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Organic Micropollutants in Stormwater and Biofilter Systems: Treatment, Accumulation, and Dynamics
Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Architecture and Water.ORCID iD: 0009-0000-5333-2971
2025 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Anthropogenic activities impact the quality of stormwater in urban areas. Urban runoff usually contains high concentrations of organic micropollutants (OMPs), which can adversely affect public health and the ecology of receiving waterbodies. The work described in this thesis aims to evaluate the concentrations, occurrences, and environmental risks of OMPs in stormwater runoff. It contributes towards identifying, monitoring, and controlling their environmental impacts and risks through mitigation strategies that protect human health and water resources.

Stormwater biofilter (bioretention) systems have been developed and implemented in recent decades as a mitigation strategy for in-situ stormwater treatment. The studies in this thesis seek to improve field-scale understanding of the fate and transport behaviors of OMPs in stormwater biofilter systems, assess biofilters’ design performance for OMP treatment from both design suitability and maintenance perspectives, and evaluate their potential to mitigate OMP risks to receiving waterbodies. This research explored/validated the treatability, short-term intra-event variations (IEVs), long-term accumulation, and environmental risks of OMPs in 27 sand-based biofilter facilities located in various catchment types and with different design features (including amendments with vegetation, chalk, and biochar). Some of the key findings revealed by the thesis are as follows:

Various OMP families, such as polycyclic aromatic hydrocarbons (PAHs), petroleum hydrocarbons (PHCs), phenolics substances, organotin compounds (OTCs), and perfluoroalkyl substances (PFASs), were present in stormwater runoff at concentrations often problematic for receiving waterbodies. Intra-event concentrations varied substantially during rain events. The rain intensity was one of the most influential factors affecting IEVs during short rainfall events.Depending on the pollutant’s physio-chemical properties and the treatment unit’s design features, the performance of the studied biofilter systems ranged from weak (negative removal efficiencies) to sufficient (up to 98%) in removing OMPs. Among the amendments used in the sand-based biofilters, the presence of a vegetated layer increased the removal (>30% improvement compared to non-vegetated or partially-vegetated biofilters) and reduced IEVs. However, no differences were observed after biochar or chalk amendment. The field observations revealed several complexities associated with applying biochar that must be considered/adapted for stormwater treatment.The long-term accumulation of hydrophobic, particle-bound OMPs, such as heavier PAHs, PHCs, and phthalates (only DEHP), in the filter materials was dominant (with higher occurrence/concentrations atop the biofilters), as they achieved higher removal from stormwater. Conversely, the removal or long-term accumulation of more mobile, hydrophilic, and slow-adsorbing OMPs, including bisphenol A (a phenolic substance), monobutyltin (an OTC), and PFASs, was lower and inconsistent in both amended and non-amended biofilters, showing a need for more effective biofilter design and maintenance strategies for these challenging compounds.

Abstract [sv]

Antropogena aktiviteter påverkar kvaliteten på dagvatten i urbana områden. Urban avrinning innehåller ofta höga koncentrationer av organiska ämnen, vilket kan ha negativa effekter på folkhälsan och ekologin i de recipienter som tar emot dagvattnet. Denna avhandling syftar till att utvärdera koncentrationer, förekomst och miljörisker av organiska mikroföroreningar (eng. organic micropollutants, OMPs) i dagvattenavrinning. Arbetet bidrar till att identifiera, övervaka och kontrollera miljöpåverkan och risker genom åtgärdsstrategier som skyddar både människors hälsa och vattenresurser.

Dagvattenbiofilter har utvecklats och implementerats under de senaste decennierna som en åtgärdsstrategi för lokal dagvattenrening. Detta arbete strävar också efter att förbättra förståelsen av organiska mikroföroreningars transport och nedbrytningsprocesser i biofilter, att bedöma biofiltrens prestanda för OMP-rening utifrån både utformning och underhållsperspektiv samt att utvärdera deras potential att minska OMP-utsläpp till recipienter. Forskningen undersökte och verifierade den generella reningen av OMP, kortsiktiga variationer under avrinningshändelser, långsiktig ackumulering OMP och därmed förknippade miljörisker i biofilteranläggningar. Några av de viktigaste resultaten i avhandlingen är följande:

