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  • 1.
    Grahn, Evastina
    Örebro University, Department of Natural Sciences.
    Lake sediment as environmental archive: natural and anthropogenic influence on the chronology of trace elements2006Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The focus of this thesis is the historical pollution of some seldom-monitored trace elements (SMTEs; Ag, Be, Ga, In, Sb and Tl) that have been involuntarily released for several thousands of years but whose usage have increased during the industrial era. Sediment cores from four rural lakes in a south to north transect in central Sweden, and two urban lakes have been used as environmental archives for chronological studies. The historical development of the SMTEs is put in perspective of frequently monitored elements (Cd, Cu, Pb and Zn) that serve as a well-known anthropogenic signal. Dating of the sediments is made with 210Pb, 137Cs and 239,240Pu as well as acid leachable lead and the 206Pb/207Pb ratio. The impact of diagenetic redistribution is included, when necessary.

    The results show that site-specific reference concentrations are required in order to estimate the present pollution as well as its historical development. Atmospheric deposition is the principal pathway of transport in rural lakes and the concentrations are lowered towards the north. It is not possible from this material, however, to separate the direct deposition on the lake surfaces from the contribution from their catchments. From 21Pb, acid-leachable Pb and the 206Pb/207Pb ratio a minimum of four periods of pollution can be discerned. For the SMTEs the quantitatively most important period of pollution took place from the Second World War until present. The growth of the domestic industrialisation as well as the early industrialisation of central Europe and the British Isles are also distinguishable. The pollution history of Ag, In and Sb goes back for several centuries as a result of metal processing whereas the levels of thallium mainly increase as a result of industrialisation. For Ag and Tl in-sediment diagenetic redistribution limits the precision of the historical estimate. The preliminary interpretation of 137Cs and 239,240Pu indicates that they are less suitable as chronological markers in the system studied. The urban impact on the trace metal sediment content in the urban lakes was lower than expected, except for Au. There is a large impact from hydrological conditions on the studied system why further investigations are recommended.

    List of papers
    1. Sediment reference concentrations of seldom monitored trace elements (Ag, Be, In, Ga, Sb, Tl) in four Swedish boreal lakes: comparison with commonly monitored elements
    Open this publication in new window or tab >>Sediment reference concentrations of seldom monitored trace elements (Ag, Be, In, Ga, Sb, Tl) in four Swedish boreal lakes: comparison with commonly monitored elements
    2006 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 367, no 2-3, p. 778-790Article in journal (Refereed) Published
    Abstract [en]

    This paper presents reference and recent acid-leachable concentrations of some seldom monitored trace elements (SMTE; Ag, Be, Ga, In, Sb and Tl) in sediments from four boreal oligotrophic lakes in a south to north transect in Sweden. For comparison commonly monitored trace elements (As, Cd, Co, Cr, Cu, Ni, Pb and Zn) are included as well as those of relevance for redistribution processes (Al, Ca, Fe, Mg and Mn).

    Pore water pH and the corresponding solid/solution distribution coefficients (Kd) indicated that redistribution of the elements due to acidification is minor. The depth of impact was defined as the level in the sediment where the mean values became constant on successive exclusion of metal concentrations in overlying strata. Reference concentrations were calculated below the depth of impact. The present concentration changes are estimated by the ratio between the average concentration above the depth of impact and the reference concentration.

    Reference concentration ranges for the SMT-elements are (mg/kg, dry wt.): Ag 0.16–0.66; Be 1.6–3.7; Ga 2.0–5.1; In 0.05–0.22; Sb 0.05–0.11 and Tl 0.17–0.70. The concentration ratios for these elements ranged in the two most southern lakes from 1.5 to 4.5 and in the two northern ones from 0.6 to 1.6. A high correlation between Kd for the SMT-elements, and iron, except for Sb and Tl, infer that the biogeochemistry of iron is quantitatively important for the accumulation of these elements.

    The reference concentration ranges for the commonly monitored trace elements are (mg/kg, dry wt.): As 7.0–29.6; Cd 0.33–0.98; Co 5.7–23.8; Cr 15.2–26.1; Cu 27.6–58.4; Ni 5.4–20.8; Pb 44–96. The corresponding concentration ratios were 1.2–18 (second highest 3.9) in the two most southern lakes and 0.8–1.6 in the two northern ones. Declining ratios were found from south to north, most obvious for cobalt and zinc. The copper ratios did not show a regional pattern, partly because of the impact from old mine waste.

    Increased concentrations of Ag, Be, Ga, In, Sb and Tl in recent sediments up to 4.5 times the reference levels in combination with the geographical pattern infer an elevated loading of these elements.

    National Category
    Environmental Sciences
    Research subject
    Enviromental Science
    Identifiers
    urn:nbn:se:oru:diva-3058 (URN)10.1016/j.scitotenv.2006.01.018 (DOI)
    Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2017-12-14Bibliographically approved
    2. Historical pollution of seldom monitored trace elements in Sweden - Part A: sediment properties and chronological indicators
    Open this publication in new window or tab >>Historical pollution of seldom monitored trace elements in Sweden - Part A: sediment properties and chronological indicators
    2006 (English)In: Journal of Environmental Monitoring, ISSN 1464-0325, E-ISSN 1464-0333, Vol. 8, no 7, p. 721-731Article in journal (Refereed) Published
    Abstract [en]

    Sediment cores from four small oligotrophic boreal lakes, with minor acidification, in remote regions of central Sweden were used for historical interpretation of their metal content, with focus on Cu, Cd, Pb and Zn in Lake Stensjön, which has the longest sediment record (at least two centuries according to 210Pb dating). Comparison is made with the other three lakes. Major and trace elements in lake water, porewater and the acid-leached (HNO3) solid sediment phase was analysed with ICP-MS. In addition, general lake water chemistry, TOC and principal anions were measured in the aqueous phases. Redistribution processes were interpreted from geochemical modelling. The solid/solution distribution of pe/pH sensitive elements, indicates a minor diagenetic redistribution and the concentration profiles are therefore suitable for chronological evaluation. The ratios of Al, Ti, Sc and V, indicated a qualitative shift of sedimenting material a century ago, which did not have any impact on the retention of trace elements. Lead had a concentration profile, supported by the 206Pb/207Pb ratio, where it was possible to distinguish preindustrial conditions, early industrialisation in Europe, industrialisation in Sweden, and the use of leaded petrol after the Second World War. Cadmium showed a similar concentration pattern. The zinc profile resembled that of cadmium, but with less enrichment. Local lithogenic sources are believed to be quantitatively important. The solid/solution distribution (Kd) was independent of depth for all four elements. The sediment concentrations of copper and zinc are not related to early industrialisation but its concentration has doubled since the Second World War.

    National Category
    Chemical Sciences Environmental Sciences
    Research subject
    Enviromental Science
    Identifiers
    urn:nbn:se:oru:diva-3059 (URN)10.1039/B601944G (DOI)16826285 (PubMedID)
    Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2017-12-14Bibliographically approved
    3. Historical pollution of seldom monitored trace elements in Sweden: Part B: sediment analysis of silver, antimony, thallium and indium
    Open this publication in new window or tab >>Historical pollution of seldom monitored trace elements in Sweden: Part B: sediment analysis of silver, antimony, thallium and indium
    2006 (English)In: Journal of Environmental Monitoring, ISSN 1464-0325, E-ISSN 1464-0333, Vol. 8, no 7, p. 732-744Article in journal (Refereed) Published
    Abstract [en]

    Sediment cores from four boreal and remote lakes in a south to north transect in central Sweden were analysed for acid leachable silver, antimony, thallium and indium in the solid sediment phase and the corresponding porewater. Dating of the cores was made by their content of acid leachable lead and the 206Pb/207Pb ratio, in one lake also by 210Pb. The impact of diagenesis on element redistribution in the sediments was included and found to be minor except for thallium. The results show lowered concentrations towards the north and most intense accumulation after the Second World War, which is taken as evidence for atmospheric deposition being the primary source. Indium has declining concentrations in recent strata while silver and antimony increase. Thallium has lowered acid-leachable concentrations in recent strata. For all metals the impact of domestic industrialisation as well as the early industrialisation of central Europe is discernible. Only thallium appears to reach a geological background at depths that correspond to the late 18th century. For the other metals elevated levels are concluded.

