Water Air Soil Pollut (2015) 226:399

DOI 10.1007/s11270-015-2657-2

Assessment of Distinctive Road Runoff Quality in Coastal

Areas, Based on a Monitoring Case Study
Pedro Antunes & Paulo J. Ramísio

Received: 10 August 2015 / Accepted: 21 October 2015

# Springer International Publishing Switzerland 2015

Abstract High levels of marine salt deposition present of the antecedent dry period prior to each rainfall event
in coastal areas have a relevant effect on road runoff and the average wind speed.
characteristics. This study assesses this effect with the
purpose of identifying the relationships between moni- Keywords Coastal areas . Exploratory statistical data
tored water quality parameters and intrinsic site vari- analysis . Monitoring . Road runoff . Salt deposition
ables. To achieve this objective, an extensive monitoring
program was conducted on a Portuguese coastal high-
way. The study included 30 rainfall events, in different
1 Introduction
weather, traffic, and salt deposition conditions. The
evaluations of various water quality parameters were
Road runoff is a linear source of diffuse pollution that
carried out in over 200 samples. In addition, the mete-
can cause significant environmental impacts (Luker and
orological, hydrological, and traffic parameters were
Montague 1994; Kayhanian et al. 2007; Crabtree et al.
continuously measured. The salt deposition rates were
2008; Opher and Friedler 2010). The pollutants result
determined by means of a wet candle device, which is an
from stationary and mobile sources. Stationary sources
innovative feature of the monitoring program. The rela-
include the erosion of embankments and the degradation
tion between road runoff pollutants and independent
of the road platform and urban infrastructures. Mobile
variables associated with weather, traffic, and salt depo-
sources are associated with road traffic (including tire
sition conditions was assessed. Significant correlations
and brake wear, oil and fuel leakages, deterioration of
among pollutants were observed. A high salinity con-
coatings, and fuel emissions) and with the transport
centration and its influence on the road runoff were
deposition of airborne pollutants (Hvitved-Jacobsen
confirmed. Furthermore, the concentrations of the most
and Vollertsen 2005). Road conservation operations,
relevant pollutants seemed to be very dependent on
the application of pesticides and fertilizers, and litter
some meteorological variables, particularly the duration
may also contribute to this type of pollution (Sansalone
and Buchberger 1997). In particular, Pio et al. (1996)
reported that Portuguese coastal areas have significant
P. Antunes (*) inputs of marine aerosols, with a very significant impact
Higher School of Technology and Management of the Polytechnic on air quality, due to the regime of dominant westerly
Institute of Viseu, Campus Politécnico, 3504-510 Viseu, Portugal (Atlantic) winds. During rainfall events, these pollutants
e-mail: baila@estgv.ipv.pt are leached to the resulting runoff.
P. J. Ramísio It is very complex to evaluate the influence of the
Department of Civil Engineering, School of Engineering, different site variables on the road runoff pollutant con-
University of Minho, 4710-057 Braga, Portugal centrations since there are no direct correlations between
399 Page 2 of 17
the runoff quality and the road characteristics, specifi-
cally the average daily traffic, the amount of precipita-
tion, the road maintenance practices, or the surrounding
land use (Smullen et al. 1999; Opher and Friedler 2010).
Previous researches (Antunes and Barbosa 2005;
Barbosa et al. 2006), based on two different monitoring
sites located on Portuguese coastal areas (highways A25
and IP6), have detected high levels of salinity, chlorides,
and chemical oxygen demand (COD). On the other
hand, typical pollutants for road runoff characterization,
such as suspended solids (TSS) and heavy metals, clear-
ly indicated different patterns of pollution. Such evi-
dences have been attributed to the proximity of the
Atlantic Ocean since non-coastal Portuguese roads did
not exhibit this pattern (Barbosa et al. 2006).
In coastal areas, maritime salts transported by the at-
mosphere are deposited on the road pavement, a phenom-
enon that may increase the risk of environmental pollution.
The salt crystallization at the surface promotes a higher
degradation of the road pavement (Woodbridge et al.
1994), with relevant structural consequences. The bitumi-
nous adhesion to the aggregate base decreases and, with
the permanent erosion resulting from vehicle movement,
small particles are released. The first reference to this
matter in international literature appears to be Antunes
and Barbosa (2005). Until then, studies that focused on
the effect of salinity in road runoff were associated to road
sites where deicing salts (sodium chloride and calcium
magnesium acetate) were applied in winter (Stotz and
Krauth 1994; Bäckström et al. 2004; Opher and Friedler
2010; Merrikhpour and Jalali 2013). The latter is a differ-
ent process, with considerable seasonal differences in the
average and median chloride concentration.
The deposition of thawing salts can also have a
significant impact on road runoff. This occurs not only
due to the high salinity input to the environment but also
due to an increased concentration of heavy metals (pres-
