Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
The measurement of chemical persistence in the field by benchmarking: Theory and Experiment
Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. (ACESo)ORCID iD: 0000-0002-7583-2982
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Persistence is one of the core criteria in chemical exposure and hazard assessment. It is often defined as the half-life for the removal of a chemical from a specified environment by transformation. Chemicals with long transformation half-lives may pose high risks for wildlife or humans and be subject to long-range transport to remote areas. It is challenging to measure persistence directly in the field in view of the complexity of the natural environment and spatial and temporal variability in environmental conditions that may affect degradation.

The mass balance approach is the most commonly used method for field measurement of persistence. In this thesis an alternative to the traditional mass balance approach that uses benchmarking is proposed and evaluated using models and field application. The benchmarking approach compares the relative behavior of chemicals, rather than measuring the absolute value of a property. The unknown property (persistence in this thesis) of test chemicals can be estimated by comparison against another chemical for which this property is known.

In Paper I, the potential of benchmarking to measure persistence in the field was evaluated by modeling. A framework for applying benchmarking to measure persistence in the field was developed. Lake systems with hydraulic residence times of the order of months were identified as appropriate field sites to measure the persistence of chemicals that are close to the regulatory thresholds, which are also on the scale of months. Field studies in two Swedish lakes were conducted. Both are shallow lakes, whereas Norra Bergundasjön (Paper II) has a longer residence time (four months) than Boren (one to two months; Paper III). In Paper II the benchmarking approach was tested to measure the persistence of a group of chemicals that were expected to stay in the water phase. Acesulfame K (artificial sweetener) without observable degradation in the lake was used as the benchmark chemical. The persistence of 9 pharmaceuticals and one X-ray contrast agent was measured to range from <1-2 days (ketoprofen) to 580-5700 days (carbamazepine). The results obtained using the benchmarking approach agreed well with the mass balance approach, indicating that the benchmarking approach can be a valid and useful method to measure persistence in the field. In Paper III the seasonality in chemical persistence was investigated by benchmarking. The seasonal difference in chemical persistence was found to be largest between spring and autumn. The persistence of 5 chemicals in spring were lower than in autumn, mainly attributed to lower temperature and less sunlight in autumn. The spatial variation of the persistence of chemicals was observed by comparing the persistence of chemicals in spring in the two lakes. Thus benchmarking is a useful tool to study the temporal and spatial variation of persistence in the real environment.  

Paper IV explores the potential of benchmarking thoroughly and the application of benchmarking in a regulatory context. Benchmarking could facilitate more field measurements of persistence, leading to a better understanding of the temporal and spatial variability of persistence in various environments and a basis for lab-to-field extrapolation. Besides quantitative estimation of persistence in the field, benchmarking can be applied to determine the relative magnitude of persistence, called threshold benchmarking which could be a valuable tool in regulatory processes.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University , 2015. , 36 p.
Keyword [en]
chemical benchmarking, persistence, half-lives, modeling, threshold benchmarking
National Category
Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-116840ISBN: 978-91-7649-146-1 (print)OAI: oai:DiVA.org:su-116840DiVA: diva2:808872
Public defence
2015-06-12, Nordenskiöldsalen, Geovetenskapens hus, Svante Arrhenius väg 12, Stockholm, 09:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Submitted. Paper 4: Manuscript.

Available from: 2015-04-21 Created: 2015-04-29 Last updated: 2015-10-28Bibliographically approved
List of papers
1. Evaluation of the potential of benchmarking to facilitate the measurement of chemical persistence in lakes
Open this publication in new window or tab >>Evaluation of the potential of benchmarking to facilitate the measurement of chemical persistence in lakes
2014 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 95, 301-309 p.Article in journal (Refereed) Published
Abstract [en]

The persistence of chemicals in the environment is rarely measured in the field due to a paucity of suitable methods. Here we explore the potential of chemical benchmarking to facilitate the measurement of persistence in lake systems using a multimedia chemical fate model. The model results show that persistence in a lake can be assessed by quantifying the ratio of test chemical and benchmark chemical at as few as two locations: the point of emission and the outlet of the lake. Appropriate selection of benchmark chemicals also allows pseudo-first-order rate constants for physical removal processes such as volatilization and sediment burial to be quantified. We use the model to explore how the maximum persistence that can be measured in a particular lake depends on the partitioning properties of the test chemical of interest and the characteristics of the lake. Our model experiments demonstrate that combining benchmarking techniques with good experimental design and sensitive environmental analytical chemistry may open new opportunities for quantifying chemical persistence, particularly for relatively slowly degradable chemicals for which current methods do not perform well.

