Karin Cederkvist a, *, Marina B. Jensen b, Peter E.

Holm a
a
Department of Plant and Environmental Sciences, Faculty of Science, University of Copenhagen, Thorvaldsensvej 40, 1871 Frederiksberg C, Denmark b Department
of Geosciences and Natural Resource Management, University of Copenhagen, Rolighedsvej 23, 1958 Frederiksberg C, Denmark

articleinfo abstract

Article history: Stormwater treatment facilities (STFs) are becoming increasingly widespread but knowledge on their performance is limited.
Received 31 October 2016 This is due to difficulties in obtaining representative samples during storm events and documenting removal of the broad range
Received in revised form of contaminants found in stormwater runoff. This paper presents a method to evaluate STFs by addition of synthetic runoff with
25 April 2017 representative concentrations of contaminant species, including the use of tracer for correction of removal rates for losses not
Accepted 29 April 2017 Available caused by the STF. A list of organic and inorganic contaminant species, including trace elements representative of runoff from
online 23 May 2017 roads is suggested, as well as relevant concentration ranges. The method was used for adding contaminants to three different
STFs including a curbstone extension with filter soil, a dual porosity filter, and six different permeable pavements. Evaluation
of the method showed that it is possible to add a well-defined mixture of contaminants despite different field conditions by
Keywords:
having a flexibly system, mixing different stock-solutions on site, and use bromide tracer for correction of outlet concentrations.
Road runoff
Field scale testing Bromide recovery ranged from only 12% in one of the permeable pavements to 97% in the dual porosity filter, stressing the
Curb extension importance of including a conservative tracer for correction of contaminant retention values. The method is considered useful
Filter soil in future treatment performance testing of STFs. The observed performance of the STFs is presented in coming papers.
Dual porosity filter © 2017 Elsevier Ltd. All rights reserved.
Permeable pavements