ent in the deicing agents) and a change in their specia-
tion, leading to higher mobility, due to their solubiliza-
tion (Bäckström et al. 2004). Stotz and Krauth (1994)
and Amini and Tehrani (2012) stated a possible physical
or structural impact due to the presence of salts in
pervious pavements: significant concentrations of calci-
um and sulfate ions that can combine with other sub-
stances form mortar-like materials.
The problem related to coastal roads (free of deicing
salts) shows different features and patterns. In coastal
areas, salts remain on the pavement and crystallize
during a long dry period (up to three months), which is
Water Air Soil Pollut (2015) 226:399
likely to change the runoff quality and have, as well, an
effect on the pavement structure itself.
Figure 1 presents the major processes associated with
salt deposition and road runoff quality in coastal areas.
The present study was included in the research pro-
ject BGuidelines for Integrated Road Runoff Pollution
Management in Portugal (G-Terra),^ a 3-year study
(2008 to 2011) funded by the Portuguese Foundation
for Science and Technology (Barbosa et al. 2011). This
project had two main objectives: to provide a consistent
answer to the question Bwhat are the particular charac-
teristics of road runoff in coastal areas?^ and to establish
a conceptual model for coastal road pollutants.
2 Materials and Methods
2.1 Characterization of the Study Area
The monitored section of the A25 highway, with two
lanes in each direction, is located less than 6 km from
and 5 m above a coastal lagoon (Ria de Aveiro), which
communicates with the Atlantic Ocean. The low eleva-
tion and the absence of constructed barriers between the
monitored site and the ocean potentiate the wind action
and the salt deposition effect (Fitzgerald 1991; Morcillo
et al. 2000). The dominant winds are from the SE
(autumn-winter) and the NW (spring-summer), with an
average speed of 9.2 m/s (TMUA 2014). The site is
located near the city of Aveiro, with about 80,000 in-
habitants. Other surrounding land uses include a sea
port, some industry, and agriculture activities.
Based on the traffic meter installed in the monitored
section, the average daily traffic during the monitoring
period varied between 31,779 and 33,830 vehicles/day.
This region is classified as ecologically sensitive by
the Portuguese law (decree law 384-B/99, 23rd of Sep-
tember). The mandatory environmental impact study for
this project recommended the construction of a runoff
treatment system, which was never implemented
(Mesoplano et al. 1994).
Table 1 presents the main characteristics of the case
study site, and Fig. 2 depicts the location of the A25
highway.
2.2 Monitoring Station
In February 2008, an automated battery-powered mon-
itoring station was installed at the case study site. It
Water Air Soil Pollut (2015) 226:399
Fig. 1 Major processes involved
in salt deposition and associated
road runoff in coastal areas
consisted of a rain gauge, a flow meter (ISCO 730
Bubbler Flow Module) with a Thel-Mar volumetric
weir, and an automatic water sampler (ISCO 6700),
working in synchronization, as is common in this type
of research (Ramísio and Vieira 2011). A schematic
diagram of the monitoring system is shown in Fig. 3.
From February 2008 to April 2011, three monitoring
campaigns were completed, comprising 30 different
rainfall events and 215 discrete runoff samples. These
samples were collected in different seasons, climatic
conditions, salt deposition rates, and traffic conditions.
At each event, the sampling routine was triggered
either by the precipitation height on the rain gauge or
by the runoff flow (the latter being the most frequent).
Eight discrete samples, or less in short-duration rainfall
events, were collected in borosilicate glass bottles (2 L
Table 1 Main characteristics of the case study at the A25 highway
Location
Distance to the Atlantic Ocean
Monitored catchment area
Characteristics of researched road section
Annual average daily traffic
Average annual rainfall
Other site relevant characteristics
Page 3 of 17 399
each). The monitoring program, with a total time of 2 h,
had an initial time interval of 10 min, which was in-
creased to 20 min after the third sample was collected.
This larger interval allowed a more accurate characteri-
zation of the initial runoff, in order to assess the occur-
rence of the first flush phenomena (Gupta and Saul 1996;
Furumai et al. 2002; Kayhanian et al. 2012), where water
pollution tends to be more concentrated when compared
with the remainder of the remnant runoff, particularly for
long antecedent dry periods (ADP).
To monitor a rainfall event, a minimum inter-event
time (which leads to ADP) of 6 h was adopted to
guarantee the independence between events, as sug-
gested by Dunkerley (2008).
One of the innovations concerning road runoff mon-
itoring was the addition of a wet candle device (placed
Geographic coordinates: 40° 37′ 57.64″ N; 8° 40′ 58.14″ W
5.6 km
287.5 m2 (totally impervious, asphalt concrete pavement)
Bitumen asphalt pavement (New Jersey reinforced
concrete) with prefabricated 0.8 m height safety barriers
Low longitudinal slope
2.5 % cross slope
11.5 m width (one direction with two lanes)
31,779 vehicles (2008); 32,765 (2009); 33,830 (2010);
in the summer months, traffic increases 40 % due to
accesses to nearby beaches
916 mm