Keyword
Benchmarking approach, Persistence, Aquatic environment, Multi-media model
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-97938 (URN)10.1016/j.chemosphere.2013.08.097 (DOI)000328868400043 ()
Available from: 2013-12-19 Created: 2013-12-19 Last updated: 2017-12-06Bibliographically approved
2. Using Chemical Benchmarking to Determine the Persistence of Chemicals in a Swedish Lake
Open this publication in new window or tab >>Using Chemical Benchmarking to Determine the Persistence of Chemicals in a Swedish Lake
Show others...
2015 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 3, 1646-1653 p.Article in journal (Refereed) Published
Abstract [en]

It is challenging to measure the persistence of chemicals under field conditions. In this work, two approaches for measuring persistence in the field were compared: the chemical mass balance approach, and a novel chemical benchmarking approach. Ten pharmaceuticals, an X-ray contrast agent, and an artificial sweetener were studied in a Swedish lake. Acesulfame K was selected as a benchmark to quantify persistence using the chemical benchmarking approach. The 95% confidence intervals of the half-life for transformation in the lake system ranged from 780-5700 days for carbamazepine to <1-2 days for ketoprofen. The persistence estimates obtained using the benchmarking approach agreed well with those from the mass balance approach (1-21% difference), indicating that chemical benchmarking can be a valid and useful method to measure the persistence of chemicals under field conditions. Compared to the mass balance approach, the benchmarking approach partially or completely eliminates the need to quantify mass flow of chemicals, so it is particularly advantageous when the quantification of mass flow of chemicals is difficult. Furthermore, the benchmarking approach allows for ready comparison and ranking of the persistence of different chemicals.

National Category
Earth and Related Environmental Sciences Chemical Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-115690 (URN)10.1021/es505548k (DOI)000349060300050 ()25565241 (PubMedID)
Note

AuthorCount:5;

Available from: 2015-03-30 Created: 2015-03-27 Last updated: 2017-12-04Bibliographically approved
3. Temporal Variation of Chemical Persistence in a Swedish Lake Assessed by Benchmarking
Open this publication in new window or tab >>Temporal Variation of Chemical Persistence in a Swedish Lake Assessed by Benchmarking
2015 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 16, 9881-9888 p.Article in journal (Refereed) Published
Abstract [en]

Chemical benchmarldng was used to investigate the temporal variation of the persistence of chemical contaminants in a Swedish lake. The chemicals studied included 12 pharmaceuticals, an artificial sweetener, and an X-ray contrast agent. Measurements were conducted in late spring, late autumn, and winter. The transformation half-life in the lake could be quantified for 7 of the chemicals. It ranged from several days to hundreds of days. For 5 of the chemicals (bezafibrate, climbazole, diclofenac, furosemide, and hydrochlorothiazide), the measured persistence was lower in late spring than in late autumn. This may have been caused by lower temperatures and/or less irradiation during late autumn. The seasonality in chemical persistence contributed to changes in chemical concentrations in the lake during the year. The impact of seasonality of persistence was compared with the impact of other important variables determining concentrations in the lake: chemical inputs and water flow/dilution. The strongest seasonal variability in chemical concentration in lake water was observed for hydrochlorothiazide (over a factor of 10), and this was attributable to the seasonality in its persistence.

National Category
Environmental Engineering Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-120649 (URN)10.1021/acs.est.5b01720 (DOI)000359891700058 ()
Available from: 2015-09-15 Created: 2015-09-15 Last updated: 2017-12-04Bibliographically approved
4. Using benchmarking to strengthen the assessment of persistence
Open this publication in new window or tab >>Using benchmarking to strengthen the assessment of persistence
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Chemical persistence is a key property for assessing chemical risk and chemical hazard. Current methods for evaluating persistence are questionable, since the relationship between conditions in the environment and conditions in the laboratory tests employed to evaluate persistence is often unclear. Chemical benchmarking opens new possibilities to measure persistence in the field. In this paper we explore how the benchmarking approach can be applied in both the laboratory and the field to deepen our understanding of chemical persistence in the environment and create a solid scientific basis for laboratory to field extrapolation of persistence test results.

Keyword
benchmarking, persistence, regulations
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-116867 (URN)
Available from: 2015-04-30 Created: 2015-04-30 Last updated: 2016-01-29Bibliographically approved

Open Access in DiVA

fulltext(1220 kB)58 downloads
File information
File name FULLTEXT01.pdfFile size 1220 kBChecksum SHA-512
4cc84d25a1a170805f3a5535f4e4800725829a89f62b57578815200e5f6edc51a62d71ecf315a50794294d84018ff180587c501cd7be441fbb36ab82210f4911
Type fulltextMimetype application/pdf

Search in DiVA

By author/editor
Zou, Hongyan
By organisation
Department of Environmental Science and Analytical Chemistry
Earth and Related Environmental Sciences

Search outside of DiVA

GoogleGoogle Scholar
Total: 58 downloads
The number of downloads is the sum of all downloads of full texts. It may include eg previous versions that are now no longer available

isbn
urn-nbn

Altmetric score

isbn
urn-nbn
Total: 279 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf