Short-Term Inhibition and Long-Term Enhancement of Irreversible Trace Metal Binding to Goethite in Multi-Metal Systems

Ledingham, Greg J.; Custis, Andrew T.; Fang, Yihang; Catalano, Jeffrey G.

doi:10.1021/acs.est.5c03866

Short-Term Inhibition and Long-Term Enhancement of Irreversible Trace Metal Binding to Goethite in Multi-Metal Systems

Journal Article · Thu Jun 12 00:00:00 EDT 2025 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.5c03866· OSTI ID:2570445

^[1]; Custis, Andrew T. ^[1]; ^[1]; ^[1]

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

Iron (oxyhydr)oxide minerals are important sorbents of trace metals in aquatic environments. Adsorption–desorption hysteresis has been documented for trace metals after aging, suggesting that they become incorporated over time. We previously found that ion size controls the extent of irreversible metal binding of single metals to goethite. In this study, we evaluate how the presence of multiple metals influences irreversible binding. Mixed Ni–Zn and Ni–Cd solutions were aged with goethite at pH 7 for 2 days, 30 days, and 60 days, after which isotope exchange experiments were performed to assess the lability of the adsorbed metal pools. After 2 days of aging, Ni and Cd in mixed-metal systems were more labile than in single-metal systems, indicating that competitive adsorption may partially block irreversible binding on short time scales. After 60 days, all three metals had larger irreversibly bound fractions than in single-metal systems. X-ray absorption near-edge structure (XANES) spectroscopy indicates that irreversibly bound fractions correlate with incorporation into goethite. This study demonstrates that pools of coadsorbed metals are bioaccessible on a time scale of minutes. Cooperative effects promote the structural sequestration of even large trace metals, causing reactive transport models to likely overpredict metal mobility. Long-term metal entrapment processes hinder micronutrient availability, impact contaminant sequestration and critical mineral recovery, and yield complex pathways through which metal solubilization may be enhanced or hindered during redox cycling.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Advanced Photon Source (APS)

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

OSTI ID:: 2570445

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 24 Vol. 59; ISSN 1520-5851; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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