Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size

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

doi:10.1021/acs.est.3c06516

Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size

Journal Article · Wed Jan 17 00:00:00 EST 2024 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.3c06516· OSTI ID:2345204

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Washington Univ., St. Louis, MO (United States)

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. Here, 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.

View Accepted Manuscript (DOE)

Research Organization:: Washington Univ., St. Louis, MO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0022213; AC02-06CH11357

OSTI ID:: 2345204

Journal Information:: Environmental Science and Technology, Vol. 58, Issue 4; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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