Olika OMP-familjer, såsom polycykliska aromatiska kolväten (PAH), petroleumkolväten (PHC), fenolföreningar, organiska tennföreningar (OTC) och perfluorerade ämnen (PFAS), påträffades i dagvattenavrinning i koncentrationer som ofta är problematiska för recipienternas miljö. Koncentrationer av PAH och fenoler var högre i avrinning från en motorväg jämfört med ett blandat stadsområde. Under regnhändelserna varierade koncentrationerna kraftigt och regnintensitet var en av de mest inflytelserika faktorerna för dessa variationer vid kortare nederbördshändelser.OMP-rening i de studerade biofiltersystemen varierade mycket, från undermålig (negativa reningsprocent) till mycket effektiv (upp till 98% rening), beroende på föroreningarnas fysikalisk-kemiska egenskaper och biofiltrens utformning. Bland de sandbaserade biofiltrens tillsatsmaterial visade sig växtlighet att vara en viktig faktor för avskiljning (över 30 % förbättring jämfört med icke-växtbevuxna eller delvis bevuxna biofilter). Däremot observerades inga signifikanta skillnader pga. tillsats av biokol och kalk. Fältstudierna avslöjade komplexiteten kopplad till användningen av biokol, som bör beaktas och anpassas vid dagvattenrening.Den långsiktiga ackumuleringen av hydrofoba, partikelbundna OMP (såsom tyngre PAH, PHC och ftalaten DEHP) i filtermaterialen var dominerande (med högre förekomst/koncentrationer i biofiltrens övre skikt). Anledningen är att dessa föroreningar effektivt avskildes från dagvattnet tillsammans med sediment. Däremot var avskiljning och långsiktig ackumulering av mer mobila, hydrofila och långsamt adsorberande OMP (inklusive bisfenol A (en fenolförening), monobutyltenn (en OTC) och PFAS) lägre och varierande i både modifierade och icke-modifierade biofilter. Detta visar på ett behov av mer effektiva biofilterdesign- och underhållsstrategier för dessa utmanande ämnen.

Place, publisher, year, edition, pages
Luleå University of Technology, 2025.
Series
Doctoral thesis / Luleå University of Technology 1 jan 1997 → …, ISSN 1402-1544
Keywords [en]
Urban runoff, Trace organic compounds (TrOCs), Bioretention, Accumulation, Vegetation, Biochar, Intra-event variations, Environmental risks
Keywords [sv]
Urban avrinning, Spåra organiska föroreningar, Bioretention, Ackumulation, Vegetation, Biokol, variationer under avrinningshändelser, Miljörisker
National Category
Water Engineering
Research subject
Urban Water Engineering
Identifiers
URN: urn:nbn:se:ltu:diva-111244ISBN: 978-91-8048-738-2 (print)ISBN: 978-91-8048-739-9 (electronic)OAI: oai:DiVA.org:ltu-111244DiVA, id: diva2:1930199
Public defence
2025-03-21, A117, Luleå University of Technology, Luleå, 09:00 (English)
Opponent
Supervisors
Available from: 2025-01-22 Created: 2025-01-22 Last updated: 2025-03-12Bibliographically approved
List of papers
1. Occurrence, Concentration, and Distribution of 35 PFASs and Their Precursors Retained in 20 Stormwater Biofilters
Open this publication in new window or tab >>Occurrence, Concentration, and Distribution of 35 PFASs and Their Precursors Retained in 20 Stormwater Biofilters
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2024 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 58, no 32, p. 14518-14529Article in journal (Refereed) Published
Abstract [en]

Current knowledge about the fate and transport behaviors of per- and polyfluoroalkyl substances (PFASs) in urban stormwater biofilter facilities is very limited. C5–14,16 perfluoroalkyl carboxylic acids [perfluorinated carboxylic acids (PFCAs)], C4,8,10 perfluoroalkanesulfonic acids (PFSAs), methyl-perfluorooctane sulfonamide acetic acid (MeFOSAA, a PFSA precursor), and unknown C6–8 PFCA and perfluorooctanesulfonic acid precursors were frequently found in bioretention media and forebay sediments at Σ35PFAS concentrations of <0.03–19 and 0.064–16 μg/kg-DW, respectively. Unknown C6–8 PFCA precursor concentrations were up to ten times higher than the corresponding PFCAs, especially at forebays and biofilters’ top layer. No significant trend could be attributed to PFAS and precursor concentrations versus depth of filter media, though PFAS concentrations were 2–3 times higher in the upper layers on average (significant difference between the upper (0–5 cm) and deepest (35–50 cm) layer). PFASs had a similar spatial concentration distribution in each filter media (no clear difference between short- and long-chain PFASs). Commercial land use and organic matter were important factors explaining the concentration variations among the biofilters and between the sampling depths, respectively. Given the comparable PFAS accumulations in deeper and superficial layers and possible increased mobility after precursor biotransformation, designing shallow-depth, nonamended sand biofilters or maintaining only the top layer may be insufficient for stormwater PFAS management.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024
Keywords
Urban runoff, Emerging contaminants, Bioretention, Filter media, Fate and Transport, Retention, TOP assay
National Category
Water Engineering
Research subject
Urban Water Engineering
Identifiers
urn:nbn:se:ltu:diva-108442 (URN)10.1021/acs.est.4c05170 (DOI)001280935500001 ()39078743 (PubMedID)2-s2.0-85199949644 (Scopus ID)
Projects
DRIZZLE
Funder
Swedish Environmental Protection Agency, NV-03810-23Vinnova, 2016-05176: DRIZZLESvenska Byggbranschens Utvecklingsfond (SBUF), 13623
Note

