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Mechanisms of Arsenic Sequestration by Prosopis juliflora during the Phytostabilization of Metalliferous Mine Tailings.

ABSTRACT: Phytostabilization is a cost-effective long-term bioremediation technique for the immobilization of metalliferous mine tailings. However, the biogeochemical processes affecting metal(loid) molecular stabilization and mobility in the root zone remain poorly resolved. The roots of Prosopis juliflora grown for up to 36 months in compost-amended pyritic mine tailings from a federal Superfund site were investigated by microscale and bulk synchrotron X-ray absorption spectroscopy (XAS) and multiple energy micro-X-ray fluorescence imaging to determine iron, arsenic, and sulfur speciation, abundance, and spatial distribution. Whereas ferrihydrite-bound As(V) species predominated in the initial bulk mine tailings, the rhizosphere speciation of arsenic was distinctly different. Root-associated As(V) was immobilized on the root epidermis bound to ferric sulfate precipitates and within root vacuoles as trivalent As(III)-(SR)3 tris-thiolate complexes. Molar Fe-to-As ratios of root epidermis tissue were two times higher than the 15% compost-amended bulk tailings growth medium. Rhizoplane-associated ferric sulfate phases that showed a high capacity to scavenge As(V) were dissimilar from the bulk-tailings mineralogy as shown by XAS and X-ray diffraction, indicating a root-surface mechanism for their formation or accumulation.

SUBMITTER: Hammond CM

PROVIDER: S-EPMC5930015 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature

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Mechanisms of Arsenic Sequestration by Prosopis juliflora during the Phytostabilization of Metalliferous Mine Tailings.

Hammond Corin M CM Root Robert A RA Maier Raina M RM Chorover Jon J

Environmental science & technology 20180122 3

Phytostabilization is a cost-effective long-term bioremediation technique for the immobilization of metalliferous mine tailings. However, the biogeochemical processes affecting metal(loid) molecular stabilization and mobility in the root zone remain poorly resolved. The roots of Prosopis juliflora grown for up to 36 months in compost-amended pyritic mine tailings from a federal Superfund site were investigated by microscale and bulk synchrotron X-ray absorption spectroscopy (XAS) and multiple en ...[more]

PMID: 29241010

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Project description:Particulate and dissolved metal(loid) release from mine tailings is of concern in (semi-) arid environments where tailings can remain barren of vegetation for decades and, therefore, become highly susceptible to dispersion by wind and water. Erosive weathering of metalliferous tailings can lead to arsenic contamination of adjacent ecosystems and increased risk to public health. Management via phytostabilization with the establishment of a vegetative cap using organic amendments to enhance plant growth has been employed to reduce both physical erosion and leaching. However, prior research suggests that addition of organic matter into the oxic weathering zone of sulfide tailings has the potential to promote the mobilization of arsenate. Therefore, the objective of the current work was to assess the impacts of phytostabilization on the molecular-scale mechanisms controlling arsenic speciation and lability. These impacts, which remain poorly understood, limit our ability to mitigate environmental and human health risks. Here we report on subsurface biogeochemical transformations of arsenic and iron from a three-year phytostabilization field study conducted at a Superfund site in Arizona, USA. Legacy pyritic tailings at this site contain up to 3 g kg-1 arsenic originating from arsenopyrite that has undergone oxidation to form arsenate-ferrihydrite complexes in the top 1 m. Tailings were amended in the top 20 cm with 100, 150, or 200 g kg-1 (300-600 T ha-1) of composted organic matter and seeded with native halotolerant plant species. Treatments and an unamended control received irrigation of 360 ± 30 mm y-1 in addition to 250 ± 160 mm y-1 of precipitation. Cores to 1 m depth were collected annually for three years and sectioned into 20 cm increments for analysis by synchrotron iron and arsenic X-ray absorption spectroscopy (XAS) coupled with quantitative wet chemical and mass balance methods. Results revealed that > 80% of arsenic exists in ammonium oxalate-extractable and non-extractable phases, including dominantly ferrihydrite and jarosite. Arsenic release during arsenopyrite oxidation resulted in both downward translocation and As(V) attenuation by stable Fe(III)(oxyhydr)oxide and Fe(III) (hydroxy)sulfate minerals over time, highlighting the need for sampling at multiple depths and time points for accurate interpretation of arsenic speciation, lability, and translocation in weathering profiles. Less than 1% of total arsenic was highly-labile, i.e. water-extractable, from all treatments, depths, and years, and more than 99% of arsenate released by arsenopyrite weathering was attenuated by association with secondary minerals. Although downward translocation of both arsenic and iron was detected during phytostabilization by temporal enrichment analysis, a similar trend was measured for the uncomposted control, indicating that organic amendment associated with phytostabilization practices did not significantly increase arsenic mobilization over non-amended controls.

