaces display adsorption–desorption hysteresis, suggesting entrapment after aging. However, desorption experiments may perturb the coordination environment of adsorbed metals, the distribution of labile Fe(III), and mineral aggregation properties, influencing the interpretation of labile metal fractions. In this study, we investigated irreversible binding of nickel, zinc, and cadmium to goethite after aging times of 2–120 days using isotope exchange. Dissolved and adsorbed metal pools exchange rapidly, with half times <90 min, but all metals display a solid-associated fraction inaccessible to isotope exchange. The size of this nonlabile pool is the largest for nickel, with the smallest ionic radius, and the smallest for cadmium, with the largest ionic radius. Spectroscopy and extractions suggest that the irreversibly bound metals are incorporated in the goethite structure. Rapid exchange of labile solid-associated metals with solution demonstrates that adsorbed metals can sustain the dissolved pool in response to biological uptake or fluid flow. Trace metal fractions that irreversibly bind following adsorption provide a contaminant sequestration pathway, limit the availability of micronutrients, and record metal isotope signatures of environmental processes.

Authors:

Ledingham, Greg; Fang, Yihang;

Washington Univ., St. Louis, MO (United States); Washington University in St. Louis
Washington Univ., St. Louis, MO (United States)

Publication Date:: Tue Jul 16 04:00:00 UTC 2024

Other Number(s):: 103704

DOE Contract Number:: SC0022213

Research Org.:: Washington Univ., St. Louis, MO (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Subject:: 58 GEOSCIENCES; adsorption; goethite; incorporation; isotope exchange; trace metals

OSTI Identifier:: 2403545

DOI:: https://doi.org/10.7936/6rxs-103704

Citation Formats


                    Ledingham, Greg, Fang, Yihang, and Catalano, Jeffrey G. Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size.  United States: N. p., 2024. 
        Web.  doi:10.7936/6rxs-103704.

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                    Ledingham, Greg, Fang, Yihang, & Catalano, Jeffrey G. Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size.  United States.  doi:https://doi.org/10.7936/6rxs-103704

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                    Ledingham, Greg, Fang, Yihang, and Catalano, Jeffrey G. 2024.  
"Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size".  United States.  doi:https://doi.org/10.7936/6rxs-103704.  https://www.osti.gov/servlets/purl/2403545. Pub date:Tue Jul 16 04:00:00 UTC 2024

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@article{osti_2403545,

  title        = {Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size},

  author       = {Ledingham, Greg and Fang, Yihang and Catalano, Jeffrey G},

  abstractNote = {The dynamics of trace metals at mineral surfaces influence their fate and bioaccessibility in the environment. Trace metals on iron (oxyhydr)oxide surfaces display adsorption–desorption hysteresis, suggesting entrapment after aging. However, desorption experiments may perturb the coordination environment of adsorbed metals, the distribution of labile Fe(III), and mineral aggregation properties, influencing the interpretation of labile metal fractions. In this study, we investigated irreversible binding of nickel, zinc, and cadmium to goethite after aging times of 2–120 days using isotope exchange. Dissolved and adsorbed metal pools exchange rapidly, with half times <90 min, but all metals display a solid-associated fraction inaccessible to isotope exchange. The size of this nonlabile pool is the largest for nickel, with the smallest ionic radius, and the smallest for cadmium, with the largest ionic radius. Spectroscopy and extractions suggest that the irreversibly bound metals are incorporated in the goethite structure. Rapid exchange of labile solid-associated metals with solution demonstrates that adsorbed metals can sustain the dissolved pool in response to biological uptake or fluid flow. Trace metal fractions that irreversibly bind following adsorption provide a contaminant sequestration pathway, limit the availability of micronutrients, and record metal isotope signatures of environmental processes.},

  doi          = {10.7936/6rxs-103704},

  journal      = {},

  number       = ,

  volume       = ,

  place        = {United States},

  year         = {Tue Jul 16 04:00:00 UTC 2024},

  month        = {Tue Jul 16 04:00:00 UTC 2024}

}

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DOI: https://doi.org/10.7936/6rxs-103704

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Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size

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