Evidences of arsenic (III) precipitation on iron (III) oxy-hydroxides from the combination of Raman spectroscopy, density functional theory calculations, and extended X-ray absorption fine structure spectroscopy

G. Duarte, V. Ciminelli, M. S.S. Dantas, I. F. Vasconcelos, Kwadwo Asare Osseo-Asare, J. D. Kubicki, H. Watts

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Abstract

Arsenite (As III) precipitation in iron (Fe III) systems was firstly suggested from the shape patterns of the isotherms obtained for As(III) immobilized on hematite and goethite at pH 7.0. Hence, Raman and EXAFS analyses were combined with Density Functional Theory (DFT) to investigate the mechanism of As(III) immobilization on Fe(III) oxy-hydroxides. XANES analyses confirmed As(III) as the sorbed species. The results from DFT calculations indicated a stable structure for As(III) precipitated on hematite with the following calculated interactions: As = O (1.70 å); As-O (1.78 å); As-As (3.30 å), and As-Fe (3.50 å). These distances were in agreement with EXAFS analyses of As(III) sorbed on hematite (0.014 mmol/m 2) and goethite (0.010 mmol/m 2) at pH 7. The As = O bond was also consistent with the Raman vibration at 860 cm -1. Therefore, the precipitation of As(III) as a mechanism involved in As fixation by Fe(III) oxy-hydroxides is supported by spectroscopic analyses combined with theoretical calculations. This is invoked as the main finding of the present investigation and it may help the prediction and control of arsenic mobility in iron-rich soils.

Original languageEnglish (US)
Title of host publicationUnderstanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress
Subtitle of host publicationArsenic in the Environment
Pages381-383
Number of pages3
StatePublished - Aug 16 2012
Event4th International Congress on Arsenic in the Environment, As 2012 - Cairns, QLD, Australia
Duration: Jul 22 2012Jul 27 2012

Publication series

NameUnderstanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment

Other

Other4th International Congress on Arsenic in the Environment, As 2012
CountryAustralia
CityCairns, QLD
Period7/22/127/27/12

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Hydroxides
Extended X ray absorption fine structure spectroscopy
Hematite
Arsenic
Raman spectroscopy
hematite
Density functional theory
hydroxide
arsenic
Iron
spectroscopy
goethite
iron
arsenite
immobilization
fixation
Isotherms
vibration
isotherm
Soils

All Science Journal Classification (ASJC) codes

  • Environmental Chemistry
  • Pollution

Cite this

Duarte, G., Ciminelli, V., Dantas, M. S. S., Vasconcelos, I. F., Osseo-Asare, K. A., Kubicki, J. D., & Watts, H. (2012). Evidences of arsenic (III) precipitation on iron (III) oxy-hydroxides from the combination of Raman spectroscopy, density functional theory calculations, and extended X-ray absorption fine structure spectroscopy. In Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment (pp. 381-383). (Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment).
Duarte, G. ; Ciminelli, V. ; Dantas, M. S.S. ; Vasconcelos, I. F. ; Osseo-Asare, Kwadwo Asare ; Kubicki, J. D. ; Watts, H. / Evidences of arsenic (III) precipitation on iron (III) oxy-hydroxides from the combination of Raman spectroscopy, density functional theory calculations, and extended X-ray absorption fine structure spectroscopy. Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment. 2012. pp. 381-383 (Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment).
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abstract = "Arsenite (As III) precipitation in iron (Fe III) systems was firstly suggested from the shape patterns of the isotherms obtained for As(III) immobilized on hematite and goethite at pH 7.0. Hence, Raman and EXAFS analyses were combined with Density Functional Theory (DFT) to investigate the mechanism of As(III) immobilization on Fe(III) oxy-hydroxides. XANES analyses confirmed As(III) as the sorbed species. The results from DFT calculations indicated a stable structure for As(III) precipitated on hematite with the following calculated interactions: As = O (1.70 {\aa}); As-O (1.78 {\aa}); As-As (3.30 {\aa}), and As-Fe (3.50 {\aa}). These distances were in agreement with EXAFS analyses of As(III) sorbed on hematite (0.014 mmol/m 2) and goethite (0.010 mmol/m 2) at pH 7. The As = O bond was also consistent with the Raman vibration at 860 cm -1. Therefore, the precipitation of As(III) as a mechanism involved in As fixation by Fe(III) oxy-hydroxides is supported by spectroscopic analyses combined with theoretical calculations. This is invoked as the main finding of the present investigation and it may help the prediction and control of arsenic mobility in iron-rich soils.",
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Duarte, G, Ciminelli, V, Dantas, MSS, Vasconcelos, IF, Osseo-Asare, KA, Kubicki, JD & Watts, H 2012, Evidences of arsenic (III) precipitation on iron (III) oxy-hydroxides from the combination of Raman spectroscopy, density functional theory calculations, and extended X-ray absorption fine structure spectroscopy. in Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment. Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment, pp. 381-383, 4th International Congress on Arsenic in the Environment, As 2012, Cairns, QLD, Australia, 7/22/12.

