Advanced

Electronic structure calculations of mercury mobilization from mineral phases and photocatalytic removal from water and the atmosphere

Da Pieve, Fabiana; Stankovski, Martin LU and Hogan, Conor (2014) In Science of the Total Environment 493. p.596-605
Abstract
Mercury is a hazardous environmental pollutant mobilized from natural sources, and anthropogenically contaminated and disturbed areas. Current methods to assess mobility and environmental impact are mainly based on field measurements, soil monitoring, and kinetic modelling. In order to understand in detail the extent to which different mineral sources can give rise to mercury release it is necessary to investigate the complexity at the microscopic level and the possible degradation/dissolution processes. In this work, we investigated the potential for mobilization of mercury structurally trapped in three relevant minerals occurring in hot spring environments and mining areas, namely, cinnabar (alpha-HgS), corderoite (alpha-Hg3S2Cl2), and... (More)
Mercury is a hazardous environmental pollutant mobilized from natural sources, and anthropogenically contaminated and disturbed areas. Current methods to assess mobility and environmental impact are mainly based on field measurements, soil monitoring, and kinetic modelling. In order to understand in detail the extent to which different mineral sources can give rise to mercury release it is necessary to investigate the complexity at the microscopic level and the possible degradation/dissolution processes. In this work, we investigated the potential for mobilization of mercury structurally trapped in three relevant minerals occurring in hot spring environments and mining areas, namely, cinnabar (alpha-HgS), corderoite (alpha-Hg3S2Cl2), and mercuric chloride (HgCl2). Quantum chemical methods based on density functional theory as well as more sophisticated approaches are used to assess the possibility of a) direct photoreduction and formation of elemental Hg at the surface of the minerals, providing a path for ready release in the environment; and b) reductive dissolution of the minerals in the presence of solutions containing halogens. Furthermore, we study the use of TiO2 as a potential photocatalyst for decontamination of polluted waters (mainly Hg2+-containing species) and air (atmospheric Hg-0). Our results partially explain the observed pathways of Hg mobilization from relevant minerals and the microscopic mechanisms behind photocatalytic removal of Hg-based pollutants. Possible sources of disagreement with observations are discussed and further improvements to our approach are suggested. (C) 2014 Elsevier B.V. All rights reserved. (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Heavy metal pollution, Mineral sources, Dissolution, Quantum-chemistry, modelling, Photocatalysis
in
Science of the Total Environment
volume
493
pages
596 - 605
publisher
Elsevier
external identifiers
  • wos:000340312000064
  • scopus:84903471110
ISSN
1879-1026
DOI
10.1016/j.scitotenv.2014.06.012
language
English
LU publication?
yes
id
db8524fb-597a-4c16-8e8f-1e8b3fbb8130 (old id 4656188)
date added to LUP
2014-09-25 15:32:45
date last changed
2017-01-01 04:13:24
@article{db8524fb-597a-4c16-8e8f-1e8b3fbb8130,
  abstract     = {Mercury is a hazardous environmental pollutant mobilized from natural sources, and anthropogenically contaminated and disturbed areas. Current methods to assess mobility and environmental impact are mainly based on field measurements, soil monitoring, and kinetic modelling. In order to understand in detail the extent to which different mineral sources can give rise to mercury release it is necessary to investigate the complexity at the microscopic level and the possible degradation/dissolution processes. In this work, we investigated the potential for mobilization of mercury structurally trapped in three relevant minerals occurring in hot spring environments and mining areas, namely, cinnabar (alpha-HgS), corderoite (alpha-Hg3S2Cl2), and mercuric chloride (HgCl2). Quantum chemical methods based on density functional theory as well as more sophisticated approaches are used to assess the possibility of a) direct photoreduction and formation of elemental Hg at the surface of the minerals, providing a path for ready release in the environment; and b) reductive dissolution of the minerals in the presence of solutions containing halogens. Furthermore, we study the use of TiO2 as a potential photocatalyst for decontamination of polluted waters (mainly Hg2+-containing species) and air (atmospheric Hg-0). Our results partially explain the observed pathways of Hg mobilization from relevant minerals and the microscopic mechanisms behind photocatalytic removal of Hg-based pollutants. Possible sources of disagreement with observations are discussed and further improvements to our approach are suggested. (C) 2014 Elsevier B.V. All rights reserved.},
  author       = {Da Pieve, Fabiana and Stankovski, Martin and Hogan, Conor},
  issn         = {1879-1026},
  keyword      = {Heavy metal pollution,Mineral sources,Dissolution,Quantum-chemistry,modelling,Photocatalysis},
  language     = {eng},
  pages        = {596--605},
  publisher    = {Elsevier},
  series       = {Science of the Total Environment},
  title        = {Electronic structure calculations of mercury mobilization from mineral phases and photocatalytic removal from water and the atmosphere},
  url          = {http://dx.doi.org/10.1016/j.scitotenv.2014.06.012},
  volume       = {493},
  year         = {2014},
}