Validerad;2024;Nivå 2;2024-08-14 (hanlid);

Full text license: CC BY

Available from: 2024-07-31 Created: 2024-07-31 Last updated: 2025-01-22Bibliographically approved
2. Intra-event variations of organic micropollutants in highway runoff and a presedimentation-biofilter treatment facility
Open this publication in new window or tab >>Intra-event variations of organic micropollutants in highway runoff and a presedimentation-biofilter treatment facility
2024 (English)In: Journal of Hazardous Materials, ISSN 0304-3894, E-ISSN 1873-3336, Vol. 476, article id 135200Article in journal (Refereed) Published
Abstract [en]

The study assessed the quality of highway runoff and a stormwater treatment system, focusing on intra-event variations (IEVs: variations within a runoff/effluent event) of the concentration of organic micropollutants (OMPs) including bisphenol-A, alkylphenols, polycyclic aromatic hydrocarbons (PAHs), and petroleum hydrocarbons (PHCs). IEVs of OMPs varied considerably with no particular recurring pattern in highway runoff and presedimentation effluent, displaying sporadic strong first flushes. IEVs are significantly associated with rainfall intensity variations, especially for particle-bound substances such as PAHs and PHCs. However, phenolic substances showed distinct IEV patterns compared to total suspended solids, PAHs, and PHCs, likely due to their higher solubility and mobility. Downstream sand filter (SF) and vegetated biofilter (BFC) mitigated IEVs, leading to more uniform discharge during outflow events. Although BFC’s IEVs were indiscernible due to low effluent concentrations, SF’s IEVs often peaked at the beginning of events (within the first 100 of ⁓600 m3), exceeding the lowest predicted non-effect concentrations for five PAHs, bisphenol-A, and octylphenol. This study highlights the advantage of IEV analysis over conventional event mean concentration analysis for identifying critical effluent stages, crucial for developing control strategies to protect sensitive water recipients or for reuse applications.

Place, publisher, year, edition, pages
Elsevier, 2024
Keywords
Bioretention, Environmental risk analysis, First flush, Intra-event dynamics, Road runoff
National Category
Water Engineering
Research subject
Urban Water Engineering
Identifiers
urn:nbn:se:ltu:diva-108409 (URN)10.1016/j.jhazmat.2024.135200 (DOI)001269134900001 ()39003807 (PubMedID)2-s2.0-85198307581 (Scopus ID)
Funder
Swedish Research Council Formas, 2016-20074Swedish Water, 16-166Vinnova, 2022-03092
Note

Validerad;2024;Nivå 2;2024-07-25 (signyg);

Fulltext license: CC BY

Available from: 2024-07-25 Created: 2024-07-25 Last updated: 2025-01-22Bibliographically approved
3. Occurrence and concentrations of organic micropollutants (OMPs) in highway stormwater: a comparative field study in Sweden
Open this publication in new window or tab >>Occurrence and concentrations of organic micropollutants (OMPs) in highway stormwater: a comparative field study in Sweden
2023 (English)In: Environmental Science and Pollution Research, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 30, no 31, p. 77299-77317Article in journal (Refereed) Published
Abstract [en]

This study details the occurrence and concentrations of organic micropollutants (OMPs) in stormwater collected from a highway bridge catchment in Sweden. The prioritized OMPs were bisphenol-A (BPA), eight alkylphenols, sixteen polycyclic aromatic hydrocarbons (PAHs), and four fractions of petroleum hydrocarbons (PHCs), along with other global parameters, namely, total organic carbon (TOC), total suspended solids (TSS), turbidity, and conductivity (EC). A Monte Carlo (MC) simulation was applied to estimate the event mean concentrations (EMC) of OMPs based on intra-event subsamples during eight rain events, and analyze the associated uncertainties. Assessing the occurrence of all OMPs in the catchment and comparing the EMC values with corresponding environmental quality standards (EQSs) revealed that BPA, octylphenol (OP), nonylphenol (NP), five carcinogenic and four non-carcinogenic PAHs, and C16-C40 fractions of PHCs can be problematic for freshwater. On the other hand, alkylphenol ethoxylates (OPnEO and NPnEO), six low molecule weight PAHs, and lighter fractions of PHCs (C10-C16) do not occur at levels that are expected to pose an environmental risk. Our data analysis revealed that turbidity has a strong correlation with PAHs, PHCs, and TSS; and TOC and EC highly associated with BPA concentrations. Furthermore, the EMC error analysis showed that high uncertainty in OMP data can influence the final interpretation of EMC values. As such, some of the challenges that were experienced in the presented research yielded suggestions for future monitoring programs to obtain more reliable data acquisition and analysis.