1. Introduction as emerging technologies specifically targeting stormwater runoff like dual

As a flexible response to climate change Sustainable Urban Drainage
Systems (SUDS) are increasingly being applied (Howe et al., 2012). SUDS
combine retention elements promoting infiltration and evaporation with
detention elements for slow discharge of water into local surface waters or
sewer systems. Due to content of contaminants in stormwater runoff,
especially runoff from trafficked surfaces, contamination of receiving water
bodies is a concern. As a consequence environmental authorities may require
removal of contaminants through treatment of the stormwater runoff prior to
infiltration or discharge. As also conventional practices of discharging runoff
into receiving waters may prevent achievement of the ecological standards
prescribed by the EU Water Frame Directive (Eriksson et al., 2007), a number
of stormwater runoff treatment facilities (STFs) are being considered,
including well known measures like wet and dry detention basins
* Corresponding author.
E-mail address: karince@plen.ku.dk (K. Cederkvist).
http://dx.doi.org/10.1016/j.jenvman.2017.04.097
0301-4797/© 2017 Elsevier Ltd. All rights reserved.
(Scholes et al., 2008) and newer measures like soil based infiltration in bioswales,
mulden rigolen, compost filters and filter soils (Ingvertsen et al., 2012), as well
porosity filtration (Jensen et al., 2011), or adaptation of well-known measures
such as disc filters and rotary filters (Nielsen et al., 2015).
Common for all STFs is the need for performance documentation (Grebel et
al., 2013). The obvious documentation based on monitoring of real stormwater
events is challenged by the unpredictable character of storm events as well as the
diverse and variable contaminant profile of stormwater runoff even at the same
site (Langeveld et al., 2012). A high number of samples are needed to provide a
statistical representative measure of variability in inlet concentrations, and a
wide range of compounds needs to be included in the chemical analytical
program due to the many contaminants that may potentially be present
(Langeveld et al., 2012). An alternative approach is to test STFs in dry weather
by adding a synthetic stormwater runoff solution to the inlet, in this way
obtaining independence of weather conditions and contaminant variability.
When using such a method, contaminants are discharged into the environment.
However, without a test it is difficult for authorities to approve STFs. Especially
some of the micro-pollutants, e.g. the pesticides, are only found sporadically,
making it hard to confirm, or disapprove, their removal. From this perspective it
is better to test them once under controlled conditions, than go ahead and install
a number of STFs with no documented effect.
The basic principle adopted for dry weather STF assessment is to relate
effluent concentrations, C, to influent concentrations, C0. As such the approach
is comparable to conventional lysimeter experiments for description of water and
substance transport through intact soil columns, (e.g. Wierenga and van
108 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117
Genuchten, 1989). Firstly, it is necessary to ensure addition of a well described
relevant contaminant influent, secondly, to ensure sufficient duration time for the
added influent to replace all antecedent water in the STF, and thirdly, to ensure
a proper sampling of both influent and effluent.
The influent addition period should ideally be long enough to cancel out
diffusion gradients between mobile water and any volumes of immobile water.
Strictly speaking this is only possible for STFs with an impermeable barrier
towards the surrounding environment. By inclusion of a conservative tracer, e.g.
bromide or tritiated water to the influent (Bowman, 1984) the loss of
contaminants caused by factors not related to the treatment process can be
accounted for. If the C/C0 ratio for the conservative tracer stays below 1 it
indicates that a fraction of the tracer has been lost, which may be due to diffusion
out of the STF-system, diffusion into immobile volumes of water trapped in the
STF (i.e. residual water), or intruding water diluting the added influent. The
fraction of nonrecovered tracer should be used to adjust contaminant removal
rates, as these substances will be subjected to a loss similar to that of the
conservative tracer, which cannot be ascribed to the STF per se.
Dry weather contaminant addition has been adopted in several cases, e.g.
Lloyd et al. (2001), Deletic and Fletcher (2006), and Hatt et al. (2009) but mainly
for evaluation of suspended solids and nutrients removal, largely omitting
organic and inorganic micropollutants as well as use of a conservative tracer.
When testing treatment capacity of an STF using a synthetic solution with
the aim to screen for a broad and relevant list of contaminants the number of
contaminants to choose among is high (Duncan, 1999; Eriksson et al., 2007;
Gobel et al., 2007; Ingvertsen€ et al., 2011; Zgheib et al., 2011; Grebel et al.,
2013). Three criteria should be considered when selecting contaminants; i)
likelihood of occurrence, ii) potential toxicological and/or ecotoxicological
effects on receiving water bodies, and iii) inclusion of heavy metals, metalloids
and organic compounds with different physicochemical properties.
According to international and Danish literature the compounds described
below seem relevant to address when assessing STFs.
As carriers of contaminants, suspended solids (SS) constitute an important
parameter in stormwater runoff (Ingvertsen et al., 2011; Zgheib et al., 2011).
Further, the solids per se turn the water turbid (Ingvertsen et al., 2011; Zgheib et
al., 2011). Since SS are ubiquitous in stormwater runoff their removal is easily
documented from ordinary monitoring programs (e.g. Li and Davis, 2008; Yu et
al., 2013).
Phosphorus (P) and nitrogen (N) may deteriorate aquatic ecosystems through
algae blooms (Egemose and Jensen, 2009). These nutrients are released from
organic matter associated with suspended solids, and may leach from lawns and
other fertile soil surfaces. Stormwater P and N are considered problematic in
many countries around the world, including United States and Australia (Taylor
et al., 2005; Collins et al., 2010; Davidson et al., 2010) as well as Denmark
(Sønderup et al., 2015).
Metals are ubiquitous in the environment and some of the most studied
pollutants in stormwater runoff, where they are ascribed to especially traffic
and roof materials. They can have a high toxicity, and tendency to accumulate
in organisms. Some of the metals most often detected in concentrations
exceeding threshold limits for drinking water and aquatic organisms are zinc
(Zn), lead (Pb), cadmium (Cd), nickel (Ni), copper (Cu), and chromium (Cr)
(Ingvertsen et al., 2011).
Like heavy metals, polyaromatic hydrocarbons (PAHs) are omnipresent in
stormwater runoff and the most intensively studied organic micro-pollutants.
Some PAHs are carcinogenic, can be toxic, and may accumulate in organisms.
PAHs are often found attached to suspended solids due to their generally high
Kow-values (Zgheib et al., 2011). Consequently, proper retention of suspended
solids secures retention of most PAHs. However the PAHs acenaphthene
(three rings), naphthalene (two rings) and phenanthrene (three rings) have
higher water solubility and may be found in dissolved form in stormwater
runoff (Ingvertsen et al., 2011; Kumata et al., 2006). Of these phenanthrene
seems to be the most abundant of the two three-ringed PAHs (Ingvertsen et
al., 2011; Kumata et al., 2006) and also naphthalene has a regular occurrence
(Ingvertsen et al., 2011; Kumata et al., 2006; Eriksson et al., 2007).
Another large group of organic micro-pollutants found in stormwater
runoff, though not as intensively studied, are detergents. Detergents have an
ecotoxicological effect on aquatic organisms and can impact the
biogeochemical cycle of other compounds by increasing solubility of metals
and oils (Okbah et al., 2013). In this group the anionic detergents are the most
widely used, in particular the linear alkylbenzene sulphonates (LAS)
(Mungray and Kumar, 2009), which are used in car wash soap, fabric
protectors, metal platings, fire-fighting foams, etc. (Rebello et al., 2013).
A third important group of organic micro-pollutants is pesticides
(Blanchoud et al., 2004). The types of pesticides that can be present in
stormwater vary and greatly depend on country, time of year, catchment land
use etc. According to sales lists, two of the most commonly used and found
pesticides in Denmark are the herbicides glyphosate and 2-methyl-4-
chlorophenoxyacetic acid (MCPA) (Nielsen et al., 2011, The Danish
Environmental Protection Agency, 2013, 2014). These two are reported
internationally to be found in other urban areas and glyphosate is the most
sold pesticide worldwide (Baylis, 2000; Blanchoud et al., 2004). MCPA is
highly mobile in soils (Hiller et al., 2006) and one of the most widespread
pesticides in terms of frequency of detection in rivers, lakes and groundwater,
also in Denmark (Nielsen et al., 2011). Glyphosate adsorbs more strongly to
soil, but is detected in high concentration levels in stormwater runoff (Tang et
al., 2015). Other frequently observed pesticides in stormwater runoff are the
herbicides mecoprop which has been documented in leachate from bitumen
membranes (Burkhardt et al., 2011; Bollmann et al., 2014), and diuron
(Blanchoud et al., 2004; Eriksson et al., 2007; Ingvertsen et al., 2011).
A fourth group of organic micro-pollutants is plasticizers of which
especially DEHP has been observed and considered problematic in
stormwater runoff (Birch et al., 2011; Clara et al., 2010).
In addition to above mentioned contaminants it is important to be aware of
emerging contaminants (Geissen et al., 2015).
Based on above considerations this paper presents a method for evaluating
STFs that targets removal of inorganic and organic micro-pollutants in
dissolved form. The specific objectives of the study were to i) suggest a
generally applicable contaminant addition method of synthetic runoff with
relevant concentrations of contaminant species, and ii) evaluate the
application of the method by testing it on three different STFs comprising a
curb extension with filter soil, a dual porosity filter with limestone, and six
types of permeable pavement systems. It should be noted that the contaminant
effluent concentrations of the tested STFs are not presented here.
2. Methods and materials
2.1. Stormwater treatment facilities
The contaminant addition method was tested on three STFs located in the
Municipality of Copenhagen (Fig. 1) in the period OctobereDecember 2014:
STF-I) a curb extension in a residential area, equipped with filter soil that
complies to German guidelines (Ingvertsen et al., 2012; Cederkvist et al.,
2016), STF-II) a dual porosity filter located in a park and receiving
stormwater runoff from residential roads after the water has passed a dry
detention pond (Cederkvist et al., 2010; Jensen et al., 2011), and STF-III) six
double car parking spots with different types of permeable pavements (PP),
see details in Table 1.
While filter soil and dual porosity filtration are developed for retention of
contaminants from stormwater runoff, permeable pavements are installed for
their hydraulic benefits. However, it has been found that permeable pavements
may work as STFs (Pratt et al., 1995; Dierkes et al., 2002; Brattebo and Booth,
2003; Drake et al., 2014).
As seen from Table 1 and Fig. 1, STF-I is an open system, losing water to the
soil surrounding the soakaway, and equipped with overflow to a sewer, while
STF-II and STF-III are systems enclosed by membranes preventing applied
water and solutes from escaping into surrounding soil or elsewhere. The STFs
have different porosities and water retention characteristics, affecting the mobile
water volumes, as estimated in Table 1. For filter soil in STF-I estimates are
 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117 109

based on a typical distribution of solids, air and water in agricultural soil

(Brouwer et al., 1985). For pre- and main filter in

Fig. 1. Cross-section of three STF tested. Full line arrows indicate flow patterns. Dotted arrows indicate sampling points. STF-I: Curb-extension. A ¼filter soil, B ¼ soakaway, shown with some water.

STF-II: Dual Porosity Filter. A ¼ pre-filter, B ¼ main filter. STF-III: Permeable Pavements. A ¼ permeable paving. B ¼ base layer. Cross sections of STF-I and STF-III are to scale in both vertical and

horizontal directions (1:50), while STF-II is to scale only in vertical direction (1:50). See Table 1 for further description.
Table 1
Details on the three STFs used for testing of dry weather contaminant addition method.
STF Curb extension with filter soil Dual porosity filter (DPF) Permeable pavements (PP)

Reference number STF-I STF-II STF-III

Location Moellebakken, Broenshoej Krogebjergparken, Vanloese Svanemoellehallen, Oesterbro

UTM-coordinates 5542016.8300N 5541049.7100N 5542052.0500N
1227044.7200E 1227050.7400E 1234042.7700E

Area of STF 18 m2 (L: 10 m, W: 1.8 m, D: 2 m) 30 m2 (L: 60 m, W: 0.5 m, D: 0.25 m) Six pavements of 25 m2 (L: 5 m, W: 5 m, D:
0,54 m)
Area of catchment attached 80 m2 of road 4000 m2 of road 25 m2 of car park per pavement
110 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117

Construction 0.4 m of filtersoil placed on top of a 1.6 m deep
soakaway stabilized with stormwater boxes. A
vertical pipe allows road runoff to enter the
soakaway directly in case of extreme events
causing ponding >0.15 m. The pipe also serves
as effluent sampling access. To ensure
emptying of the upper 1.3 m of the soakaway
a throttled outlet to the sewer is placed 0.3 m
above the bottom of the soakaway.
20 m long pre-filter followed by 40 m long main filter,
both containing 9 horizontal layers of DPF- plates with
6 mm high-flow layers for water transport and 10 mm
low-flow layers for contaminant accumulation. The
main filter is equipped with lime stone and ochreous
sludge as filter material in the low-flow layers. The
porosity of the lime stone is approximately 50%.
Different types of permeable paving on top of different
base layer materials, with a total depth of 54 cm.
PP1: paver with permeable joints on top of gravel with
fine fraction removed (2e32 mm) PP2: permeable
concrete paver on top of gravel with fine fraction
removed (2e32 mm) PP3: permeable asphalt paving on
top of gravel with fine fraction removed (2e32 mm)
PP4: permeable epoxy-stone paving on top of crushed
concrete (0e32 mm)
PP5: permeable epoxy-stone paving on top of crushed
stones (25e32 mm)
PP6: paver with permeable joints on top of crushed
stones (25e32 mm)

Normal flow of stormwater
runoff through STF
Vertical flow direction.
Gap in curb allows road runoff to enter. The
runoff distributes over the vegetated surface
and infiltrates the filtersoil. Leachate ponds in
stormwater boxes before infiltrating to
surrounding local soil. At 0.3 m leachate
overflow to sewer.
Horizontal flow direction.
Road runoff enters a dry detention basin lined with
bentonite, and flows from there at a constant flowrate of
0.5 m/s to the inlet chamber of the prefilter, further on
to the main filter, and from here to a local stream. After
rain, highflow layers drain completely, while lowflow
layers drain only half (5 mm remains water filled).
Effluent samples can be obtained from well between
pre- and main filter and from outlet well after main
filter.
Vertical flow direction.
Stormwater percolates the permeable pavement and
into the sub-base materials. A 2 cm elevated edge
prevents runoff from neighboring areas from entering.
All six pavements are individually sealed off with an
impermeable membrane, forming a ‘bath tub’,
connected to a well from where leachate is pumped with
a submersible pump to the sewer.
Effluent can be sampled from the well.

Total pore volume of 3.6, corresponding to 50% of the volume of the 4.0, distributed on 1.4 in pre-filter, 2.0 in main filter, and PP1: 4.22 (0.07 þ 4.15)
STF (m3) a filtersoil) 0.6 in pipes and well
PP2: 4.45 (0.30 þ 4.15)

PP3: 4.45 (0.38 þ 4.15)

PP4: 4.91 (0.54 þ 4.36)

Estimated mobile pore 1.8, corresponding to 50% of the porous volume 3.1, distributed on 1.0 in pre-filter: 1.5 in main filter, and PP5: 4.53 (0.54 þ 3.98)
volume (m3)b of filter soil 0.6 in pipes and wells: 0.6
PP6: 3.88 (0.07 þ 3.82)

PP1: 3.79 (0.06 þ 3.74)

PP2: 3.98 (0.24 þ 3.74)

PP3: 3.96 (0.23 þ 3.74)

PP4: 3.73 (0.43 þ 3.29)

PP5: 4.32 (0.43 þ 3.89)

