Arsenic Species Formed from Arsenopyrite Weathering along a Contamination Gradient in Circumneutral River Floodplain Soils
Arsenic is a toxic trace element, which commonly occurs as contaminant in riverine floodplains and associated wetlands affected by mining and ore processing. In this study, we investigated the solid-phase speciation of As in river floodplain soils characterized by circumneutral pH (5.7–7.1) and As c...
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| Veröffentlicht in: | Environ. Sci. Technol 2014-01, Vol.48 (1), p.208-217 |
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| creator | Mandaliev, Petar N Mikutta, Christian Barmettler, Kurt Kotsev, Tsvetan Kretzschmar, Ruben |
| description | Arsenic is a toxic trace element, which commonly occurs as contaminant in riverine floodplains and associated wetlands affected by mining and ore processing. In this study, we investigated the solid-phase speciation of As in river floodplain soils characterized by circumneutral pH (5.7–7.1) and As concentrations of up to 40.3 g/kg caused by former mining of arsenopyrite-rich ores. Soil samples collected in the floodplain of Ogosta River (Bulgaria) were size-fractionated and subsequently analyzed using a combination of X-ray fluorescence (XRF) spectrometry, powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and selective chemical extraction of poorly crystalline mineral phases. Arsenic and Fe were found to be spatially correlated and both elements were strongly enriched in the fine soil particle size fractions ( |
| doi_str_mv | 10.1021/es403210y |
| format | Article |
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(ANL), Argonne, IL (United States). Advanced Photon Source (APS)</creatorcontrib><description>Arsenic is a toxic trace element, which commonly occurs as contaminant in riverine floodplains and associated wetlands affected by mining and ore processing. In this study, we investigated the solid-phase speciation of As in river floodplain soils characterized by circumneutral pH (5.7–7.1) and As concentrations of up to 40.3 g/kg caused by former mining of arsenopyrite-rich ores. Soil samples collected in the floodplain of Ogosta River (Bulgaria) were size-fractionated and subsequently analyzed using a combination of X-ray fluorescence (XRF) spectrometry, powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and selective chemical extraction of poorly crystalline mineral phases. Arsenic and Fe were found to be spatially correlated and both elements were strongly enriched in the fine soil particle size fractions (<2 μm and 2–50 μm). Between 14 and 82% of the total As was citrate-ascorbate extractable. Molar As/Fe ratios were as high as 0.34 in the bulk soil extracts and increased up to 0.48 in extracts of the fine particle size fractions. Arsenic K-edge XAS spectra showed the predominance of As(V) and were well fitted with a reference spectrum of As(V) adsorbed to ferrihydrite. Whereas no As(III) was detected, considerable amounts of As(-I) were present and identified as arsenopyrite originating from the mining waste. Iron K-edge XAS revealed that in addition to As(V) adsorbed to ferrihydrite, X-ray amorphous As(V)-rich hydrous ferric oxides (“As-HFO”) with a reduced number of corner-sharing FeO6 octahedra relative to ferrihydrite were the dominating secondary As species in the soils. The extremely high concentrations of As in the fine particle size fractions (up to 214 g/kg) and its association with poorly crystalline Fe(III) oxyhydroxides and As-HFO phases suggest a high As mobilization potential under both oxic and anoxic conditions, as well as a high bioaccessibility of As upon ingestion, dermal contact, or inhalation by humans or animals.