“…Furthermore, Pb isotopes have been used for tracing the transport and redistribution of Pb in the atmosphere (Desenfant et al, 2006;Hamelin et al, 1997;Shotyk et al, 2002;Véron et al, 1999;Weiss et al, 2002). More recently, Cu and Zn isotopes were used to link increased metal concentrations in soils or sediments to the emissions of metallurgic plants (Araújo et al, 2018;Bigalke et al, 2010a;Juillot et al, 2011;Kříbek et al, 2018;Mihaljevič et al, 2018;Sivry et al, 2008;Sonke et al, 2008;Thapalia et al, 2010), or for sourcing metal particles from mining and tailing sites (Borrok et al, 2009;Kimball et al, 2009;Song et al, 2016;Viers et al, 2018).…”
Sourcing and understanding the fate of anthropogenic metals in a historical contamination context is challenging. Here we combined elemental and isotopic (Pb, Zn, Cu) analyses with X-ray absorption spectroscopy (XAS) measurements (Zn) to trace the fate, in undisturbed soil profiles, of historical metal contamination emitted by a 167-year-old Pb-Ag smelter decommissioned 100 years ago located in the Calanques National Park (Marseilles, France). Lead isotopic measurements show that entire soil profiles were affected by 74 years of Pb emissions up to ~7 km from the smelter under the main NNW wind, and indicate particulate transfer down to 0.8 m at depth. This vertical mobility of anthropogenic Pb contrasts with previous studies where Pb was immobilized in surface horizons. The contribution of anthropogenic Pb to the total Pb concentration in soils was estimated at 95% in surface horizons, and 78% in the deepest horizons. Zinc isotopic signatures of past emissions, that are enriched in light isotopes compared to the natural geological background (-0.69 ±0.03‰ and-0.15 ±0.02‰, respectively), were detected only in the surface horizons of the studied soils. Using XAS analyses, we showed that anthropogenic Zn was transformed and immobilized in surface horizons as Zn-Layered Double Hydroxide, thus favoring the enrichment in heavy isotopes in these surface horizons. No clear evidence of copper contamination by the smelter was found and Cu isotopes point to a bedrock origin and a natural distribution of Cu concentrations. Highlights: • δPb, Zn, Cu in soils impacted by emissions 100 y ago from a smelter • Pb contamination was detected 7 km away from the smelter and down the soil profiles • Light δ 66 Zn values were measured in the chimney and in soil surface horizons • Precipitation of Zn-Layered Double Hydroxide prevented downwards migration of anthropogenic Zn • Cu isotopes indicate its geogenic origin and redistribution in soils by pedogenesis
“…Furthermore, Pb isotopes have been used for tracing the transport and redistribution of Pb in the atmosphere (Desenfant et al, 2006;Hamelin et al, 1997;Shotyk et al, 2002;Véron et al, 1999;Weiss et al, 2002). More recently, Cu and Zn isotopes were used to link increased metal concentrations in soils or sediments to the emissions of metallurgic plants (Araújo et al, 2018;Bigalke et al, 2010a;Juillot et al, 2011;Kříbek et al, 2018;Mihaljevič et al, 2018;Sivry et al, 2008;Sonke et al, 2008;Thapalia et al, 2010), or for sourcing metal particles from mining and tailing sites (Borrok et al, 2009;Kimball et al, 2009;Song et al, 2016;Viers et al, 2018).…”
Sourcing and understanding the fate of anthropogenic metals in a historical contamination context is challenging. Here we combined elemental and isotopic (Pb, Zn, Cu) analyses with X-ray absorption spectroscopy (XAS) measurements (Zn) to trace the fate, in undisturbed soil profiles, of historical metal contamination emitted by a 167-year-old Pb-Ag smelter decommissioned 100 years ago located in the Calanques National Park (Marseilles, France). Lead isotopic measurements show that entire soil profiles were affected by 74 years of Pb emissions up to ~7 km from the smelter under the main NNW wind, and indicate particulate transfer down to 0.8 m at depth. This vertical mobility of anthropogenic Pb contrasts with previous studies where Pb was immobilized in surface horizons. The contribution of anthropogenic Pb to the total Pb concentration in soils was estimated at 95% in surface horizons, and 78% in the deepest horizons. Zinc