PP6: 3.78 (0.06 þ 3.73)

a
For permeable pavements the volume distribution on paver and subbase is shown in parenthesis.
b Mobile pore volume for permeable pavements is calculated as difference between total pore volume and estimated retained water after 24 h of drainage (residual water).
STF-II the porous volume is calculated from manufacture data on bulk porosity
of filter material, while fractions of immobile water volumes are estimated. For
STF-III paving layers’ parameters are estimated and subbase parameters are
based on laboratory measurements (data not shown).
2.2. Composition and addition of synthetic runoff
The suggested synthetic road runoff (Table 2) encompasses all species
identified in the introduction, except a few. One nonincluded specie is N, since
the main concern in Denmark regarding nutrients is P since it is often the
limiting nutrient for algal growth and because excess P may accumulate in
bottom sediments to constitute a continuous internal source (Ingvertsen et al.,
2011). Diuron was also omitted as its use was recently banned in Denmark.
Since mecoprop and MCPA are chemically analogues (Werner et al., 2013),
MCPA was added as a model compound for both. It was not possible to add
DEHP, since it would sorb to the equipment used. Chromium was added as
Cr(VI) which is the more toxic form of Cr, to simulate a worst case scenario,
Table 2
Overview of added stock solutions, chemicals and container materials.
Stock solution no. Contaminant species Solvent and container material
and since the literature is scarce with information on chromium speciation in
stormwater runoff (Cederkvist, 2012).
To represent the PAHs acenaphthene, naphthalene and phenanthrene were
chosen, as these three are more likely to occur in dissolved state compared to
heavier PAHs found in stormwater runoff. The final list of contaminants thus
included Zn, Pb, Cd, Ni, Cu (all added as divalent cations), Cr (added as the
anion chromate Cr2O2-4 ), P (added as phosphate), linear alkylbenzene
sulphonates (LAS), acenaphthene, naphthalene, phenanthrene, glyphosate and
MCPA.
All compounds were added in dissolved form to mimic removal of non-
particulate contaminants. The concentration levels were chosen to represent
high, but still realistic situations (see e.g. Duncan, 1999; Gobel et al., 2007€ )
in this way the STF testing can be considered conservative. Targeted
concentrations can be seen in Table 4. Permission was granted by
environmental authorities. It should be noted that Cr was added solely as
Cr(VI), and that in some cases it may be necessary to collect the effluent or
divert it to the
Chemical used for stock solutions

#1 a
Pb (Pb )2þ
Deionized water 1000 mg Pb, (Pb(NO₃)₂ in H₂O) Titrisol®, Merck, Germany
Cationic metal solution Cd (Cd2þ) Polyethylene 1000 mg Cd, (CdCl₂ in H₂O) Titrisol®, Merck, Germany
Ni (Ni2þ) 1000 mg Ni, (NiCl₂ in H₂O) Titrisol®, Merck, Germany
 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117 111

Cu (Cu2þ) 1000 mg Cu, (CuCl₂ in H₂O) Titrisol®, Merck, Germany

Zn (Zn2þ) 1000 mg Zn (ZnCl2 in 0.06% HCl) Titrisol®, Merck, Germany

P (PO34) Phosphor 10.000 mg/L in H2O (from H3PO4) Certipur®, Merck, Germany

Br (Br) KBr, AnalaR NORMAPUR® analytical reagent VWR chemicals,

United States of America
#2b Cr(VI) (CrO2-4 ) Deionized water K2Cr2O7, MerckApplichem, Germany
Cr(VI) and detergent solution Linear alkylbenzene Polyethylene Linear alkylbenzenesulfonic acid, 97% Alfa Aesar, GmbH & Co, Germany
sulphonates

#3 Acenaphthene Methanol Acenaphthene 99%, Aldrich, United States

PAH-solution Naphthalene Borosilicate glass Naphthalene analytical standard, Fluka, Germany
Phenanthrene Phenanthrene 98%, Aldrich, United States

#4 Glyphosate Deionized water Glyphosate 98%, Dr Ehrenstorfer GmbH, Germany

Pesticide solution MCPA Borosilicate glass MCPA 98%, Dr Ehrenstorfer GmbH, Germany
a
For the first addition (STF-I, test 1) LAS were mixed into stock solution #1, which caused the LAS, Zn and Ni to precipitate and in the following mixtures LAS was instead
mixed into stock solution #2 with Cr(VI). b For the permeable pavements this stock solution was modified
to only contain Cr(VI).

Table 3
Overview of conditions for test of the contaminant addition method.

Replicate 1 2 1 2 1
Date of addition (all in 2014) Sept. 24 Dec. 15 Oct. 23 Dec. 17 Dec. 19
Volume applied (m3) 10.6 11 7.2 7.2 0.3
Duration of application (h) 5.9 6.1 3.9 4.6 1
Addition system Continuous mixing in small container Continuous mixing in small container Mixing in container from start
Source of dilution watera Hydrant Hydrant indoor tap
Applied stock solutions (Table 2) 1, 2, 3, 4 1, 2, 3, 4 1, 2
a
The water source has in all cases drinking water quality and origins from the public water supply system, which in Copenhagen is based on groundwater abstracted from lime stone aquifers.

