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Solute Transport Across Scales: Time Series Analyses of Water Quality Responses to Quantify Retention and Attenuation Mechanisms in Watersheds
KTH, School of Architecture and the Built Environment (ABE), Civil and Architectural Engineering, Hydraulic Engineering.ORCID iD: 0000-0003-2716-4446
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The intra-continental movement of waterborne contaminants is governed by the distribution of solute load in the landscape along with the characteristics and distribution of the hydrological pathways that transport the solutes. An understanding of the processes affecting the transport and fate of the contaminants is crucial for assessments of solute concentrations and their environmental effect on downstream recipients. Elevated concentration of nutrients and the presence of anthropogenic substances, such as pharmaceutical residues, are two examples of the current problems related to hydrological transport. The overall objective of this thesis is to increase the mechanistic understanding of the governing hydrological transport processes and their links to geomorphological and biogeochemical retention and attenuation processes. Specifically, this study aims to quantify the processes governing the transport and fate of waterborne contaminants on the point, stream reach, and watershed scales by evaluating time series obtained from stream tracer tests and water quality monitoring data. The process quantification was achieved by deriving formal expressions for the key transport characteristics, such as the central temporal moments of a unit solute response function and the spectral scaling function for time series of solute responses, which attributes the solute response in the Laplace and Fourier domains to the governing processes and spatial regions within the watershed. The results demonstrate that in addition to the hydrological and biogeochemical processes, the distribution of the load in the landscape and the geomorphological properties in terms of the distribution of transport pathway distances have defined effects on the solute response. Furthermore, the spatial variability between and along the transport pathways significantly affect the solute response. The results indicate that environments with high retention and attenuation intensity, such as stream-reaches with pronounced hyporheic zones, may often dominate the solute flux in the watershed effluent, especially for reactive solutes. The mechanistic-based framework along with the evaluation methodologies presented within this study describes how the results can be generalized in terms of model parameters that reflect the hydrology, geomorphology and biogeochemistry in the studied area. This procedure is demonstrated by the parameterization of a compartment-in-series model for phosphorous transport.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2014. , x, 62 p.
Series
TRITA-LWR. PHD, ISSN 1650-8602 ; 2014:05
Keyword [en]
Solute transport modeling; Transient storage; Tracer test; Central temporal moments; Spectral analysis; Parameterization
National Category
Oceanography, Hydrology, Water Resources
Identifiers
URN: urn:nbn:se:kth:diva-149528ISBN: 978-91-7595-232-1 (print)OAI: oai:DiVA.org:kth-149528DiVA: diva2:739901
Public defence
2014-09-12, F3, Lindstedtvägen 26, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20140826

Available from: 2014-08-26 Created: 2014-08-22 Last updated: 2015-06-15Bibliographically approved
List of papers
1. Response functions for in-stream solute transport in river networks
Open this publication in new window or tab >>Response functions for in-stream solute transport in river networks
2011 (English)In: Water resources research, ISSN 0043-1397, E-ISSN 1944-7973, Vol. 47, no W06502Article in journal (Refereed) Published
Abstract [en]

This paper analyzes the effects of different hydrological mechanisms on the solute response in watershed stream networks. Important processes are due to the hydraulic and chemical retention of reactive solutes in transient storage zones and the cumulative consequences of these processes from a single transport pathway as well as from the network of transport pathways. Temporal moments are derived for a distributed stream network and for a compartment-in-series model. The temporal moments are evaluated and are utilized to derive formal expressions for translating the network parameters into compartmental model parameters. The analysis reveals that in addition to the hydraulic and chemical retention processes, the morphological and topological properties of a watershed have a distinct impact on the central temporal moments in terms of averaging of the solute load weighted distances as well as the transport parameters over the network. Kinetic (rate-limited) transient storage affects second-order and higher central temporal moments and thus has a secondary effect on the parameterization of compartmental models. Additional considerable contributions to all temporal moments are introduced when parameter variability along transport pathways is considered. The paper demonstrates an improved model outcome for phosphorus transport in a small Swedish watershed by accounting for the overall network effects when parameterizing a compartment-in-series model.

Keyword
subsurface water exchange, transient storage model, hyporheic exchange, longitudinal dispersion, compartmental-models, hydrologic response, bed forms, zone, catchment, tracer
National Category
Water Engineering
Identifiers
urn:nbn:se:kth:diva-39185 (URN)10.1029/2010WR009412 (DOI)000291560500001 ()2-s2.0-79958138016 (Scopus ID)
Note

QC 20110908

Available from: 2011-09-08 Created: 2011-09-08 Last updated: 2017-12-08Bibliographically approved
2. Spectral scaling of heat fluxes in streambed sediments
Open this publication in new window or tab >>Spectral scaling of heat fluxes in streambed sediments
Show others...
2012 (English)In: Geophysical Research Letters, ISSN 0094-8276, E-ISSN 1944-8007, Vol. 39, no 23, L23402- p.Article in journal (Refereed) Published
Abstract [en]

Advancing our predictive capabilities of heat fluxes in streams and rivers is important because of the effects on ecology and the general use of heat fluxes as analogues for solute transport. Along these lines, we derived a closed-form solution that relates the in-stream temperature spectra to the responding temperature spectra at various depths in the sediment through a physical scaling factor including the effective thermal diffusivity and the Darcy flow velocity. This analysis considers the range of frequencies in temperature fluctuations that occur due to diurnal and meteorological variation both in the long and short term. This approach provides insight regarding the key frequencies for analysing temperature responses at different depths within the sediment and also provides a simple and accurate method that offers quantitative insight into heat transport and surface water interactions with groundwater. We demonstrate for Sava Brook, Sweden, how the values of effective thermal diffusivities can be estimated based on the observed in-stream and sediment temperature time series and explain the temporal scaling of the heat transport as a function of a dimensionless frequency number. We find that the lower limit of periods of significance for the analysis increases with depth, and we recommend further research regarding appropriate frequency windows.