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/es403210y</identifier><identifier>PMID: 24283255</identifier><identifier>CODEN: ESTHAG</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Applied sciences ; Arsenic ; Arsenic - analysis ; Arsenic - chemistry ; Arsenicals - chemistry ; Biological and physicochemical properties of pollutants. Interaction in the soil ; Bulgaria ; Data collection ; Diffraction ; Earth sciences ; Earth, ocean, space ; Engineering and environment geology. Geothermics ; Exact sciences and technology ; Extraction processes ; Ferric Compounds - chemistry ; Floodplains ; Fluorescence ; Freshwater ; Iron - analysis ; Iron - chemistry ; Iron Compounds - chemistry ; Minerals - chemistry ; Mining ; Particle Size ; Pollution ; Pollution, environment geology ; Rivers ; Soil - chemistry ; Soil and sediments pollution ; Soil contamination ; Soil Pollutants - analysis ; Soil Pollutants - chemistry ; Spatial Analysis ; Spectrometry, X-Ray Emission ; Sulfides - chemistry ; X-Ray Absorption Spectroscopy ; X-Ray Diffraction</subject><ispartof>Environ. Sci. Technol, 2014-01, Vol.48 (1), p.208-217</ispartof><rights>Copyright © 2013 American Chemical Society</rights><rights>2015 INIST-CNRS</rights><rights>Copyright American Chemical Society Jan 7, 2014</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a499t-aa3fc40eff349ccba40ce58f83e6e057b2df37b68f1c8759fc6b7e88ac6bcddc3</citedby><cites>FETCH-LOGICAL-a499t-aa3fc40eff349ccba40ce58f83e6e057b2df37b68f1c8759fc6b7e88ac6bcddc3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/es403210y$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/es403210y$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,885,2765,27076,27924,27925,56738,56788</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=28268806$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/24283255$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1120975$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Mandaliev, Petar N</creatorcontrib><creatorcontrib>Mikutta, Christian</creatorcontrib><creatorcontrib>Barmettler, Kurt</creatorcontrib><creatorcontrib>Kotsev, Tsvetan</creatorcontrib><creatorcontrib>Kretzschmar, Ruben</creatorcontrib><creatorcontrib>Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)</creatorcontrib><title>Arsenic Species Formed from Arsenopyrite Weathering along a Contamination Gradient in Circumneutral River Floodplain Soils</title><title>Environ. Sci. Technol</title><addtitle>Environ. Sci. Technol</addtitle><description>Arsenic is a toxic trace element, which commonly occurs as contaminant in riverine floodplains and associated wetlands affected by mining and ore processing. In this study, we investigated the solid-phase speciation of As in river floodplain soils characterized by circumneutral pH (5.7–7.1) and As concentrations of up to 40.3 g/kg caused by former mining of arsenopyrite-rich ores. Soil samples collected in the floodplain of Ogosta River (Bulgaria) were size-fractionated and subsequently analyzed using a combination of X-ray fluorescence (XRF) spectrometry, powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and selective chemical extraction of poorly crystalline mineral phases. Arsenic and Fe were found to be spatially correlated and both elements were strongly enriched in the fine soil particle size fractions (<2 μm and 2–50 μm). Between 14 and 82% of the total As was citrate-ascorbate extractable. Molar As/Fe ratios were as high as 0.34 in the bulk soil extracts and increased up to 0.48 in extracts of the fine particle size fractions. Arsenic K-edge XAS spectra showed the predominance of As(V) and were well fitted with a reference spectrum of As(V) adsorbed to ferrihydrite. Whereas no As(III) was detected, considerable amounts of As(-I) were present and identified as arsenopyrite originating from the mining waste. Iron K-edge XAS revealed that in addition to As(V) adsorbed to ferrihydrite, X-ray amorphous As(V)-rich hydrous ferric oxides (“As-HFO”) with a reduced number of corner-sharing FeO6 octahedra relative to ferrihydrite were the dominating secondary As species in the soils. The extremely high concentrations of As in the fine particle size fractions (up to 214 g/kg) and its association with poorly crystalline Fe(III) oxyhydroxides and As-HFO phases suggest a high As mobilization potential under both oxic and anoxic conditions, as well as a high bioaccessibility of As upon ingestion, dermal contact, or inhalation by humans or animals.