Table 4
Contaminant target concentrations in synthetic runoff and observed influent concentrations. pH and suspended solids values are also included. The observed concentrations for both tests of STF-I and
second test of STF-II are presented jointly (average values with standard deviations in brackets). Likewise the observed concentrations for the six different pavements at STF-III are presented jointly.
Dissolved concentrations of metals are in italic.
Compound Target concentration after dilution Observed concentrationa STF-I and STF-II Observed concentrationa STF-III

pH neutral 7.9 (0.1) 8.1 (0.04)

Suspended solids [mg/L] 0 1.1 (0.4) 0.5 (0.1)
Br [𝜇g/L] 4500 3067 (208) 5250 (383)
Zn [𝜇g/L] 200 185.0 (7.1) 232 (7.5)
180.0 (0.0) 222 (7.5)

Pb [𝜇g/L] 20 18.3 (0.6) 15.5 (1.6)

9.6 (6.9) 9.1 (2.0)

Cd [𝜇g/L] 5 4.3 (0.4) 3.8 (0.1)

4.2 (0.4) 3.7 (0.1)

Ni [𝜇g/L] 20 18.0 (2.8) 26.5 (17.0)

16.5 (0.7) 18.2 (0.98)

Cu [𝜇g/L] 50 50.0 (4.6) 56.3 (4.2)

42.7 (2.1) 49.0 (13.7)

Cr(VI) [𝜇g/L] 20 25.3 (9.7) 19.2 (1.2)