The highway crosses an ecologically sensitive coastal
lagoon, with high salinity
399 Page 4 of 17
Fig. 2 Location and satellite view of the study area: 1—Atlantic Ocean, 2—A25 highway, 3—site location, 4—meteorological station
on top of the shelter, as shown in Fig. 3) to determine the
salt deposition rate (SDR)—amount of atmospheric
chloride salts deposited in a given area, per unit time,
according to the ASTM standard G-240 (ASTM 2002).
In the framework of the present research, the SDR data
was collected monthly.
There was a second wet candle device at a weather
station located at the University of Aveiro, approximately
Fig. 3 Schematic diagram of the
monitoring system
Water Air Soil Pollut (2015) 226:399
2 km east of the A25 monitoring section (see Fig. 2). The
continuous meteorological and atmospheric data provid-
ed by this weather station contributed to investigate the
transport of air masses and salt deposition variables rel-
evant to this research.
For the monitoring site and research period, a numer-
ical model from the European Centre for Medium-Range
Weather Forecasts (ECMWF) provided the sea data.
Water Air Soil Pollut (2015) 226:399
2.3 Measured Parameters and Analytical Methods
The performed sampling, preparation, preservation, and
analytical procedures followed the international stan-
dard procedures, including an adequate quality assur-
ance and quality control (QA/QC) plan established for
the G-Terra Project, based on Caltrans (2003) and
APHA (1998).
The 20 quality parameters analyzed for the road
runoff characterization were divided into the following
six groups:
– Physicochemical in situ determinations (immediate-
ly after sampling): temperature (Temp), pH, con-
ductivity (Cond), salinity (Sal), and turbidity (Turb)
– Solids: total suspended solids (TSS)
– Inorganic chemicals: hardness (Hard) and chlorides
(Cl−)
– Nutrients: Kjeldahl nitrogen (TKN) and total phos-
phorus (P)
– Aggregated organics: biochemical oxygen demand
(BOD5), chemical oxygen demand (COD), total
organic carbon (TOC), oil and grease (O&G)
– Heavy metals: total contents of Fe, Zn, Cu, and Pb
The water quality parameters and the considered
analytical methods are shown in Table 2.
2.4 Data Treatment
Given the variability within and among rainfall
events, it is important to find the proper treatment
of concentrations in discrete samples of the road
runoff and to establish reliable and comparable
definitions of the water quality parameters for road
runoff characterization, in order to evaluate envi-
ronmental impacts and establishing mitigation mea-
sures and treatments.
Thus, to overcome the runoff concentration var-
iability during each rainfall event, the event mean
concentration (EMC) was considered, representing
the average concentration of a specific analytical
parameter in an event, weighted by the runoff vol-
ume. EMC is therefore defined as the ratio between
the pollutant load during an event at a specific site
and the volume of the road runoff discharged dur-
ing that rainfall event (Smullen et al. 1999;
Ramísio 2007).
Page 5 of 17 399
M ∫C ðt ÞQðt Þdt
EMC ¼ ¼
V ∫Qðt Þdt
where
C(t) represents the pollutant mass concentration as a
function of time
Q(t) represents the runoff flow as a function of time
The site mean concentration (SMC) of a specific
analytical parameter represents the average of several
EMC in the monitored events. The site average pollutant
loads can be estimated by multiplying the SMC of each
pollutant by the runoff volume during a given period.
Pollutant concentrations frequently decrease over
time, which tends to create greater emission rates at
the beginning of the runoff—a phenomenon often called
a first flush.
According to Gupta and Saul (1996), a first flush
occurs when the slope of the normalized cumulative
pollutant mass emission plotted against the normalized
cumulative runoff volume is greater than 45 %. Alter-
natively, Bertrand-Krajewski et al. (1998) defined the
occurrence of a first flush when at least 80 % of the
pollutant load is emitted in the first 30 % of the runoff
volume.
A third possibility, and quite an effective method for
evaluating the first flush occurrence and extension, is to
plot the percentage of pollutant transport (in terms of
accumulated pollutant load) versus the cumulative vol-
ume of road runoff, as depicted in Fig. 4. If the slope
variation of this curve is negative, such as pollutant Y in
the figure, there is a first flush; otherwise, such as
pollutant X in the figure, there is not a first flush. This
was the adopted criterion in the present study.
For each pollutant, descriptive statistics parameters
were computed to address the distribution and charac-
teristics of the road runoff quality, including information
such as the number of data, percentage of detected data,
minimum and maximum detected values, mean, and
standard deviation.
As usual in road runoff quality parameters, EMC
were found to be generally better represented by a
lognormal distribution (FHWA 1996; Hvitved-
Jacobsen and Yousef 1991; Smullen et al. 1999). For
each pollutant, the normality of the distributions was
evaluated (skewness and excess kurtosis cannot be close
to zero) prior to performing additional data analyses.
Pollutant with concentrations below the detection limit
were reported as non-detects (ND). The ND may
399 Page 6 of 17 Water Air Soil Pollut (2015) 226:399

