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Mercury immobilization: a requirement for permanent disposal of mercury waste in Sweden
Örebro University, Department of Natural Sciences.
2006 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The Swedish Government states that mercury in the Swedish industry and private use shall be collected and waste containing more than 1% of mercury shall be conditioned for permanent storage in proposed groundwater-saturated repository in deep bedrock. The owners of mercury waste in Sweden are responsible for finding ways to the conversion of the mercury waste to insoluble forms.

The aim of this thesis was to investigate different low-cost immobilization methods for mercury. Choice of treatment method depends on the nature of the waste, such as the mercury concentration and matrix constituents. High-contaminated waste would be suitable to transform to chemically insoluble mercury forms, while low-contaminated wastes would be suitable to treat with an encapsulation method. The investigations assessed conditions favourable for the formation of HgS at room temperature from elemental mercury as well as from mercury oxide. Elemental sulphur in an alkaline anaerobic environment gave a yield of close to 100% mercury sulphide within two years.

The stabilization/solidification (S/S) method was estimated as a suitable treatment method for low contaminated mercury waste (below 5%w/w). The lowest leaching rate was observed from slag monoliths with elemental sulphur as sulphur source. After one year the accumulated leaching amount was 0.008-0.013%w/w of the total mercury content of the monolith (1% of the monolith mass). This is about 100-150 times more than from monoliths that initially contained black meta-cinnabar.

Apparent diffusion coefficients for Hg(II)(aq) were determined in cement monoliths with different constituents (10-14-10-15 m2/s), for a barrier of Standard Portland concrete (10-14 m2/s) and in quartz sand (10-13 m2/s). After some 60 d in the leaching test, the apparent diffusion coefficient was of the order 10-17-10-21 m2/s, which was indicative of a slow release rate of the remaining mercury that could represent the dissolution/transformation of HgS, which gradually was formed during curing of the cement (aged for one year). The apparent diffusion coefficient for Hg(0) could not be measured since the mercury species oxidizes in aerobic systems.

Place, publisher, year, edition, pages
Örebro: Örebro universitetsbibliotek , 2006. , p. 35
Series
Örebro Studies in Environmental Science, ISSN 1650-6278 ; 8
Keywords [en]
mercury, mercury sulphide, cinnabar, stabilization, solidification, encapsulation, monolith leaching, solubility, mercury speciation, diffusion, apparent diffusion coefficient
National Category
Chemical Sciences
Research subject
Enviromental Science
Identifiers
URN: urn:nbn:se:oru:diva-207ISBN: 91-7668-466-0 (print)OAI: oai:DiVA.org:oru-207DiVA, id: diva2:135847
Public defence
2006-02-03, P1, Prismahuset, Örebro universitet, Örebro, 10:00
Opponent
Supervisors
Available from: 2006-01-13 Created: 2006-01-12 Last updated: 2017-10-18Bibliographically approved
List of papers
1. Speciation and solubility of mercury in aerobic solutions
Open this publication in new window or tab >>Speciation and solubility of mercury in aerobic solutions
(English)Manuscript (Other academic)
National Category
Chemical Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-2969 (URN)
Available from: 2006-01-13 Created: 2006-01-13 Last updated: 2017-10-18Bibliographically approved
2. Formation of cinnabar: an estimation of favourable conditions
Open this publication in new window or tab >>Formation of cinnabar: an estimation of favourable conditions
2006 (English)Manuscript (preprint) (Other academic)
National Category
Chemical Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-2970 (URN)
Available from: 2006-01-13 Created: 2006-01-13 Last updated: 2017-10-18Bibliographically approved
3. Formation of HgS: mixing HgO or elemental Hg with S, FeS or FeS2
Open this publication in new window or tab >>Formation of HgS: mixing HgO or elemental Hg with S, FeS or FeS2
2006 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 368, no 1, p. 418-423Article in journal (Refereed) Published
Abstract [en]

The aim of this study is to assess the feasibility for generation of the sparingly soluble solid HgS from HgO or elemental Hg by mixing with a suitable sulphur source under various conditions (dry, wet at different pH, and room temperature). The formation of mercury sulphide was confirmed in 14 of the 36 combinations of Hg and S sources. Mercury sulphide was generally formed under alkaline conditions. Almost 100% HgS was obtained in anaerobic systems at high pH in the presence of elemental sulphur after about two years. Thus, it is feasible to create an environment at room temperature that, with time, leads to the generation of HgS from elemental Hg or HgO. This is relevant for the design of a repository for permanent geologic disposal of mercury. Choosing wrong components and conditions can however lead to a reduction of Hg(II) to elemental mercury.

National Category
Chemical Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-2971 (URN)10.1016/j.scitotenv.2005.09.040 (DOI)
Note
Selected papers from the 7th International Conference on Mercury as a Global Pollutant, Ljubljana, Slovenia June 27 - July 2, 2004Available from: 2006-01-13 Created: 2006-01-13 Last updated: 2017-12-14Bibliographically approved
4. Leaching of mercury-containing cement monoliths aged for one year
Open this publication in new window or tab >>Leaching of mercury-containing cement monoliths aged for one year
2008 (English)In: Waste Management, ISSN 0956-053X, E-ISSN 1879-2456, Vol. 28, no 3, p. 597-603Article in journal (Refereed) Published
Abstract [en]

A directive from the Swedish Government states that waste containing more than 1% of mercury shall be permanently deposited. The stabilization of mercury by conversion to a sparingly soluble compound like the sulphide is crucial to ensure long-term immobilization in a permanent storage. Immobilization by the solidification/stabilization (S/S) method and possible formation of HgS from mercury oxide or elemental mercury by reaction with a sulphur source (S or FeS) is investigated by a modified version of the NEN 7345 Dutch tank-leaching test. The diffusion of mercury during 11 months from 1-year-old mercury containing monoliths of Portland and slag cement is demonstrated. In a geologic repository under conditions representative of deep granitic bedrock (bicarbonate buffered to pH 8.6), a favourable monolith combination is slag cement with addition of the iron sulphide troilite. The apparent diffusion coefficient of mercury is estimated.

National Category
Environmental Sciences Chemical Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-2972 (URN)10.1016/j.wasman.2007.02.031 (DOI)000253097600016 ()17544639 (PubMedID)2-s2.0-37449015893 (Scopus ID)
Available from: 2006-01-13 Created: 2006-01-13 Last updated: 2017-12-14Bibliographically approved
5. Diffusion tests of mercury through concrete, bentonite-enhanced sand and sand
Open this publication in new window or tab >>Diffusion tests of mercury through concrete, bentonite-enhanced sand and sand
(English)Manuscript (preprint) (Other academic)
National Category
Chemical Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-2973 (URN)
Available from: 2006-01-13 Created: 2006-01-13 Last updated: 2017-10-18Bibliographically approved

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