Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size
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 envir...
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| Veröffentlicht in: | Environmental science & technology 2024-01, Vol.58 (4), p.2007-2016 |
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| container_title | Environmental science & technology |
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| creator | Ledingham, Greg J. Fang, Yihang Catalano, Jeffrey G. |
| description | 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 |
| doi_str_mv | 10.1021/acs.est.3c06516 |
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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.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/acs.est.3c06516</identifier><identifier>PMID: 38232091</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Adsorption ; Aging ; Aging (metallurgy) ; Binding ; Bioavailability ; Cadmium ; Contaminants ; Desorption ; Entrapment ; Exchanging ; Fluid flow ; GEOSCIENCES ; Goethite ; Heavy metals ; incorporation ; Iron ; isotope exchange ; Metals ; Micronutrients ; Nickel ; Nutrient availability ; Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants ; Spectroscopy ; Surface chemistry ; Trace metals</subject><ispartof>Environmental science & technology, 2024-01, Vol.58 (4), p.2007-2016</ispartof><rights>2024 American Chemical Society</rights><rights>Copyright American Chemical Society Jan 30, 2024</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-a342t-28ace2683f6a9e789a20a340bfc73c62384ddbbe58b4966cb199945fa009bb0b3</cites><orcidid>0000-0001-8937-4209 ; 0000-0002-8218-5883 ; 0000-0001-9311-977X ; 000000019311977X ; 0000000189374209 ; 0000000282185883</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.est.3c06516$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.est.3c06516$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/38232091$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/servlets/purl/2345204$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Ledingham, Greg J.</creatorcontrib><creatorcontrib>Fang, Yihang</creatorcontrib><creatorcontrib>Catalano, Jeffrey G.</creatorcontrib><creatorcontrib>Argonne National Laboratory (ANL), Argonne, IL (United States)</creatorcontrib><creatorcontrib>Washington Univ., St. Louis, MO (United States)</creatorcontrib><title>Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>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.</description><subject>Adsorption</subject><subject>Aging</subject><subject>Aging (metallurgy)</subject><subject>Binding</subject><subject>Bioavailability</subject><subject>Cadmium</subject><subject>Contaminants</subject><subject>Desorption</subject><subject>Entrapment</subject><subject>Exchanging</subject><subject>Fluid flow</subject><subject>GEOSCIENCES</subject><subject>Goethite</subject><subject>Heavy metals</subject><subject>incorporation</subject><subject>Iron</subject><subject>isotope exchange</subject><subject>Metals</subject><subject>Micronutrients</subject><subject>Nickel</subject><subject>Nutrient availability</subject><subject>Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants</subject><subject>Spectroscopy</subject><subject>Surface chemistry</subject><subject>Trace metals</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNp1kc1PGzEQxS1EBSlw5lZZcKmENoztXWMfIYI0ElUPUKk3y_bOkkWbNbUdJPrX11ECh0o9zWF-783HI-SUwZQBZ5fWpymmPBUeZMPkHpmwhkPVqIbtkwkAE5UW8tch-ZzSMwBwAeqAHArFBQfNJmS-iBFfMabeDUgfo_VIv2O2A73px7Yfn2gOdB4wL_uMdBbGHMMwYEvdG81LpIsw0of-Dx6TT50dEp7s6hH5eXf7OPtW3f-YL2bX95UVNc8VV2UAl0p00mq8UtpyKB1wnb8SXnKh6rZ1Dhvlai2ld0xrXTedBdDOgRNH5GzrG1LuTfJlK7_0YRzRZ8NFXa6vC_R1C73E8Htd_mNWffI4DHbEsE6GayZrULoRBT3_B30O6ziWEwrFQcpGgSzU5ZbyMaQUsTMvsV_Z-GYYmE0QpgRhNupdEEXxZee7ditsP_j3zxfgYgtslB8z_2f3F5CKkUE</recordid><startdate>20240130</startdate><enddate>20240130</enddate><creator>Ledingham, Greg J.</creator><creator>Fang, Yihang</creator><creator>Catalano, Jeffrey G.</creator><general>American Chemical Society</general><general>American Chemical Society (ACS)</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope><scope>7X8</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0001-8937-4209</orcidid><orcidid>https://orcid.org/0000-0002-8218-5883</orcidid><orcidid>https://orcid.org/0000-0001-9311-977X</orcidid><orcidid>https://orcid.org/000000019311977X</orcidid><orcidid>https://orcid.org/0000000189374209</orcidid><orcidid>https://orcid.org/0000000282185883</orcidid></search><sort><creationdate>20240130</creationdate><title>Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size</title><author>Ledingham, Greg J. ; Fang, Yihang ; Catalano, Jeffrey G.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a342t-28ace2683f6a9e789a20a340bfc73c62384ddbbe58b4966cb199945fa009bb0b3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Adsorption</topic><topic>Aging</topic><topic>Aging (metallurgy)</topic><topic>Binding</topic><topic>Bioavailability</topic><topic>Cadmium</topic><topic>Contaminants</topic><topic>Desorption</topic><topic>Entrapment</topic><topic>Exchanging</topic><topic>Fluid flow</topic><topic>GEOSCIENCES</topic><topic>Goethite</topic><topic>Heavy metals</topic><topic>incorporation</topic><topic>Iron</topic><topic>isotope exchange</topic><topic>Metals</topic><topic>Micronutrients</topic><topic>Nickel</topic><topic>Nutrient availability</topic><topic>Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants</topic><topic>Spectroscopy</topic><topic>Surface chemistry</topic><topic>Trace metals</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ledingham, Greg J.</creatorcontrib><creatorcontrib>Fang, Yihang</creatorcontrib><creatorcontrib>Catalano, Jeffrey G.</creatorcontrib><creatorcontrib>Argonne National Laboratory (ANL), Argonne, IL (United States)</creatorcontrib><creatorcontrib>Washington Univ., St. Louis, MO (United States)</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ledingham, Greg J.</au><au>Fang, Yihang</au><au>Catalano, Jeffrey G.</au><aucorp>Argonne National Laboratory (ANL), Argonne, IL (United States)</aucorp><aucorp>Washington Univ., St. Louis, MO (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2024-01-30</date><risdate>2024</risdate><volume>58</volume><issue>4</issue><spage>2007</spage><epage>2016</epage><pages>2007-2016</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><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. 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| subjects | Adsorption Aging Aging (metallurgy) Binding Bioavailability Cadmium Contaminants Desorption Entrapment Exchanging Fluid flow GEOSCIENCES Goethite Heavy metals incorporation Iron isotope exchange Metals Micronutrients Nickel Nutrient availability Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants Spectroscopy Surface chemistry Trace metals |
| title | Irreversible Trace Metal Binding to Goethite Controlled by the Ion Size |
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