</description><subject>Applied sciences</subject><subject>Arsenic</subject><subject>Arsenic - analysis</subject><subject>Arsenic - chemistry</subject><subject>Arsenicals - chemistry</subject><subject>Biological and physicochemical properties of pollutants. Interaction in the soil</subject><subject>Bulgaria</subject><subject>Data collection</subject><subject>Diffraction</subject><subject>Earth sciences</subject><subject>Earth, ocean, space</subject><subject>Engineering and environment geology. Geothermics</subject><subject>Exact sciences and technology</subject><subject>Extraction processes</subject><subject>Ferric Compounds - chemistry</subject><subject>Floodplains</subject><subject>Fluorescence</subject><subject>Freshwater</subject><subject>Iron - analysis</subject><subject>Iron - chemistry</subject><subject>Iron Compounds - chemistry</subject><subject>Minerals - chemistry</subject><subject>Mining</subject><subject>Particle Size</subject><subject>Pollution</subject><subject>Pollution, environment geology</subject><subject>Rivers</subject><subject>Soil - chemistry</subject><subject>Soil and sediments pollution</subject><subject>Soil contamination</subject><subject>Soil Pollutants - analysis</subject><subject>Soil Pollutants - chemistry</subject><subject>Spatial Analysis</subject><subject>Spectrometry, X-Ray Emission</subject><subject>Sulfides - chemistry</subject><subject>X-Ray Absorption Spectroscopy</subject><subject>X-Ray Diffraction</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNpl0UuLFDEQAOAgijuuHvwDEhRBD615dLrTx2VwVmFBcBW9NenqipulO5lN0sL46804467oJXWoj0o9CHnK2RvOBH-LqWZScLa7R1ZcCVYprfh9smKMy6qTzbcT8iila8aYkEw_JCeiFloKpVbk51lM6B3Qyy2Cw0Q3Ic44UhvDTH_nwnYXXUb6FU2-wuj8d2qmsH_pOvhsZudNdsHT82hGhz5T5-naRVhmj0uOZqKf3A-MdDOFMG4nU9KXwU3pMXlgzZTwyTGeki-bd5_X76uLj-cf1mcXlam7LlfGSAs1Q2tl3QEMpmaASlstsUGm2kGMVrZDoy0H3arOQjO0qLUpEcYR5Cl5fqgbUnZ9gjIMXEHwHiH3nAvWtaqgVwe0jeFmwZT72SXAaTIew5J6XneN1lwqWeiLf-h1WKIvIxTVtqJTXbMv-PqgIIaUItp-G91s4q7nrN9frb-9WrHPjhWXoSz_Vv45UwEvj8AkMJONxoNLd06L0hxr7pyB9FdX_334CzbPrPY</recordid><startdate>20140107</startdate><enddate>20140107</enddate><creator>Mandaliev, Petar N</creator><creator>Mikutta, Christian</creator><creator>Barmettler, Kurt</creator><creator>Kotsev, Tsvetan</creator><creator>Kretzschmar, Ruben</creator><general>American Chemical Society</general><scope>IQODW</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><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>7QH</scope><scope>7TG</scope><scope>7TV</scope><scope>7UA</scope><scope>F1W</scope><scope>H97</scope><scope>KL.</scope><scope>L.G</scope><scope>OTOTI</scope></search><sort><creationdate>20140107</creationdate><title>Arsenic Species Formed from Arsenopyrite Weathering along a Contamination Gradient in Circumneutral River Floodplain Soils</title><author>Mandaliev, Petar N ; Mikutta, Christian ; Barmettler, Kurt ; Kotsev, Tsvetan ; Kretzschmar, Ruben</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a499t-aa3fc40eff349ccba40ce58f83e6e057b2df37b68f1c8759fc6b7e88ac6bcddc3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>Applied sciences</topic><topic>Arsenic</topic><topic>Arsenic - analysis</topic><topic>Arsenic - chemistry</topic><topic>Arsenicals - chemistry</topic><topic>Biological and physicochemical properties of pollutants. Interaction in the soil</topic><topic>Bulgaria</topic><topic>Data collection</topic><topic>Diffraction</topic><topic>Earth sciences</topic><topic>Earth, ocean, space</topic><topic>Engineering and environment geology. Geothermics</topic><topic>Exact sciences and technology</topic><topic>Extraction processes</topic><topic>Ferric Compounds - chemistry</topic><topic>Floodplains</topic><topic>Fluorescence</topic><topic>Freshwater</topic><topic>Iron - analysis</topic><topic>Iron - chemistry</topic><topic>Iron Compounds - chemistry</topic><topic>Minerals - chemistry</topic><topic>Mining</topic><topic>Particle Size</topic><topic>Pollution</topic><topic>Pollution, environment geology</topic><topic>Rivers</topic><topic>Soil - chemistry</topic><topic>Soil and sediments pollution</topic><topic>Soil contamination</topic><topic>Soil Pollutants - analysis</topic><topic>Soil Pollutants - chemistry</topic><topic>Spatial Analysis</topic><topic>Spectrometry, X-Ray Emission</topic><topic>Sulfides - chemistry</topic><topic>X-Ray Absorption Spectroscopy</topic><topic>X-Ray Diffraction</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Mandaliev, Petar N</creatorcontrib><creatorcontrib>Mikutta, Christian</creatorcontrib><creatorcontrib>Barmettler, Kurt</creatorcontrib><creatorcontrib>Kotsev, Tsvetan</creatorcontrib><creatorcontrib>Kretzschmar, Ruben</creatorcontrib><creatorcontrib>Argonne National Lab. (ANL), Argonne, IL (United States). 