22.0 (9.8) 15.7(2.3)
112 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117
P [𝜇g/L] 400
Linear alkylbenzensulphonates [𝜇g/L] 200
Acenaphthene [𝜇g/L] 1 0.9 (0.2)
Naphthalene [𝜇g/L] 1 0.8 (0.04)
Phenanthrene [𝜇g/L] 1 0.8 (0.18)
Glyphosate [𝜇g/L] 1 0.8 (0.04)
MCPA [mg/L] 1 1.0 (0.46)
a
In STF-I and STF-II n ¼ 3 for all the added contaminants, with the exception of Ni, Zn, LAS, where n ¼ 2, due to precipitation of Ni, Zn and LAS in STF-I test 1 (see note 1 of Table 2). In STF-III
n ¼ 6 for all the added contaminants.
sewer to avoid impacting surrounding environment.
For correction of contaminant removal not caused by the STF the
conservative tracer Br was added.
To prevent contaminants from adsorbing to surfaces of containers or
precipitating when mixed, four different stock solutions were prepared, and
diluted on site with a local water source (Table 2). All four stock solutions were
added to STF-I and STF-II, but due to budget constraints only stock solution #1
and #2 were added to STF-III.
2.3. Field procedure
All tests were performed under dry weather conditions. STF-I (curb
extension) and STF-II were tested twice, while STF-3 (six types of permeable
pavements) was tested once. For STF-I antecedent water in the soakaway was
pumped away prior to testing. STF-II (DPF) was fully drained on arrival. For
STF-III a 10.8 mm rain event the previous day was still seeping through the
pavements. The tests on STF-I and STF-II were repeated while the six individual
pavements of STF-III were tested only once.
2.3.1. Steady addition and influent sampling
Context dependent variables resulted in different addition systems, volumes
and durations being employed, see Table 3. The added volume should match at
least the estimated mobile pore volume to ensure sampling of added water rather
than antecedent water. Preferably the added volume should be even larger to
reduce the diffusion gradient between mobile water and non- or less mobile water
(residual water). A comparison with Table 1 shows that for STF-I and STF-II a
volume corresponding to four to six times the estimated mobile pore volume was
added. Added volumes to STF-III were limited to only 0.3 m3 due to practical
reasons of completing all six tests in one day. This is a low volume compared to
retained water volume in some of the pavements.
For STF-I and STF-II a 0.05 m3 open glass container (aquarium) was used for
diluting and mixing of the four stock solutions before addition. Water was in
both cases obtained from a hydrant (tapwater quality), equipped with a valve to
regulate flow rate. The aquarium was mounted on a wooden plate, which was
slightly tilted towards the inlet of the STF to allow influent to flow over the edge.
Stock solutions were pumped simultaneously into the aquarium with a multiple
head peristaltic dosing pump (Ismatec VP tubing pump). Turbulence from the
hydrant water ensured proper mixing as previously tested with a brilliant blue
solution mimicking stock solutions (results not shown). For STF-III the influent
to be applied was mixed in 0.8 m3 containers by filling the container
approximately 1/2 with water from indoor-tap, then adding stock solutions #1
and #2, and finally mixed in by further adding water to a total volume of 0.8 m3.
Influent was distributed over each of the 25 m2 pavements by manually moving
the container outlet hose in a systematic zig-zag pattern across the area.
For all three STFs influent flow rate and accumulated flow was measured with
a flowmeter (Brunata Optuna W Ø 25 mm) mounted on the hose after the
regulating valve. To catch any unintended variations influent sample (C0) was
composed of grab samples obtained every 20 min throughout the addition period.
A plastic jar was used to collect samples for heavy metals analysis and a glass
jar was used to collect samples for organic compounds analysis.
380.0 (10.0) 343 (29)
366.7 (20.8) 273(20)
135.0 (7.1) Not added
Not added
Not added
Not added
Not added
Not added
Any additions of contaminants from dilution water were acceptable since the
resulting influent (C0) was sampled immediately before addition to the STF.
Influent and effluent were analysed for pH and suspended solids. Suspended
solids were included to ensure that no were present in the influent and to see if
solids were released from the STFs into the effluent.
Bromide was analysed after ISO 10304-2 IC with a detection limit of 10
mg/L. The metals Pb, Cd, Ni, Cu, Zn and Cr were all analysed by ICP-MS
after method ISO 17294m:2005 with detection limits of 0.5 mg/L, 0.05 mg/L,
1 mg/L, 1 mg/L, 5 mg/L and 0.5 mg/L respectively. Phosphorus was
analysed by standard method (SM)17 version 4500-P (F) with a detection
limit of 0.005 mg/L. The linear alkylbenzene sulphonates were analysed after
Danish Standard 237, based on reaction with methylthioninium chloride and
absorbance measurements at 652 nm, with a detection limit of 0.03 mg/L. The
PAHs acenaphthene, naphthalene and phenanthrene were analysed by GC-
MS after M0250, all with a detection limit of 0.01 mg/L. Glyphosate was
analysed by LC-MS-MS after method M8270 with a detection limit of 0.01
mg/L. MCPA was analysed by GC-MS after method M2270 with a detection
limit of 0.01 mg/L.
2.3.2. Water volumes, electric conductivity and effluent sampling
For STF-I the response in effluent flow was monitored by measuring
increase in water level in the soakaway every 20 min with a simple folding
ruler. The increase in water level is not a direct measure of flow rate as a
fraction of the added water is constantly being infiltrated. Further, at water
depth exceeding 0.3 m the soakaway overflows to the sewer. For STF-II
effluent flow rate was measured with a flowmeter (Brunata Optuna W Ø 25
mm) mounted on the discharge pipe downstream of main filter. Apart from an
offset in time flow through the pre-filter is identical to the flow through the
main filter. For STF-III the discharge rate was calculated from observations
of water level increase in the monitoring well as registered with a pressure
transducer (HOBO® Water Level Logger) and compensating for non-measured
increases during pump-out time events by linear regression.
Electric conductivity (EC) of influent and effluent was monitored using a
field EC-meter (ECTestr, Waterproof Electrical Conductivity Meter Oakton).
It was observed that EC of the added influent was in all but one case (in STF-
III) higher than the EC of the first effluent from the STF. Thus, changes in
effluent EC were used as an on-site indicator of breakthrough of the applied
influent. For STF-I and STFII EC was frequently observed in influent and
effluent, while for STF-III it was measured less frequently due to time
constrains.
The effluent sample for tracer and contaminant analysis was obtained from
STF-I and STF-II when EC in the effluent stabilized at a maximum, and the
full planned volume of synthetic influent had been added. At this time
maximum water level in STF-I soakaway was reached as well as maximum
flow rate in STF-II. For STF-III effluent was sampled when discharge flow
rate was at maximum based on visual assessment of flow rate in discharge
well. The effluent sample was not composed of more grab samples as it was
assumed that complete mixing occurred in the STFs. As for sampling of
 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117
influent, a plastic jar was used for heavy metals analysis and a glass jar for
organic compounds analysis. All samples were collected in prescribed
containers, stored dark and cold and analysed within 24 h after sampling by
an accredited analytical company (results only showed for Br-).
3. Results and discussion
3.1. Observed influent concentrations versus target concentrations
In Table 4 observed concentrations in the composite influent samples from
the three STFs are shown together with target concentrations. As the same
addition system was used concentration data for STF-I and STF-II are merged