    National Category
    Environmental Sciences Chemical Sciences
    Research subject
    Enviromental Science
    Identifiers
    urn:nbn:se:oru:diva-3053 (URN)10.1039/B601948J (DOI)
    Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2017-12-14Bibliographically approved
    4. Seldom monitored trace elements (Ag, Au, Ga, In, Sb, Tl) in two urban lake sediments in Central Sweden: a case study
    Open this publication in new window or tab >>Seldom monitored trace elements (Ag, Au, Ga, In, Sb, Tl) in two urban lake sediments in Central Sweden: a case study
    (English)Manuscript (Other academic)
    National Category
    Environmental Sciences
    Research subject
    Enviromental Science
    Identifiers
    urn:nbn:se:oru:diva-3061 (URN)
    Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2017-10-18Bibliographically approved
    5. Failure of 137Cs and 239/240Pu dating of lake sediments: fallout from nuclear weapons testing and from the Chernobyl accident as well as redistribution processes?
    Open this publication in new window or tab >>Failure of 137Cs and 239/240Pu dating of lake sediments: fallout from nuclear weapons testing and from the Chernobyl accident as well as redistribution processes?
    Show others...
    (English)Manuscript (Other academic)
    National Category
    Environmental Sciences
    Research subject
    Enviromental Science
    Identifiers
    urn:nbn:se:oru:diva-3062 (URN)
    Available from: 2006-03-09 Created: 2006-03-09 Last updated: 2017-10-18Bibliographically approved
  • 2.
    Grahn, Evastina
    et al.
    Örebro University, Department of Natural Sciences.
    Karlsson, Stefan
    Örebro University, Department of Natural Sciences.
    Düker, Anders
    Örebro University, Department of Natural Sciences.
    Sediment reference concentrations of seldom monitored trace elements (Ag, Be, In, Ga, Sb, Tl) in four Swedish boreal lakes: comparison with commonly monitored elements2006In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 367, no 2-3, p. 778-790Article in journal (Refereed)
    Abstract [en]

    This paper presents reference and recent acid-leachable concentrations of some seldom monitored trace elements (SMTE; Ag, Be, Ga, In, Sb and Tl) in sediments from four boreal oligotrophic lakes in a south to north transect in Sweden. For comparison commonly monitored trace elements (As, Cd, Co, Cr, Cu, Ni, Pb and Zn) are included as well as those of relevance for redistribution processes (Al, Ca, Fe, Mg and Mn).

    Pore water pH and the corresponding solid/solution distribution coefficients (Kd) indicated that redistribution of the elements due to acidification is minor. The depth of impact was defined as the level in the sediment where the mean values became constant on successive exclusion of metal concentrations in overlying strata. Reference concentrations were calculated below the depth of impact. The present concentration changes are estimated by the ratio between the average concentration above the depth of impact and the reference concentration.

    Reference concentration ranges for the SMT-elements are (mg/kg, dry wt.): Ag 0.16–0.66; Be 1.6–3.7; Ga 2.0–5.1; In 0.05–0.22; Sb 0.05–0.11 and Tl 0.17–0.70. The concentration ratios for these elements ranged in the two most southern lakes from 1.5 to 4.5 and in the two northern ones from 0.6 to 1.6. A high correlation between Kd for the SMT-elements, and iron, except for Sb and Tl, infer that the biogeochemistry of iron is quantitatively important for the accumulation of these elements.

    The reference concentration ranges for the commonly monitored trace elements are (mg/kg, dry wt.): As 7.0–29.6; Cd 0.33–0.98; Co 5.7–23.8; Cr 15.2–26.1; Cu 27.6–58.4; Ni 5.4–20.8; Pb 44–96. The corresponding concentration ratios were 1.2–18 (second highest 3.9) in the two most southern lakes and 0.8–1.6 in the two northern ones. Declining ratios were found from south to north, most obvious for cobalt and zinc. The copper ratios did not show a regional pattern, partly because of the impact from old mine waste.

    Increased concentrations of Ag, Be, Ga, In, Sb and Tl in recent sediments up to 4.5 times the reference levels in combination with the geographical pattern infer an elevated loading of these elements.

  • 3.
    Grahn, Evastina
    et al.
    Örebro University, Department of Natural Sciences.
    Karlsson, Stefan
    Örebro University, Department of Natural Sciences.
    Karlsson, Ulrika
    Örebro University, Department of Natural Sciences.
    Düker, Anders
    Örebro University, Department of Natural Sciences.
    Historical pollution of seldom monitored trace elements in Sweden: Part B: sediment analysis of silver, antimony, thallium and indium2006In: Journal of Environmental Monitoring, ISSN 1464-0325, E-ISSN 1464-0333, Vol. 8, no 7, p. 732-744Article in journal (Refereed)
    Abstract [en]

    Sediment cores from four boreal and remote lakes in a south to north transect in central Sweden were analysed for acid leachable silver, antimony, thallium and indium in the solid sediment phase and the corresponding porewater. Dating of the cores was made by their content of acid leachable lead and the 206Pb/207Pb ratio, in one lake also by 210Pb. The impact of diagenesis on element redistribution in the sediments was included and found to be minor except for thallium. The results show lowered concentrations towards the north and most intense accumulation after the Second World War, which is taken as evidence for atmospheric deposition being the primary source. Indium has declining concentrations in recent strata while silver and antimony increase. Thallium has lowered acid-leachable concentrations in recent strata. For all metals the impact of domestic industrialisation as well as the early industrialisation of central Europe is discernible. Only thallium appears to reach a geological background at depths that correspond to the late 18th century. For the other metals elevated levels are concluded.