Evidences of arsenic (III) precipitation on iron (III) oxy-hydroxides from the combination of Raman spectroscopy, density functional theory calculations, and extended X-ray absorption fine structure spectroscopy. / Duarte, G.; Ciminelli, V.; Dantas, M. S.S.; Vasconcelos, I. F.; Osseo-Asare, Kwadwo Asare; Kubicki, J. D.; Watts, H.

Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment. 2012. p. 381-383 (Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment).

Research output: Chapter in Book/Report/Conference proceedingConference contribution

TY - GEN

T1 - Evidences of arsenic (III) precipitation on iron (III) oxy-hydroxides from the combination of Raman spectroscopy, density functional theory calculations, and extended X-ray absorption fine structure spectroscopy

AU - Duarte, G.

AU - Ciminelli, V.

AU - Dantas, M. S.S.

AU - Vasconcelos, I. F.

AU - Osseo-Asare, Kwadwo Asare

AU - Kubicki, J. D.

AU - Watts, H.

PY - 2012/8/16

Y1 - 2012/8/16

N2 - Arsenite (As III) precipitation in iron (Fe III) systems was firstly suggested from the shape patterns of the isotherms obtained for As(III) immobilized on hematite and goethite at pH 7.0. Hence, Raman and EXAFS analyses were combined with Density Functional Theory (DFT) to investigate the mechanism of As(III) immobilization on Fe(III) oxy-hydroxides. XANES analyses confirmed As(III) as the sorbed species. The results from DFT calculations indicated a stable structure for As(III) precipitated on hematite with the following calculated interactions: As = O (1.70 å); As-O (1.78 å); As-As (3.30 å), and As-Fe (3.50 å). These distances were in agreement with EXAFS analyses of As(III) sorbed on hematite (0.014 mmol/m 2) and goethite (0.010 mmol/m 2) at pH 7. The As = O bond was also consistent with the Raman vibration at 860 cm -1. Therefore, the precipitation of As(III) as a mechanism involved in As fixation by Fe(III) oxy-hydroxides is supported by spectroscopic analyses combined with theoretical calculations. This is invoked as the main finding of the present investigation and it may help the prediction and control of arsenic mobility in iron-rich soils.

AB - Arsenite (As III) precipitation in iron (Fe III) systems was firstly suggested from the shape patterns of the isotherms obtained for As(III) immobilized on hematite and goethite at pH 7.0. Hence, Raman and EXAFS analyses were combined with Density Functional Theory (DFT) to investigate the mechanism of As(III) immobilization on Fe(III) oxy-hydroxides. XANES analyses confirmed As(III) as the sorbed species. The results from DFT calculations indicated a stable structure for As(III) precipitated on hematite with the following calculated interactions: As = O (1.70 å); As-O (1.78 å); As-As (3.30 å), and As-Fe (3.50 å). These distances were in agreement with EXAFS analyses of As(III) sorbed on hematite (0.014 mmol/m 2) and goethite (0.010 mmol/m 2) at pH 7. The As = O bond was also consistent with the Raman vibration at 860 cm -1. Therefore, the precipitation of As(III) as a mechanism involved in As fixation by Fe(III) oxy-hydroxides is supported by spectroscopic analyses combined with theoretical calculations. This is invoked as the main finding of the present investigation and it may help the prediction and control of arsenic mobility in iron-rich soils.

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M3 - Conference contribution

AN - SCOPUS:84864885489

SN - 9780415637633

T3 - Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment

SP - 381

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BT - Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress

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Duarte G, Ciminelli V, Dantas MSS, Vasconcelos IF, Osseo-Asare KA, Kubicki JD et al. Evidences of arsenic (III) precipitation on iron (III) oxy-hydroxides from the combination of Raman spectroscopy, density functional theory calculations, and extended X-ray absorption fine structure spectroscopy. In Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment. 2012. p. 381-383. (Understanding the Geological and Medical Interface of Arsenic, As 2012 - 4th International Congress: Arsenic in the Environment).