Place, publisher, year, edition, pages
Springer Nature, 2023
Keywords
Road runoff, Quality monitoring, Monte-Carlo simulation, Uncertainty analysis, Censored data, Correlated parameters
National Category
Water Engineering
Research subject
Urban Water Engineering; Centre - Centre for Stormwater Management (DRIZZLE)
Identifiers
urn:nbn:se:ltu:diva-96463 (URN)10.1007/s11356-023-27623-9 (DOI)000999658600002 ()37253915 (PubMedID)2-s2.0-85160668482 (Scopus ID)
Funder
Swedish Research Council Formas, 2016–20074Vinnova, 2016–05176
Note

Validerad;2023;Nivå 2;2023-06-29 (sofila);

Available from: 2023-04-13 Created: 2023-04-13 Last updated: 2025-01-22Bibliographically approved
4. Performance of a gross pollutant trap-biofilter and sand filter treatment train for the removal of organic micropollutants from highway stormwater (Field study)
Open this publication in new window or tab >>Performance of a gross pollutant trap-biofilter and sand filter treatment train for the removal of organic micropollutants from highway stormwater (Field study)
2023 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 900, article id 165734Article in journal (Refereed) Published
Abstract [en]

This field study assessed the occurrence, event mean concentrations (EMCs), and removal of selected organic micro-pollutants (OMPs), namely, polycyclic aromatic hydrocarbons (PAHs), petroleum hydrocarbons (PHCs), nonylphenol (NP), 4-t-octylphenol (OP), and bisphenol A (BPA), in a gross pollutant trap (GPT)-biofilter/sand filter stormwater treatment train in Sundsvall, Sweden. The effects of design features of each treatment unit, including pre-sedimentation (GPT), sand filter medium, vegetation, and chalk amendment, were investigated by comparing the units' removal performances. Overall, the treatment train removed most OMPs from highway runoff effectively. The results showed that although the sand filter provided moderate (<50 % for phenolic substances) to high (50–80 % for PAHs and PHCs) removal of OMPs, adding a vegetated soil layer on top of the sand filter considerably improved the removal performance (by at least 30 %), especially for BPA, OP, and suspended solids. Moreover, GTP did not contribute to the treatment significantly. Uncertainties in the removal efficiencies of PAHs and PHCs by the filter cells increased substantially when the ratio of the influent concentration to the limit of quantification decreased. Thus, accounting for such uncertainties due to the low OMP concentrations should be considered when evaluating the removal performance of biofilters.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
Road runoff, Bioretention, Retention soil filter, Vegetation, Censored data, Uncertainty analysis, Risk analysis
National Category
Water Engineering Other Environmental Engineering
Research subject
Urban Water Engineering; Centre - Centre for Stormwater Management (DRIZZLE)
Identifiers
urn:nbn:se:ltu:diva-96477 (URN)10.1016/j.scitotenv.2023.165734 (DOI)001051910700001 ()37495141 (PubMedID)2-s2.0-85166273222 (Scopus ID)
Funder
Swedish Research Council Formas, 2016-20074Vinnova, 2016-05176
Note

Validerad;2023;Nivå 2;2023-08-14 (joosat);

Licens fulltext: CC BY License

This article has previously appeared as a manuscript in a thesis.

Available from: 2023-04-20 Created: 2023-04-20 Last updated: 2025-01-22Bibliographically approved
5. Critical field evaluations of biochar-amended stormwater biofilters for PFAS and other organic micropollutant removals
Open this publication in new window or tab >>Critical field evaluations of biochar-amended stormwater biofilters for PFAS and other organic micropollutant removals
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(English)Manuscript (preprint) (Other academic)
Keywords
Urban runoff, Bioretention, Biochar, Accumulation, Retention, PFAS
National Category
Water Engineering
Research subject
Centre - Centre for Stormwater Management (DRIZZLE); Urban Water Engineering; Experimental Physics; Experimental Mechanics
Identifiers
urn:nbn:se:ltu:diva-111366 (URN)
Available from: 2025-01-22 Created: 2025-01-22 Last updated: 2025-01-24

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Beryani, Ali

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