Table 2 Water quality parameters and analytical methods

Parameters Units Analytical method Preservation, Validitye Volume min. DL QL Controlsf Accuracyg Precisionh
extra <4 °C (mL)

Temp °C – a
– – – – – – –
pH Sørensen scale Electrometric a
0.25 h – – – – – –
Cond μS/cm Electrometric a
– – 0.1 0.3 – – –
Turb NTU – – – – – – – – –
TSS mg/L (APHA) – 7d 200 1.5 5 B,D – 20
2540 D
Cl− mg Cl/L (APHA) 4500Cl B – 28 d 50 1.3 4.3 B,S,D,V 80–120 20
Hard mg CaCO3/L (APHA) d
6M 50 B,D – 20
2340 C
Sal mg/L Electrometric a
– – – – – – –
TOC mg/L EN 1484 b
7d 100 0.5 1 – – –
b
COD mg O2/L (APHA) 28 d 50 3.3 10 B,S,D,V 80–120 20
5220 B
BOD5 mg O2/L (APHA) – 24 h 500 2 5 B,S,D 80–120 20
5210 B
O&G mg /L EPA 413.2 c
28 d 1000 0.1 0.2 B,S,V 80–120 –
b
TKN mg N/L (APHA) 4500Norg.B 28 d 50 0.2 0.7 B,S,D 80–120 20
b
Total P mg P/L (APHA) 4500P E 28 d 50 0.05 0.16 B,S,D,V 80–120 20
Total Fe mg/L (APHA) – – – 0.129 0.395 B,S,D,V 85–115 20
3111 B
Total Zn mg/L (APHA) – – – 0.026 0.081 B,S,D,V 85–115 20
3111 B
Total Cu mg/L (APHA) – – – 0.005 0.015 B,S,D,V – 20
3111 B
d
Total Pb mg/L (APHA) 6M 100 0.006 0.018 B,P,D,V 85–115 20
3113 B
a
In situ analysis
b
H2SO4 addition to pH <2
c
HCl addition to pH <2
d
HNO3 addition to pH <2
e
Validity: maximum time interval between the end of sampling and analysis; units in hours (h), days (d), and months (M)
f
Controls completed, one per event or lot of samples: blanc method (B), standard monitoring (S), duplicate sample (D), calibration
verification (V)
g
Acceptance accuracy limits for the recovery obtained in the control pattern (S) (APHA 1998)
h
Acceptance precision limits for duplicates (%)

provide potentially useful information in descriptive
statistics. In the present study, a method commonly used
to consider non-detects, regression on order statistics
(ROS), was applied with the adaptations suggested by
Shumway et al. (2002).
Data concerning the various monitored rainfall
events was collected and processed, as summarized in
Table 3.
2.5 Multivariate Statistical Analysis
A better understanding of the correlation among the
main constituents in highway runoff may reduce the
huge costs associated with monitoring (Thomson et al.
1997) and provide knowledge that may contribute to the
future modeling of these processes. An exploratory data
analysis was therefore conducted with different statisti-
cal techniques, including determination of Pearson co-
efficients, cluster analysis (CA), and principal compo-
nent analysis (PCA).
In different ways, these methods highlight the qual-
itative and/or quantitative correlations between parame-
ters in terms of EMC.
Besides these analyses, the correlation between pa-
rameters (also in terms of EMC) and the following
groups of independent variables was also analyzed:
Water Air Soil Pollut (2015) 226:399
Fig. 4 First flush graph verification: the decreasing slope of
pollutant Y discloses a first flush
– Conditions of the precipitation event (e.g., rainfall,
maximum intensity of rainfall, cumulative rainfall,
and antecedent dry period);
– Specificity of the monitored sections (e.g., average
daily traffic, contributing watershed area and imper-
vious fraction);
– Air mass transport and other processes related to
salt deposition, including their dependency on pre-
vious weather phenomena such as temperature, hu-
midity, or evaporation.
Figure 5 shows the sequence of data processing and
analysis performed in the present research.
Table 3 Rainfall data for the monitored events
Circumstances related to the sampling
Precipitation data
Rainfall events and ADP
Pollutant concentration and load
Analysis of the first-flow occurrence
Page 7 of 17 399
Fig. 5 Sequence of data treatment and exploratory statistical
analysis preformed
The Pearson coefficient (r) is a measure of the linear
correlation between two sets of data, varying between +
1 and −1: the closer the modulus of r to 1, the stronger
the linear correlation between the two sets of data while
closer to 0 denotes a weaker correlation. When there are
more than two sets of data, the corresponding Pearson
coefficients define a matrix. A given Pearson coefficient
is only statistically significant if the data sample is large
enough. Therefore, alongside each Pearson coefficient,
a p value is computed to evaluate its significance: if it is
less than 0.05, results are considered statistically signif-
icant and if it is less than 0.001, they are highly statis-
tically significant.
Cluster analysis (CA) is another common technique
for statistical data analysis that groups into distinct clus-
ters variables that are quite similar to each other. CA can
The date and time of the beginning of the sample collection; data
to interpret the results (e.g., light rains or very intense rainstorms)
Data stored in the data logger (rainfall and flow), rainfall intensity,
an estimation of the runoff coefficient, and partial volumes
between discrete sample collections
Duration of the event, ADP, duration of the antecedent rainfall event,
volume of the antecedent rainfall event
Intensity of the antecedent rainfall event
Concentrations of discrete samples for all events; concentrations: mean,
median, percentiles 10, 25, 75, and 90 %; minimum; maximum;
standard deviation; percentages of concentrations above the
emission limit value (ELV) of wastewater discharge law; calculation
of the pollutant mass carried in each event; calculation of average
concentrations per event; calculation of SMC; and pollutographs
Calculations of the mass of each pollutant transported in a certain
percentage of the same volume; graphics: accumulated relative
mass vs. relative volume of accumulated road runoff
399 Page 8 of 17 Water Air Soil Pollut (2015) 226:399

Table 4 Criteria for cluster analysis

Criteria CA presented Other CA tested

Variables (pollutant EMC)
Variables normalization
Measure of dissimilarity
between variables
Hierarchical clustering
Cond, Turb, TSS, Hard, Cl−, total P, COD, Salt, TOC, BOD5, total Pb,
O&G, total Fe, total Zn, total Cu total Cd, total Cr
Measurements in the range 0 to 1 [−1;1]; max=1, mean=1,
standard deviation=1
Square Euclidean distance Euclidean distance, Pearson
correlation distance
Centroid method Nearest neighbor, furthest
neighbor, by a median
clustering, Ward’s method

be used to detect structures in data without providing an
explanation/interpretation for their presence. Table 4
identifies the various criteria used in the CA performed
in this study and those selected because of their
relevance.
Principal component analysis (PCA) applies an
orthogonal transformation to convert two, or more,
sets of data into their principal components, which
are linearly uncorrelated, and condense the informa-
tion contained in the original data. PCA can reveal
interaction patterns that cannot be detected by means
of analyzing each set individually. Table 5 presents
the criteria for PCA.
3 Results and Discussion
Table 6 summarizes the hydrological information about
the monitored rainfall events.
One observes that the sampling events represent a
broad spectrum of weather, in terms of precipitation and
of quantitative characteristics of road runoff.
The average event rainfall height was not very high
(5.2 mm) and did not show extreme values of rainfall,
e.g., levels above 10 mm only occurred in two events,
with a maximum of 16.8 mm. The average intensity of
the monitored rainfall events was 0.047 mm/min, with a
maximum of 1.02 mm/min at event 12.
The runoff coefficient, representing the rate between
the volumes of runoff and received precipitation, was
estimated by linear regression for the case study catch-
ment area. It was quite significant and relatively con-
stant throughout the various monitoring campaigns,
with a value close to 0.91, which is consistent with the
size of the catchment area and, especially, with its sig-
nificant impermeability.
In the monitored events, the ADP varied between a
minimum of 6.7 h in event 10 and a maximum of 299.3 h
(12 days) in event 30, with a mean value of 95.6 h,
approximately 4 days. Table 7 presents the frequency
distribution of ADP among monitored events. This range
permitted us to consider different types of events.
For the different water quality parameters, Table 8
summarizes the descriptive statistics of concentrations,

Table 5 Criteria for principal component analysis

Criteria PCA presented Other PCA tested

Variables (pollutant EMC) Cond, Turb, TSS, Hard, Cl−, total P, Sal, TOC, BOD5, total Pb,
COD, O&G, total Fe, total Zn, total Cu total Cd, total Cr
Variables normalization Measurements in the range −1 to 1 –
Extraction method PCA –
Analyzed matrix Correlation coefficients Variance matrix
Extraction of principal components Eigenvalue greater than one Fixed number of components
Maximum value of interactions 25 –
in the estimation

The data analysis was performed with Microsoft Excel and the Statistical Package IBM SPSS Statistics V21.0
Water Air Soil Pollut (2015) 226:399 Page 9 of 17 399

Table 6 Hydrological indices for monitored rainfall events

Event number RDa RMIb MAXIc Runoff volume Runoff flow ADPd RIAEe
(mm) (mm/min) (mm/min) (m3) (m3/min) (h) (mm/min)

1 4.8 0.060 0.11 1.211 0.015 123.0 0.049

2 2.5 0.036 0.08 0.641 0.009 43.2 0.100
3 4.6 0.054 0.12 1.148 0.014 244.3 0.016
4 4.5 0.035 0.06 1.186 0.009 26.0 0.080
5 1.9 0.025 0.10 0.575 0.008 115.0 0.080
6 3.9 0.039 0.08 0.999 0.010 52.1 0.020
7 3.1 0.036 0.10 0.837 0.010 218.5 0.013
8 3.4 0.028 0.08 0.911 0.008 93.8 0.060
9 5.3 0.041 0.16 1.495 0.011 183.1 0.020
10 7.5 0.060 0.12 1.918 0.015 6.7 0.041
11 8.4 0.065 0.18 2.233 0.017 53.0 0.011
12 13.7 0.110 1.02 3.662 0.029 30.8 0.060
13 5.6 0.043 0.28 1.590 0.012 52.3 0.041
14 3.0 0.023 0.08 0.781 0.006 21.0 0.020
15 2.6 0.020 0.06 0.685 0.005 7.8 0.015
16 7.5 0.058 0.38 2.111 0.016 89.3 0.015
17 2.4 0.022 0.10 0.619 0.006 122.3 0.020
18 3.1 0.024 0.06 0.752 0.006 25.7 0.130
19 3.4 0.026 0.12 0.899 0.007 47.0 0.025
20 3.0 0.046 0.05 0.673 0.010 63.7 0.025
21 5.3 0.041 0.14 1.326 0.010 227.1 0.022
22 2.1 0.042 0.14 0.589 0.012 21.7 0.022
23 9.6 0.080 0.15 2.552 0.021 103.6 0.040
24 1.9 0.027 0.12 0.518 0.007 63.1 0.214
25 6.8 0.052 0.18 1.812 0.014 178.0 0.045
26 16.8 0.129 0.38 4.393 0.034 93.0 0.020
27 3.2 0.025 0.06 0.890 0.007 41.2 0.550
28 6.7 0.052 0.10 1.726 0.013 45.5 0.100
29 6.4 0.049 0.10 1.397 0.011 185.3 1.800
30 3.4 0.068 0.14 0.916 0.018 299.3 0.120
Med. 5.2 0.047 0.16 1.368 0.012 95.9 0.130
Min. 1.9 0.020 0.05 0.518 0.005 6.7 0.011
Max. 16.8 0.129 1.02 4.393 0.034 299.3 1.80
a
RD=rainfall depth
b
RMI=rainfall mean intensity
c
MAXI=rainfall maximum intensity
d
ADP=antecedent dry period
e
RIAE=rainfall intensity during antecedent event

EMC, and mass loads and Table 9 presents the matrix of correlation coefficients, AC and PCA, several con-
Pearson coefficients. clusions may be drawn about the physicochemical
From the sequential analysis of the EMC, follow- characteristics and specificities of the investigated
ed by the descriptive statistics, matrix of Pearson road runoff.
399 Page 10 of 17
Table 7 Frequency distribution of ADP among monitored events
ADP (h) 6.0– 12.1– 24.1– 48.1– 64.1– 128.1– >256.0
12.0 24.0 48.0 64.0 128.0 256.0
n.° events 2 2 7 5 7 6 1
The first clearly emerging feature of the road runoff is
its high salinity and its influence in related water quality
parameters, such as conductivity and chloride content.
The mean EMC for salinity, conductivity, and chlo-
rides was 0.1 g/L, 339.0 μS/cm, and 68.5 mg/L, respec-
tively. The conductivity reached a maximum value of
1288.0 μS/cm. In Portugal, figures close to these were
found only in a study conducted at a site on the IP6
highway, located 1.1 km away from the Atlantic Ocean
(Barbosa et al. 2006).
Table 9 shows that there is a strong correlation be-
tween salinity and conductivity (r>0.9) while the cor-
relation of these two water quality parameters with
chlorides is close to 0.8.
In all the events, the pH values are similar to those of
seawater, with a very low coefficient of variation.
The hardness was rather expressive, with a mean
EMC of 76.7 mg CaCO3/L, showing little correlation
with the road runoff salinity. This seems to be related to
the geology and soil characteristics of the surrounding
area. The information presented in Table 8 shows that
the hardness coefficient is not very significant, proving
the relevant and constant source of this parameter.
The correlation between organic matter (in terms
of COD and TOC) and the parameters associated
with salinity seems noticeable. However, despite the
high values found for the organic matter (with a mean
EMC of 85.6 mg O2/L for COD and 21.6 mg/L for
TOC), they have no significance when compared to
the average values of the first study done at this site.
Nonetheless, it is relevant that a higher concentration
of COD and TOC in EMC match with higher salinity
levels.
The ratio between SMC BOD5 and SMC COD is
1:8.5, suggesting a low biodegradability of this road
runoff, a conclusion that is in line with the findings of
other researchers (Gan et al. 2008). The total Cu, with
slightly higher values than those found in other studies
in this field, and with a mean EMC of 86.9 μg/L,
showed a relatively significant correlation not only with
organic matter but also with conductivity and salinity,
Water Air Soil Pollut (2015) 226:399
something that the present research did not try to ex-
plain. It seems, however, that Cu may be one of the
specificities of road runoff in coastal areas.
The concentration of Cu deviates from other heavy
metals such as Zn and Fe, which show high correlations
with TSS (r ∼ 0.8). Fe, with a maximum EMC of
7352.2 μg/L, has shown high concentrations in some
events. As also found in other studies, other heavy
metals showed very low concentrations (ND in many
analyses), confirming the trend for significant decrease
in the concentration of Pb in road runoff (Kayhanian
2012).
It is important to state that some parameters, like Fe,
TSS, and COD, presented at several events a higher
concentration (respectively, 27, 21, and 12 %) than the
emission limit value (ELV) for wastewater discharge
permitted by Portuguese law (with reference to Portu-
guese decree law 236/98, even though it is related to
point, instead of linear, sources of pollution).
The data analysis showed that some important water
quality parameters could be divided into two clusters
based on their correlations to (1) conductivity (often
used as an indicator of the total dissolved solids in
water) and (2) total suspended solids (TSS, particles
which will not pass through a filter):
1. Salinity, chlorides, COD, TOC, BOD5;
2. Turbidity, Fe, Zn.
The CA and PCA confirmed the latter conclusion. In
Fig. 6, a dendrogram represents one of the relevant
cluster analysis of EMC water quality parameters, epito-
mizing the relative distances between them. The analysis
of Fig. 6 allows identifying the following four clusters:
1. TSS, Fe, Zn, and turbidity;
2. Conductivity, COD and chlorides;
3. O&G, P, and Cu;
4. Hardness.
However, for other CA methodologies, Cu gets clos-
er to COD.
Figure 7 shows the projection of the variables
EMC on the planes corresponding to the three prin-
cipal PCA components and identifies the two groups
referred to above. This figure also shows that hard-
ness, as well as other parameters not emphasized in
this paper, such as O&G and total P, are too far away
from these two clusters.
Table 8 Summary of descriptive statistic information for water quality parameters