and presented jointly as average values with standard deviations. For the same
reason concentration data for the six individual pavements of STF-III are
merged. Due to pump failure data from the first test of STF-II are not included.
Because of practical constraints in the field only total concentrations of
organic micro-pollutants were analysed, since these were added in dissolved
form and due to the low concentration of SS it is assumed that they stayed in
dissolved form. Similarity in dissolved and total concentrations indicates that
most metals remained in the dissolved form, and only insignificant amounts
precipitated or sorbed to the glass of the influent dilution chamber (aquarium)
of STF-I and STF-II. Pb and P were observed in lower concentrations than
the targeted. Geochemical equilibrium calculations were applied to the water
samples using Visual Minteq version 3.0 (Gustafsson, 2013) determining
equilibrium solubility indices of the potential minerals/solid precipitates, and
indicated that solutions could be oversaturated with respect to minerals/
precipitates containing Pb, Cu, Ni and P. This could be the explanation for
the slightly lower observed concentration of some of the contaminants.
Mixing water originated from a water hydrant/tap and therefore had a high
content of Ca and Mg as is typical in groundwater in Eastern Denmark
(Marcussen et al., 2013). The fact that mixing water in all cases had a different
composition than typical stormwater runoff is not considered critical to the
test of the STFs as long as the added contaminants stay in solution. Impact of
a higher ionic strength of hydrant water is likely to enhance the sorption of
contaminants that form inner sphere complexes (McBride, 1994) and thus
make the test less conservative. This is however considered insignificant due
to the rather high influent contaminant concentrations.
No suspended solids were added, but small amounts in the influent were
still observed, possibly originating from mixing water or blown in dust during
the test.
The Br concentrations in STF-I and STF-II influent were below target
concentrations, and above target concentration in STF-III, possibly indicating
some error in the stock solution preparation. This error is not crucial for the
experiments, since the inlet concentration is known, making it still possible
to use Br for correction of contaminant effluent concentrations.
As seen from Table 4 the observed concentrations in the composite
influent sample for each test of STF overall compare well with target
concentrations, considering the large scale of field experiments and high
volume batches. It is concluded that both employed addition systems,
developed based on the considerations in the methods section, can be
recommended. The conditions simulated will in many cases be unusual for
the location, since the influent concentrations are in the high end of intervals
reported in the international literature, and since heavy metals are often found
attached to suspended solids. However, this approach is recommended to
ensure that the test simulates a worst case scenario and to make the test results
conservative.
Attention should be paid to potential precipitation due to interaction of
compounds and stock matrix as described for the first addition to STF-I. By
sampling influent for C0 determination after dilution and discharge from
mixing chamber any changes impaired on the influent in the field are ruled
out. While most of the employed contaminants are likely to represent a threat
to urban freshwater quality ubiquitously and for many decades to come it is
important to stay updated on some of the suggested contaminants, not least
113
the selection of pesticides, which may show significant local differences.
Attention must also be paid to emerging contaminants.
3.2. Effluent sampling time based on water volumes and electric
conductivity
When testing treatment performance of a STF effluent should be sampled at
worst case conditions. The time for sampling of effluent should ideally take
place when all mobile antecedent water of the system has been replaced with
added influent and when the water has the shortest retention time in the facility.
In these experiments this was verified in the field with EC/EC0-ratio and by
observing flow patterns, as shown in Fig. 2.
For the two tests of STF-I, 10 and 11 m3 of synthetic runoff was added during
5.9 and 6.1 h respectively (Table 3). Added influent was observed as increase in
water level in soak-away after approximately 30 min (Fig. 2). This increase is
not a direct measure of flow rate as a fraction of the added water is constantly
being infiltrated. The information was used to estimate when the retention time
of water in the trench was lowest. The water level reached maximum depth
(corresponding to overflow to sewer system) after approximately 3 h of influent
addition. Effluent was sampled after six hours.
For the two tests of STF-II, 7.2 m3 of synthetic runoff was added during 3.9
and 4.6 h. During test 1 (Fig. 2) the influent flow rate was slightly faster than for
test 2 (Fig. 2). For STF-II first effluent from the pre-filter was observed after
approximately 45 min (data not shown) and from the main filter after
approximately 1 h. In both tests maximum flow was observed after
approximately 2.5 h and corresponded to influent addition rate. Sampling of
effluent happened after the filter had been running full for more than 2 h.
All six pavements in STF-III were subjected to 0.3 m3 of influent during 1 h
corresponding to a rain event of 12 mm. Consequently effluent sampling was in
the case of STF-III based more on water discharge rate meaning that effluent was
sampled after addition of full influent volume and when effluent discharge rate
was visually considered no longer to increase. From Fig. 2 it is observed, that
even though subjected to the same water volume, the drainage pattern from the
six plots, are very different due to both the different pavements and base-course
materials. Effluent sampling times varied markedly.
The use of EC as an indicator for tracking movement of the added synthetic
runoff was possible for STF-I and STF-II as clear differences were observed in
EC of added influent versus EC of first effluent discharged. EC of the influent
was in the range of 800e1000 mS/cm, while EC of the antecedent water and thus
first effluent of the STFs was lower, reflecting stormwater runoff. According to
previous measurements, stormwater runoff in the area has EC in the range of
70e130 mS/cm. As seen from Fig. 2 main increase in EC of effluent of STF-I
and STF-II reflects main increase in water flow, where after EC gradually
increases to a more or less steady level. This shows that EC of the effluent is
dominated by EC of the added influent, but also affected to various degrees by
specific flow patterns of individual STF, i.e. exchange of solutes between mobile
water and non-mobile water trapped in the STFs, and in case of the non-sealed
STF-I also the surrounding soil. Similar patterns can be recognized for STF-III,
but since testing of the six pavements was conducted simultaneously EC-
measurements were fewer than for STF-I and STF-II. For PP 4 of STF-III, EC
of the effluent was much higher than the influent, apparently due to salts released
from the subbase materials (Table 1).
The sampling of effluent from STF-I took place after all planned influent
volume had been added, equivalent to more than 5 times the estimated mobile
water volume (Tables 1 and 3). At this time effluent EC was still significantly
lower than influent EC, due to antecedent non-mobile and surrounding soil water
acting as a sink for added solutes, but the ratio had in test 1 and test 2 reached a
steady level around 0.8 and 0.6 respectively (Fig. 2). It is therefore assumed that
effluent samples were taken at appropriate times.
114 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117