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Sci. Technol</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Mandaliev, Petar N</au><au>Mikutta, Christian</au><au>Barmettler, Kurt</au><au>Kotsev, Tsvetan</au><au>Kretzschmar, Ruben</au><aucorp>Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Arsenic Species Formed from Arsenopyrite Weathering along a Contamination Gradient in Circumneutral River Floodplain Soils</atitle><jtitle>Environ. Sci. Technol</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2014-01-07</date><risdate>2014</risdate><volume>48</volume><issue>1</issue><spage>208</spage><epage>217</epage><pages>208-217</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><coden>ESTHAG</coden><abstract>Arsenic is a toxic trace element, which commonly occurs as contaminant in riverine floodplains and associated wetlands affected by mining and ore processing. In this study, we investigated the solid-phase speciation of As in river floodplain soils characterized by circumneutral pH (5.7–7.1) and As concentrations of up to 40.3 g/kg caused by former mining of arsenopyrite-rich ores. Soil samples collected in the floodplain of Ogosta River (Bulgaria) were size-fractionated and subsequently analyzed using a combination of X-ray fluorescence (XRF) spectrometry, powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and selective chemical extraction of poorly crystalline mineral phases. Arsenic and Fe were found to be spatially correlated and both elements were strongly enriched in the fine soil particle size fractions (<2 μm and 2–50 μm). Between 14 and 82% of the total As was citrate-ascorbate extractable. Molar As/Fe ratios were as high as 0.34 in the bulk soil extracts and increased up to 0.48 in extracts of the fine particle size fractions. Arsenic K-edge XAS spectra showed the predominance of As(V) and were well fitted with a reference spectrum of As(V) adsorbed to ferrihydrite. Whereas no As(III) was detected, considerable amounts of As(-I) were present and identified as arsenopyrite originating from the mining waste. Iron K-edge XAS revealed that in addition to As(V) adsorbed to ferrihydrite, X-ray amorphous As(V)-rich hydrous ferric oxides (“As-HFO”) with a reduced number of corner-sharing FeO6 octahedra relative to ferrihydrite were the dominating secondary As species in the soils. The extremely high concentrations of As in the fine particle size fractions (up to 214 g/kg) and its association with poorly crystalline Fe(III) oxyhydroxides and As-HFO phases suggest a high As mobilization potential under both oxic and anoxic conditions, as well as a high bioaccessibility of As upon ingestion, dermal contact, or inhalation by humans or animals.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>24283255</pmid><doi>10.1021/es403210y</doi><tpages>10</tpages></addata></record> |
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| subjects | Applied sciences Arsenic Arsenic - analysis Arsenic - chemistry Arsenicals - chemistry Biological and physicochemical properties of pollutants. Interaction in the soil Bulgaria Data collection Diffraction Earth sciences Earth, ocean, space Engineering and environment geology. Geothermics Exact sciences and technology Extraction processes Ferric Compounds - chemistry Floodplains Fluorescence Freshwater Iron - analysis Iron - chemistry Iron Compounds - chemistry Minerals - chemistry Mining Particle Size Pollution Pollution, environment geology Rivers Soil - chemistry Soil and sediments pollution Soil contamination Soil Pollutants - analysis Soil Pollutants - chemistry Spatial Analysis Spectrometry, X-Ray Emission Sulfides - chemistry X-Ray Absorption Spectroscopy X-Ray Diffraction |
| title | Arsenic Species Formed from Arsenopyrite Weathering along a Contamination Gradient in Circumneutral River Floodplain Soils |
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