Metal Stable Isotope Signatures as Tracers in Environmental Geochemistry

Wiederhold, Jan G.

doi:10.1021/es504683e

Cited by 384 publications

(261 citation statements)

References 295 publications

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“…Note the lack of redox speciation and organic complexation for silicon limits fractionation effects to predominately inorganic kinetic exchange factors, contrary to many other elements (Wiederhold, 2015). The following is a description of the systems, processes and transformations that control the global silica cycle, and the known constraints on the δ 30 Si (see Figure 1).…”

Section: Stable Silicon Isotope Ratios To Study the Global Si Cyclementioning

confidence: 99%

A Review of the Stable Isotope Bio-geochemistry of the Global Silicon Cycle and Its Associated Trace Elements

et al. 2018

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Section: Stable Silicon Isotope Ratios To Study the Global Si Cyclementioning

confidence: 99%

A Review of the Stable Isotope Bio-geochemistry of the Global Silicon Cycle and Its Associated Trace Elements

et al. 2018

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“…Therefore, the recently explored application of non-54 traditional stable isotopes for source identification of metal pollutants in the atmosphere is of 55 great interest as it requires smaller sets of samples. 3 …”

Section: Introduction 49mentioning

confidence: 99%

New Insights from Zinc and Copper Isotopic Compositions into the Sources of Atmospheric Particulate Matter from Two Major European Cities

Gonzalez

Strekopytov

Amato

et al. 2016

Environ. Sci. Technol.

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This study reports spatial and temporal variability of Zn and Cu isotopes in atmospheric particulate matter (PM) collected in two major European cities with contrasting atmospheric pollution, Barcelona and London. We demonstrate that nontraditional stable isotopes identify source contributions of Zn and Cu and can play a major role in future air quality studies. In Barcelona, samples of fine PM were collected at street level at sites with variable traffic density. The isotopic signatures ranged between −0.13 ± 0.09 and −0.51 ± 0.05‰ for δ 66 Zn IRMM and between +0.04 ± 0.20 and +0.33 ± 0.15‰ for δ 65 Cu AE633 .Copper isotope signatures similar to those of Cu sulfides and Cu/ Sb ratios within the range typically found in brake wear suggest that nonexhaust emissions from vehicles are dominant. Negative Zn isotopic signatures characteristic for gaseous emissions from smelting and combustion and large enrichments of Zn and Cd suggest contribution from metallurgical industries. In London, samples of coarse PM collected on the top of a building over 18 months display isotope signatures ranging between +0.03 ± 0.04 and +0.49 ± 0.02‰ for δ 66 Zn IRMM and between +0.37 ± 0.17 and +0.97 ± 0.21‰ for δ 65 Cu AE633 . Heavy Cu isotope signatures (up to +0.97 ± 0.21‰) and higher enrichments and Cu/Sb ratios during winter time indicate important contribution from fossil fuel combustion. The positive δ 66 Zn IRMM signatures are in good agreement with signatures characteristic for ore concentrates used for the production of tires and galvanized materials, suggesting nonexhaust emissions from vehicles as the main source of Zn pollution.

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“…The AgNPs were enriched in the heavy isotope and the residual Ag + was enriched in the light isotope. Assuming that the fractionation followed the Rayleigh model 19 , ε was estimated to be 0.63, 0.73 and 0.82‰ for HA concentrations of 5, 10 and 50 mg l -1 , respectively ( Supplementary Fig. 3).…”

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“…This could be explained by a photo-oxidationinduced formation of an intermediate metal oxide phase (Ag 2 O, for example) at the surface of the AgNPs 25,26 . According to equilibrium isotope fractionation rules 19 , the heavy isotope is prone to being concentrated in compounds with a higher oxidation state. As a result, the metal oxide phase should be enriched in 109 Ag, thus causing the released Ag + to be enriched in 109 Ag.…”

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Stable silver isotope fractionation in the natural transformation process of silver nanoparticles

et al. 2016

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Nanoparticles in the environment can form by natural processes or be released due to human activities 1 . Owing to limited analytical methods, the behaviour of nanoparticles in the natural environment is poorly understood and until now they have only been described by the variations in the nanoparticle size or the concentration of the element of interest. Here we show that by using inductively coupled plasma mass spectrometry to measure silver (Ag) isotope ratios it is possible to understand the transformation processes of silver nanoparticles (AgNPs) in the environment. We found that the formation and dissolution of AgNPs under natural conditions caused significant variations in the ratio of natural Ag isotopes ( 107 Ag and 109 Ag) with an isotopic enrichment factor (ε) up to 0.86‰. Furthermore, we show that engineered AgNPs have distinctly different isotope fractionation effects to their naturally formed counterparts. Further studies will be needed to understand whether isotope analysis can be used to reveal the sources of AgNPs in the environment.AgNPs are the most widely used nanomaterial due to their broad spectrum in antimicrobial activities 2 . An exponential increase in the environmental levels of AgNPs is predicted due to their rising usage and disposal levels 3,4 . As the natural abundance of Ag in the Earth's crust is extremely low (∼0.07 mg kg -1 ; ref. 5), the release of even a small mass of Ag to the environment from anthropogenic activities may lead to proportionally large deviations from natural conditions 6 . AgNPs present in the environment are normally thought to originate from human activities. However, recent studies reveal that AgNPs can also form naturally via the reduction of Ag + in natural waters mediated by dissolved organic matter (DOM) 7,8 and sunlight 9 , which implies that the level of AgNPs in the environment may be underestimated. There is evidence that AgNPs are potentially harmful for organisms and human health 1 and that AgNP loading can significantly influence important ecosystem processes 10,11 . However, little is known about the natural processes and fate of AgNPs due to the lack of proper methods to detect or trace AgNPs in environmental media.Here, we studied the variations in the stable Ag isotope ratio in the natural transformation process of AgNPs. Ag isotopes have previously been applied as chronometers for early-stage planetary differentiation 12,13 and as tracers in archaeometry 14,15 , whereas other applications are rare in the literature. Naturally occurring Ag is composed of 107 Ag and 109 Ag with approximately equal natural abundances (51.8% versus 48.2%) and subtle variations in 107 Ag/ 109 Ag ratio were observed in various terrestrial samples 16,17 . We hypothesized that variations in the natural stable isotope ratio may provide a new means to study the environmental processes of NPs. To test this hypothesis, we studied two reversible processes of AgNPs in natural waters (Fig. 1): the formation of AgNPs via the reduction of Ag + in the presence of DOM and the...

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Metal Stable Isotope Signatures as Tracers in Environmental Geochemistry

Cited by 384 publications

References 295 publications

A Review of the Stable Isotope Bio-geochemistry of the Global Silicon Cycle and Its Associated Trace Elements

A Review of the Stable Isotope Bio-geochemistry of the Global Silicon Cycle and Its Associated Trace Elements

New Insights from Zinc and Copper Isotopic Compositions into the Sources of Atmospheric Particulate Matter from Two Major European Cities

Stable silver isotope fractionation in the natural transformation process of silver nanoparticles

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