The STF-II effluent was sampled when all planned influent had been added, For STF-III EC measurements were less useful, because the difference between
corresponding to 4e5 times replacement of estimated mobile water volume EC of effluent and influent were not in all cases significant, and because of few

Fig. 2. Field observations of effluent water flow and EC measurements for the three STFs. The effluent sampling time is marked with a vertical dotted line. For STF-II: only one discharge rate is shown,
since it is the same for pre-filter and main filter. The grey curve shows EC/EC0 for the pre-filter, the black curve for the main filter. For STF-II test 1 the first dotted line shows sampling from pre-filter,
the second dotted line for main filter. In test 2 samples were taken at the same time.
(Tables 1 and 3). At this time EC of the effluent from the main filter had almost measurements due to practical constraints. The time of effluent sampling was
reached the level of influent with a ratio of 0.97 in both tests. For STF-II EC based on visual estimates of maximum increase in discharge rates. When
measurements provided strong support for the decision of effluent sampling time, comparing rates with recordings of former rain events maximum flow seemed
as the curves developed clearly throughout the experiments, reflecting only little to have been reached. Effluent samples from PP1, 3, 5 and 6 (Fig. 2) were taken
non-mobile water and little exchange of ions between added synthetic runoff and when discharge rate was at maximum and steady for a while. Contrarily the
materials in the STF. In this case ECmeasurements could have replaced addition sampling from PP2 and 4 was taken when discharge rate had decreased
of bromide tracer (Fig. 2). When comparing discharge rates and EC/EC0-ratios significantly. For PP2 this may be due to a lack of attention, while for PP4 it
with sampling time (dotted line) at STF-II, it is observed that the samples after was difficult to visually observe a maximum flow due to only small changes in
both pre- and main filter are taken at highest flowrate. effluent flow rate. Thus for PP2 and 4 the effluent sample is not representing
water with shortest retention time.
 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117
3.3. Bromide correction factor
Despite addition of large influent volumes, some 30e52% of Br added to
STF-I test 1 and 2 did not reappear in the effluent (Table 5). Goldberg and
Kabengi (2010) suggest that mineralogy should carefully be evaluated before
assuming that Br can be applied as a conservative tracer since they observed
a specific inner-sphere sorption to Al- and Fe-oxides at pH-values below 7.
However, pH of effluent in STF-I was 7.9 (Table 4) and therefore significant
losses of Br in STF-I due to sorption seem unlikely. This indicates that Br is
subjected to significant diffusion gradients causing a loss of Br from the
mobile water into non-mobile water (Lloyd et al., 2001). While the diffusion
gradient between mobile and stagnant water in the filter soil could eventually
be levelled out the loss into surrounding soil will be continuous and prevent
bromide (and EC) level in the effluent from ever reaching influent level. As
all added solutes are subjected to similar diffusion losses as the non-reactive
bromide tracer observed effluent concentrations must be corrected as this loss
cannot be ascribed to a removal of the solute from the water phase. In worst
case this apparent loss may be overestimated, in that the contaminant may
travel back into mobile water volumes once the diffusion gradient changes
direction due to inflow of stormwater runoff with a lower content. It is also
possible that a portion of the solutes lost by diffusion will react with the soil
and thus be removed from the water, in which case the correction may be too
conservative, but this is unknown.
For STF-II only Br in test 2 was analysed. Here a Br/Br0-ratio close to 1
was obtained (Table 5), reflecting a system with limited volume and large
surfaces of immobile water, and no exchange of matter with surrounding soil.
With a loss of conservative tracer in the order of only 3%, the removal rates
of other added solutes hardly need correction. The almost full breakthrough
of bromide is in accordance with observations of EC (Fig. 2).
The Br/Br0 ratios found for STF-III at the time of sampling differed
significantly among pavements, with recoveries ranging from 12 to 52%, and
were in all cases rather low (Table 5). For reasons described in section 2.3.1
only 0.3 m3 of influent was applied per pavement, corresponding to less than
10% of the estimated mobile pore volume (Table 1). In consequence the
resulting effluent concentrations all need significant corrections based on the
Br/Br0 ratio.
To better understand the low recovery of Br in effluent from STF-III the
total amount of antecedent water in each of the six pavements was estimated
based on retained water (difference between total porosity and mobile water
in Table 1) plus water from a 10.8 mm storm event the day before that was
not fully drained at the time of conducting the experiment (based on
registrations of discharge volumes). Plotting observed Br/Br0 ratios against
antecedent water volumes gave a correlation of R2 ¼ 0.83 (Fig. 3). This rather
high correlation indicates that most of the variation in Br/
Table 5
Effluent levels of tracers compared to influent levels at time of effluent sampling. Observed
Br/Br0 ratios are to be used for correction of removal rates of contaminants added in dissolved
form.
STF-I STF-II
Test 1 0.70 pre-filter: not meas. main
filter: not meas.
Test 2 0.48 pre-filter: 0.97 main
filter: 0.97
115
Fig. 3. Br/Br0 ratio plotted against water content in the six permeable pavements (PP) of STF-III.
Br0-ratios is explained by differences in antecedent water content and underlines
the importance of including a conservative tracer in such experiments. As
mentioned previously effluent samples from PP2 and 4 where not taken when
effluent flow peaked and could thus be connected with some uncertainty,
however when looking at Fig. 3 the two pavements fit well with the correlation.
The remaining differences may be explained by differences in flow patterns with
more or less preferential flow.
The Br/Br0 ratio should be used to adjust the removal rate of an added
contaminant by reducing influent concentrations with the ratio. Thus, if the
observed Br/Br0 ratio is 0.7 influent concentration of all added solutes should be
reduced to 70% before comparison is made with effluent concentrations. The
logic is that if there was no effect of the STF the solute would be reduced to the
same degree as the non-reactive tracer. Only an additional reduction in
concentration can be ascribed to the STF per se. By employing the correction
factor the test becomes conservative, in that it must be assumed that some of the
contaminants lost due to diffusion would never diffuse back to mobile water, but
be removed by sorption or degradation in the matrix around the immobile water.
4. Conclusion
Based on three field experiments it is concluded that the developed method
for assessment of stormwater treatment facilities with synthetic road runoff can
be applied to test the facilities in a well-defined way in dry weather, thus
providing a test method that is independent of rain events. By use of different
stock solutions a broad spectrum of carefully selected potential stormwater
contaminants including organic micro-pollutants in different concentration
ranges and with different physical and chemical properties can be added in
dissolved form simultaneously. In all three test-cases most added contaminants
reached the influent target concentrations and with low standard deviations,
despite large volumes of water and variable field conditions.
The use of EC/EC0 for in-field observation of full replacement of all
antecedent mobile water with applied influent worked well for STF-I curb
STF-III extension and STF-II dual porosity filter, but not for STFIII permeable
pavements where added water volume was small compared with the volume of
PP1: 0.44 antecedent water, and where subbase materials in some cases released salts,
PP2: 0.37 resulting in a high EC already of the first effluent samples, masking breakthrough
PP3: 0.22 of added influent. The aim was to test the facilities under most critical conditions,
PP4: 0.12 i.e. shortest residence time of the water, and with replacement of all antecedent
PP5: 0.52 water with incoming water, but still under considerations to practical
PP6: 0.49
possibilities.
STF performance at maximum flow rate was reached for STF-II where
effluent flow rate corresponded to maximum flow for the dual porosity filter, and
for STF-III where the maximum flow in most, but not all, cases seemed to have
been reached by comparison with recordings of previous rain events. For STF-I
maximum flow rate may have been reached as indicated by steady rise in water
level in soakaway, but overflow to sewer system at 0.3 m height interrupted
further flow indications based on water level rise. This indicates that knowledge
116 K. Cederkvist et al. / Journal of Environmental Management 198 (2017) 107e117
of STFs hydraulic performance can be an advantage when testing STF treatment
capabilities.
A core finding from testing this dry weather contaminant addition method
was the importance of including a conservative tracer that can be used to measure
the possible loss of contaminants due to diffusion of contaminants into non-
mobile water volumes of the STF. The addition of a conservative tracer allow for
adjusting observed effluent concentrations of reactive contaminants for losses
caused by diffusion. Having said this it should also be stressed that by employing
the correction factor the test becomes conservative, in that it must be assumed
that some of the added contaminants lost due to diffusion would never diffuse
back to mobile water, but be removed by sorption or degradation in the matrix
holding the immobile water.
Acknowledgements
The authors wish to thank several people that have assisted in the laboratory,
field and with data processing, namely Per Bjerager, Anita Schjødt Sandager, Jan
Støvring, Mikkel Priess and Preben Frederiksen. Furthermore we wish to thank
Ann-Charlott Eriksen for illustrations of Fig. 1 and Mark Taylor Randall for
proofreading the manuscript.
Data presented in this paper was generated as part of the project ‘Cities in
Water Balance’ financed by The Danish Council for Technology and Innovation,
performed in collaboration with Danish Technological Institute. Several partners
have contributed with their expertise, materials and additional funding and we
wish to thank HOFOR A/S, Aarhus Vand, Municipalities of Copenhagen and
Aarhus, Aarsleff A/S, Wavin and Orbicon.
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