Arsenic uptake by natural calcite: An XAS study

Bardelli, Fabrizio; Benvenuti, Marco; Costagliola, Pilario; Benedetto, Francesco Di; Lattanzi, Pierfranco; Meneghini, Carlo; Romanelli, Marco; Valenzano, Loredana

doi:10.1016/j.gca.2011.03.003

Cited by 69 publications

(38 citation statements)

References 59 publications

(85 reference statements)

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“…A better fit was obtained with a distance of 2.85 Å for the 5-3 µm fraction and 2.86 Å for the 3-0.2 µm fraction. The presence of other light atoms was also considered but finally ruled out because they would result in longer interatomic distances for Ca and Al (Arai et al, 2001;Bardelli et al, 2011) or a shorter interatomic distance for S (Hoffmann et al, 2014).…”

Section: Speciation Of Arsenic By X-ray Absorption Spectroscopymentioning

confidence: 99%

Highlighting the wide variability in arsenic speciation in wetlands: A new insight into the control of the behavior of arsenic

Guénet

Davranche

Vantelon

et al. 2017

Geochimica et Cosmochimica Acta

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Highlighting the wide variability in arsenic speciation in wetlands: a new insight into the control of the behavior of arsenic. Geochimica et Cosmochimica Acta, Elsevier, 2017, 203, pp.284-302 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. 1Highlighting the wide variability in arsenic speciation in wetlands: AbstractAlthough the behavior of Arsenic (As) under reducing conditions in periods of high water levels in wetlands is well understood and documented, there is a lack of information under oxidizing conditions when the water level decreases. In this study, we were interested in the first stage of the oxidizing period, when oxidation products are still in suspension. A soil sample from the Naizin Kervidy wetland (France) was incubated in the laboratory to produce a reduced soil solution. The reduced solution was subsequently oxidized, filtered and ultrafiltered using decreasing pore size membranes (5 µm, 3 µm, 0.2 µm, 30 kDa and 5 kDa). The distribution of As and Fe was investigated in each size fraction of the oxidized solution and their speciations were studied using XAS, HPLC and SEC-ICP-MS. Organic matter was characterized using thermally assisted hydrolysis and methylation gas chromatography-mass spectrometry (THM-GC-MS) and fluorescence spectroscopy. The majority of the As was present as As(V) but a small amount of As(III) still remained despite the advanced oxidized conditions. In the > 0.2 µm fractions, the XAS analyses showed that As was associated, in the second shell, with Fe (As-Fe = 3.35 Å) as bidentate binuclear complexes and C (As-C = 2.90 Å), suggesting the integration of As in biological objects. In the < 30 kDa fraction, As was directly bound to C (As-C = 1.96 Å) in the first shell indicating the presence of organic As species. In the second shell, an As-Fe distance of 3.35 Å was found showing that 2 part of the As was still complexed with Fe. The 0.2 µm-30 kDa fraction was a transitional fraction in terms of the Fe species and OM composition. In this fraction, organic matter exhibited a more humic character (aromatic molecules) inducing an increasing cation binding capacity. As a consequence, in this fraction and in the smallest one, As, Fe and OM seemed to form ternary complexes in which the Fe or nano-oxides in the > 30 kDa fraction and as monomer, or cluster in < 30 kDa fraction acted as a bridge. In all of the fractions, a proportion of As(V) was present as organic methylated species. These organic species might be produced by several organisms (animal or plant) via a detoxification process. They seemed to be bound to the particulate and colloidal Fe/OM phases as well as integ...

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Section: Speciation Of Arsenic By X-ray Absorption Spectroscopymentioning

confidence: 99%

Highlighting the wide variability in arsenic speciation in wetlands: A new insight into the control of the behavior of arsenic

Guénet

Davranche

Vantelon

et al. 2017

Geochimica et Cosmochimica Acta

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“…Fossil travertines were sampled at the Bullicame area (samples BL4, BL5, BL7) and in the Pecora Valley district (Southern Tuscany, Italy; cfr. Costagliola et al, 2010Costagliola et al, , 2013Bardelli et al, 2011;sample TRSE). Presently forming travertines were all sampled at Bullicame Hot Springs (samples BL1, BL2, BL3) and Zitelle Hot Spring (ZIT).…”

Section: Reference Materials Collection Production and Analysismentioning

confidence: 99%

“…The enhanced stability is speculated to result from the incorporation and ordering of As in the calcite lattice, following the substitution of the As oxyanion for CO 3 2À in the crystal lattice (Di Benedetto et al, 2006). This substitution leads to a partial distortion of the calcite lattice, usually an expansion of the unit cell along the c axis, due to the size difference between the two anions (Cheng et al, 1999;Román-Ross et al, 2006;Bardelli et al, 2011).…”

Section: Introductionmentioning

confidence: 99%

“…Natural calcite also generally contains more As(V) compared to As(III), consistent with these laboratory results Costagliola et al, 2013;Winkel et al, 2013), but with some notable exceptions. Di Benedetto et al (2006) and Bardelli et al (2011), on the basis of Electron Paramagnetic Resonance (EPR) and X-ray Absorption Spectroscopy (XAS) measurements, found that natural calcite from travertine deposits of Central Italy prevalently host As(V) but may indeed contain a significant fraction of As(III). Bardelli et al (2011) speculated that bacteria could have played an important role in favouring the uptake of As(III) in the calcite lattice.…”

Section: Introductionmentioning

confidence: 99%

“…Di Benedetto et al (2006) and Bardelli et al (2011), on the basis of Electron Paramagnetic Resonance (EPR) and X-ray Absorption Spectroscopy (XAS) measurements, found that natural calcite from travertine deposits of Central Italy prevalently host As(V) but may indeed contain a significant fraction of As(III). Bardelli et al (2011) speculated that bacteria could have played an important role in favouring the uptake of As(III) in the calcite lattice. Calcium carbonate precipitation by bacteria is a widespread process, occurring in different taxonomic groups and in different environments (including lakes and hot springs) at a scale ranging from micrometer size bacterial cells to that of meters of rocks (Warren et al, 2001;Perito and Mastromei, 2011).…”

Section: Introductionmentioning

confidence: 99%

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Arsenic uptake in bacterial calcite

Catelani

Perito

Bellucci

et al. 2018

Geochimica et Cosmochimica Acta

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Bio-mediated processes for arsenic (As) uptake in calcite were investigated by means of X-ray Diffraction (XRD) and Xray Absorption Spectroscopy (XAS) coupled with X-ray Fluorescence measurements. The environmental bacterial strain Bacillus licheniformis BD5, sampled at the Bullicame Hot Springs (Viterbo, Central Italy), was used to synthesize calcite from As-enriched growth media. Both liquid and solid cultures were applied to simulate planktonic and biofilm community environments, respectively. Bacterial calcite samples cultured in liquid media had an As enrichment factor (Kd) 50 times higher than that from solid media. The XRD analysis revealed an elongation of the crystal lattice along the c axis (by 0.03 Å ) for biogenic calcite, which likely resulted from the substitution of larger arsenate for carbonate in the crystal. The XAS data also showed a clear difference in the oxidation state of sorbed As between bacterial and abiotic calcite. Abiotic chemical processes yielded predominantly As(V) uptake whereas bacterial precipitation processes led to the uptake of both As(III) and As(V). The presence of As(III) in bacterial calcite is proposed to result from subsequent reduction of arsenate to arsenite by bacterial activities. To the best of our knowledge, this is the first experimental observation of the incorporation of As(III) in the calcite crystal lattice, revealing a critical role of biochemical processes for the As cycling in nature.

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