Keyword
Temperature Time-Series, Tracer, Discharge, Exchange, Solutes
National Category
Geophysics
Identifiers
urn:nbn:se:kth:diva-109608 (URN)10.1029/2012GL053922 (DOI)000312094200002 ()2-s2.0-84870899209 (Scopus ID)
Funder
StandUp
Note

QC 20130108

Available from: 2013-01-08 Created: 2013-01-08 Last updated: 2017-12-06Bibliographically approved
3. Evaluating the fate of six common pharmaceuticals using a reactive transport model: Insights from a stream tracer test
Open this publication in new window or tab >>Evaluating the fate of six common pharmaceuticals using a reactive transport model: Insights from a stream tracer test
2013 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 458, 344-354 p.Article in journal (Refereed) Published
Abstract [en]

Quantitative information regarding the capacity of rivers to self-purify pharmaceutical residues is limited. To bridge this knowledge gap, we present a methodology for quantifying the governing processes affecting the fate of pharmaceuticals in streaming waters and, especially, to evaluate their relative significance for tracer observations. A tracer test in Sava Brook, Sweden was evaluated using a coupled physical-biogeochemical model framework containing surface water transport together with a representation of transient storage in slow/immobile zones of the stream, which are presumably important for the retention and attenuation of pharmaceuticals. To assess the key processes affecting the environmental fate of the compounds, we linked the uncertainty estimates of the reaction rate coefficients to the relative influence of transformation and sorption that occurred in different stream environments. The hydrological and biogeochemical contributions to the fate of the pharmaceuticals were decoupled, and the results indicate a moderate hydrological retention in the hyporheic zone as well as in the densely vegetated parts of the stream. Biogeochemical reactions in these transient storage zones further affected the fate of the pharmaceuticals, and we found that sorption was the key process for bezafibrate, metoprolol, and naproxen, while primary transformation was the most important process for clofibric acid and ibuprofen. Conversely, diclofenac was not affected by sorption or transformation.

Keyword
Pharmaceutical residues, Reactive transport modeling, Tracer test, Attenuation, Retention, Global sensitivity analysis
National Category
Oceanography, Hydrology, Water Resources
Identifiers
urn:nbn:se:kth:diva-124025 (URN)10.1016/j.scitotenv.2013.03.077 (DOI)000320901700039 ()23669580 (PubMedID)2-s2.0-84877815773 (Scopus ID)
Funder
Formas
Note

QC 20130813

Available from: 2013-06-25 Created: 2013-06-25 Last updated: 2017-12-06Bibliographically approved
4. Spatiotemporal decomposition of solute dispersion in watersheds
Open this publication in new window or tab >>Spatiotemporal decomposition of solute dispersion in watersheds
2015 (English)In: Water resources research, ISSN 0043-1397, E-ISSN 1944-7973, Vol. 51, no 4, 2377-2392 p.Article in journal (Refereed) Published
Abstract [en]

Information about the effect of different dispersion mechanisms on the solute response in watersheds is crucial for understanding the temporal dynamics of many water quality problems. However, to quantify these processes from stream water quality time series may be difficult because the governing mechanisms responsible for the concentration fluctuations span a wide range of temporal and spatial scales. In an attempt to address the quantification problem, we propose a novel methodology that includes a spectral decomposition of the watershed solute response using a distributed solute transport model for the network of transport pathways in surface and subsurface water. Closed form solutions of the transport problem in both the Laplace and Fourier domains are used to derive formal expressions of (i) the central temporal moments of a solute pulse response and (ii) the power spectral response of a solute concentration time series. By evaluating high-frequency hydrochemical data from the Upper Hafren Watershed, Wales, we linked the watershed dispersion mechanisms to the damping of the concentration fluctuations in different frequency intervals reflecting various environments responsible for the damping. The evaluation of the frequency-dependent model parameters indicate that the contribution of the different environments to the concentration fluctuations at the watershed effluent varies with period. For the longest periods (predominantly groundwater transport pathways) we found that the frequency typical transport time of chloride was 100 times longer and that sodium had a 2.5 times greater retardation factor compared with the shortest periods (predominantly shallow groundwater and surface water transport pathways).

Keyword
solute transport, watershed dispersion, transport network, modeling, spectral analysis, central temporal moments
National Category
Oceanography, Hydrology, Water Resources
Research subject
Land and Water Resources Engineering
Identifiers
urn:nbn:se:kth:diva-149531 (URN)10.1002/2014WR016385 (DOI)000354733500029 ()2-s2.0-84929624256 (Scopus ID)
Note

QC 20150615. Updated from manuscript to article in journal.

Available from: 2014-08-22 Created: 2014-08-22 Last updated: 2017-12-05Bibliographically approved

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