isotopic signatures of past emissions, that are enriched in light isotopes compared to the natural geological background (-0.69 ±0.03‰ and-0.15 ±0.02‰, respectively), were detected only in the surface horizons of the studied soils. Using XAS analyses, we showed that anthropogenic Zn was transformed and immobilized in surface horizons as Zn-Layered Double Hydroxide, thus favoring the enrichment in heavy isotopes in these surface horizons. No clear evidence of copper contamination by the smelter was found and Cu isotopes point to a bedrock origin and a natural distribution of Cu concentrations. Highlights: • δPb, Zn, Cu in soils impacted by emissions 100 y ago from a smelter • Pb contamination was detected 7 km away from the smelter and down the soil profiles • Light δ 66 Zn values were measured in the chimney and in soil surface horizons • Precipitation of Zn-Layered Double Hydroxide prevented downwards migration of anthropogenic Zn • Cu isotopes indicate its geogenic origin and redistribution in soils by pedogenesis
and copper wire, were dissolved in 1000 ml Teflon® bottles, to result in 200 µg ml -1 stock solutions (hereafter referred to as NWU-Cu-A and NWU-Cu-B), and cryogenically stored. The Cu isotopic compositions of the two samples were determined in three different laboratories using multi-collector inductively coupled plasma-mass spectrometry, and the Cu isotopic compositions obtained from the standard-sample bracketing method were consistent within the two standard deviation (2s) range. The Cu isotopic compositions of the NWU-Cu-A and NWU-Cu-B standard solutions were δ 65 Cu = +0.91 ± 0.03‰ (2s, n = 42) and δ 65 Cu = -0.05 ± 0.03‰ (2s, n = 49), respectively, relative to the reference material NIST NBS 976.
“…Large variation of δ 65 Cu (−16.49 to +20.04‰) was observed in ores and minerals [6,59,69,70], averaging +0.11‰, as summarized in Figure 2. Hypogene minerals (e.g., chalcopyrite, chalcocite, covellite, and pyrite enargite) usually had a narrow δ 65 Cu variation around zero, whereas leached (e.g., hematite, jarosite, and goethite) was isotopically lighter and supergene minerals (e.g., chalcocite, hematite, and Cu oxide) isotopically heavier [57,68,71,72,73,74]. Narrow variations of Cu isotopic composition in silicate reservoirs (e.g., basalts, granites) were reported recently [75,76].…”
Section: Cu Isotope Compositions In Earth Surface Reservoirsmentioning
confidence: 99%
“…Sulfide-bearing tailing profiles showed that light Cu isotope was enriched in the oxidized zone than in the original materials [84]. Song et al [73] observed a large δ 65 Cu variation (−0.44‰ to +24.4‰) in stream water (impacted by mining activities at the Dexing Mine, the largest Cu mine in Asia), which could be stemmed from pyrite tailings and chalcopyrite weathering. Both results were consistent with the leaching experiments that heavy Cu was preferentially enriched in solutions [42,44,45,48].…”
Section: Cu Isotope Compositions In Earth Surface Reservoirsmentioning
confidence: 99%
“…The δ 65 Cu (‰) values of various natural materials [6,7,15,19,20,21,26,32,40,59,61,63,64,65,66,68,70,72,73,76,80,81,82,83,84,85,86,87,88,89,90,91,92,93]. …”
Copper (Cu) is a transition metal and an essential micronutrient for organisms, but also one of the most widespread toxic inorganic contaminants at very high content. The research on Cu isotopes has grown rapidly in the last decade. Hitherto, a large number of studies have been published on the theoretical fractionation mechanisms, experimental data and natural variations of Cu isotopes in variable environments and ecosystems. These studies reported a large variation of δ65Cu (−16.49 to +20.04‰) in terrestrial samples and showed that Cu isotopes could be fractionated by various biogeochemical processes to different extent. Several papers have previously reviewed the coupling of Cu and Zn isotope systematics, and we give here a tentative review of the recent publications only on Cu isotopesin variable surface repositories, animals and human beings, with a goal to attract much attention to research on Cu (and other metals) behaviors in the environment and biological systems.
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