  • 4.
    Karlsson, Stefan
    et al.
    Örebro University, School of Science and Technology.
    Allard, Bert
    Örebro University, School of Science and Technology.
    Grahn, Evastina
    Örebro University, School of Science and Technology.
    Mobility of Cs and Pu from fallout in boreal lake sediments2009Conference paper (Refereed)
  • 5.
    Karlsson, Stefan
    et al.
    Örebro University, Department of Natural Sciences.
    Düker, Anders
    Örebro University, Department of Natural Sciences.
    Grahn, Evastina
    Örebro University, Department of Natural Sciences.
    Sediment chronologies of As, Bi, and Ga in Sweden - impact of industrialisation2007In: Journal of Environmental Science and Health. Part A: Toxic/Hazardous Substances and Environmental Engineering, ISSN 1093-4529, E-ISSN 1532-4117, Vol. 42, no 2, p. 155-164Article in journal (Refereed)
    Abstract [en]

    The acid-leachable amount and pore water concentration of As, Bi and Ga in sediment cores from four remote lakes in a south to north transect in Sweden were used to recapitulate the pollution history of the elements. The diagenetic impact on the element distribution was elucidated from their solid/solution partition and relationships to elements indicative for diagenesis. Dating was made by their acid-leachable lead content in combination with the Pb-206/Pb-207 ratio. In one of the lakes this approach was validated against dating with Pb-210. The impact of diagenesis on the sediment distribution of theses elements was found to be low enough for a chronological interpretation of the sediment profiles, as evidenced by their ratios to elements indicative of the geological background. A closer examination of the diagenetic impact would however be required if a more detailed chronology is desired. This study has demonstrated that atmospheric deposition of arsenic, bismuth and gallium contributes to the sediment inventory of these elements. The major part of the deposition of arsenic and bismuth took place after the Second World War. For gallium no concentrations exceeding background were detected before circa 1930. Increased levels of arsenic are traceable to circa 1850. For bismuth increased levels are concluded to extend before 1790, i.e., background concentrations were not reached in the present cores. For all elements the atmospheric deposition has been lower towards the north.

  • 6.
    Karlsson, Stefan
    et al.
    Örebro University, Department of Natural Sciences.
    Grahn, Evastina
    Örebro University, Department of Natural Sciences.
    Düker, Anders
    Örebro University, Department of Natural Sciences.
    Bäckström, Mattias
    Örebro University, Department of Natural Sciences.
    Historical pollution of seldom monitored trace elements in Sweden - Part A: sediment properties and chronological indicators2006In: Journal of Environmental Monitoring, ISSN 1464-0325, E-ISSN 1464-0333, Vol. 8, no 7, p. 721-731Article in journal (Refereed)
    Abstract [en]

    Sediment cores from four small oligotrophic boreal lakes, with minor acidification, in remote regions of central Sweden were used for historical interpretation of their metal content, with focus on Cu, Cd, Pb and Zn in Lake Stensjön, which has the longest sediment record (at least two centuries according to 210Pb dating). Comparison is made with the other three lakes. Major and trace elements in lake water, porewater and the acid-leached (HNO3) solid sediment phase was analysed with ICP-MS. In addition, general lake water chemistry, TOC and principal anions were measured in the aqueous phases. Redistribution processes were interpreted from geochemical modelling. The solid/solution distribution of pe/pH sensitive elements, indicates a minor diagenetic redistribution and the concentration profiles are therefore suitable for chronological evaluation. The ratios of Al, Ti, Sc and V, indicated a qualitative shift of sedimenting material a century ago, which did not have any impact on the retention of trace elements. Lead had a concentration profile, supported by the 206Pb/207Pb ratio, where it was possible to distinguish preindustrial conditions, early industrialisation in Europe, industrialisation in Sweden, and the use of leaded petrol after the Second World War. Cadmium showed a similar concentration pattern. The zinc profile resembled that of cadmium, but with less enrichment. Local lithogenic sources are believed to be quantitatively important. The solid/solution distribution (Kd) was independent of depth for all four elements. The sediment concentrations of copper and zinc are not related to early industrialisation but its concentration has doubled since the Second World War.

1 - 6 of 6
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