Project description:Phytostabilized highly acidic, pyritic mine tailings are susceptible to re-acidification over time despite initial addition of neutralizing amendments. Studies examining plant-associated microbial dynamics during re-acidification of phytostabilized regions are sparse. To address this, we characterized the rhizosphere and bulk bacterial communities of buffalo grass used in the phytostabilization of metalliferous, pyritic mine tailings undergoing re-acidification at the Iron King Mine and Humboldt Smelter Superfund Site in Dewey-Humboldt, AZ. Plant-associated substrates representing a broad pH range (2.35-7.76) were sampled to (1) compare the microbial diversity and community composition of rhizosphere and bulk compartments across a pH gradient, and (2) characterize how re-acidification affects the abundance and activity of the most abundant plant growth-promoting bacteria (PGPB; including N2-fixing) versus acid-generating bacteria (AGB; including Fe-cycling/S-oxidizing). Results indicated that a shift in microbial diversity and community composition occurred at around pH 4. At higher pH (>4) the species richness and community composition of the rhizosphere and bulk compartments were similar, and PGPB, such as Pseudomonas, Arthrobacter, Devosia, Phyllobacterium, Sinorhizobium, and Hyphomicrobium, were present and active in both compartments with minimal presence of AGB. In comparison, at lower pH (<4) the rhizosphere had a significantly higher number of species than the bulk (p < 0.05) and the compartments had significantly different community composition (unweighted UniFrac; PERMANOVA, p < 0.05). Whereas some PGPB persisted in the rhizosphere at lower pH, including Arthrobacter and Devosia, they were absent from the bulk. Meanwhile, AGB dominated in both compartments; the most abundant were the Fe-oxidizer Leptospirillum and Fe-reducers Acidibacter and Acidiphilium, and the most active was the Fe-reducer Aciditerrimonas. This predominance of AGB at lower pH, and even their minimal presence at higher pH, contributes to acidifying conditions and poses a significant threat to sustainable plant establishment. These findings have implications for phytostabilization field site management and suggest re-application of compost or an alternate buffering material may be required in regions susceptible to re-acidification to maintain a beneficial bacterial community conducive to long-term plant establishment.

Project description:Understanding the temporal effects of organic matter input and water influx on metal lability and translocation is critical to evaluate the success of the phytostabilization of metalliferous mine tailings. Trends of metal lability, e.g., V, Cr, Mn, Co, Ni, Cu, Zn, and Pb, were investigated for three years following a direct-planting phytostabilization trial at a Superfund mine tailings site in semi-arid central Arizona, USA. Unamended tailings were characterized by high concentrations (mmol kg-1) of Fe (2100), S (3100), As (41), Zn (39), and Pb (11), where As and Pb greatly exceeded non-residential soil remediation levels established by Arizona. Phytostabilization treatments included a no-compost control, 100 g kg-1 compost with seed, and 200 g kg-1 compost with and without seed to the top 20 cm of the tailings profile. All plots received supplemental irrigation, effectively doubling the mean annual precipitation. Tailings cores up to 90 cm were Collected at the time of planting and every summer for 3 years. The cores were sub-sectioned at 20 cm increments and analyzed via total digestion and an operationally defined sequential extraction for elemental analysis and the calculation of a mass transfer coefficient normalized to Ti as an assigned immobile element. The results indicate that Pb was recalcitrant and relatively immobile in the tailings environment for both the uncomposted control and composted treatments with a maximum variation in the total concentration of 9-14 mmol kg-1 among all samples. Metal lability and translocation above the redox boundary (ca. 30 cm depth) was governed by acid generation, where surficial pH was measured as low as 2.7 ± 0.1 in year three and strongly correlated with the increased lability of Mn, Co, Ni, Cu, and Zn. There was no significant pH effect on the lability of V, Cr, or Pb. Translocation to depths was greatest for Mn and Co; however, Zn, Ni, Cr, and Cu were also mobilized. The addition of organic matter enhanced the mobilization of Cr from the near surface to 40-60 cm depth (pH > 6) over the three-year phytostabilization study compared to the control. The increased enrichment of some metals at 60-90 cm indicates that the long-term monitoring of elemental translocation is necessary to assess the efficacy of phytostabilization to contain subsurface metal contaminants and thereby protect the surrounding community from exposure.

Project description:Compost-assisted phytostabilization has recently emerged as a robust alternative for reclamation of metalliferous mine tailings. Previous studies suggest that root-associated microbes may be important for facilitating plant establishment on the tailings, yet little is known about the long-term dynamics of microbial communities during reclamation. A mechanistic understanding of microbial community dynamics in tailings ecosystems undergoing remediation is critical because these dynamics profoundly influence both the biogeochemical weathering of tailings and the sustainability of a plant cover. Here we monitor the dynamics of soil microbial communities (i.e. bacteria, fungi, archaea) during a 12-month mesocosm study that included 4 treatments: 2 unplanted controls (unamended and compost-amended tailings) and 2 compost-amended seeded tailings treatments. Bacterial, fungal and archaeal communities responded distinctively to the revegetation process and concurrent changes in environmental conditions and pore water chemistry. Compost addition significantly increased microbial diversity and had an immediate and relatively long-lasting buffering-effect on pH, allowing plants to germinate and thrive during the early stages of the experiment. However, the compost buffering capacity diminished after six months and acidification took over as the major factor affecting plant survival and microbial community structure. Immediate changes in bacterial communities were observed following plant establishment, whereas fungal communities showed a delayed response that apparently correlated with the pH decline. Fluctuations in cobalt pore water concentrations, in particular, had a significant effect on the structure of all three microbial groups, which may be linked to the role of cobalt in metal detoxification pathways. The present study represents, to our knowledge, the first documentation of the dynamics of the three major microbial groups during revegetation of compost-amended, metalliferous mine tailings.

Dataset Information

Mechanisms of Arsenic Sequestration by Prosopis juliflora during the Phytostabilization of Metalliferous Mine Tailings.

Publications

Mechanisms of Arsenic Sequestration by Prosopis juliflora during the Phytostabilization of Metalliferous Mine Tailings.

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