Parameter pH Cond Sal Turb TSS Hard Cl− COD TOC BOD5 Fe Zn Cu Pb

Unitsf (μS/cm) (g/L) (FNU) (mg/L) (mg CaCO3/L) (mg/L) (mgO2/L) (mg/L) (mgO2/L) (μg/L) (μg/L) (μg/L) (μg/L)
Water Air Soil Pollut (2015) 226:399

Concentrations n.° samples 215 215 215 215 215 215 207 215 204 144 211 211 211 211
Mean 7.2 325.0 0.16 28.6 49.2 73.2 63.2 80.2 21.99 13.0 13.0 1688.8 133.91 85.62
a
Med. 7.2 243.0 0.10 20.3 27.0 68.0 36.5 60.0 14.50 5.0 5.0 969.0 84.00 45.38
Min.b 6.1 55.6 0.05 1.3 1.2 6.5 2.2 5.9 1.60 ND ND <81.0 <15.0 ND
Max.c 8.9 1288.0 0.60 118.0 642.0 208.7 370.9 375.0 160.30 90.0 11658.0 635.00 771.00 108.80
SDd 0.6 226.5 0.11 24.6 74.6 41.0 73.1 73.0 24.32 15.1 1988.5 99.47 135.11 16.54
CVe 8% 70 % 69 % 86 % 151 % 56 % 116 % 91 % 111 % 115 % 118 % 74.3 % 158 % 58 %
EMC Mean (SMC) 339.0 0.2 30.0 57.9 76.7 68.5 85.6 21.6 10.1 1858.0 139.7 86.9 28.7
Med. 261.7 0.1 23.6 44.3 72.1 47.3 74.1 14.8 6.4 1348.8 124.1 61.2 21.0
Min. 101.4 0.1 1.8 2.2 15.7 2.2 11.8 1.4 0.0 35.4 30.2 5.5 6.5
Max. 953.7 0.5 74.6 207.3 170.5 285.1 304.6 97.4 33.6 7352.2 406.9 655.8 69.7
SD 219.6 0.1 20.0 48.0 37.6 70.1 58.5 20.5 11.1 1635.2 76.3 116.6 15.7
CV 65 % 66 % 67 % 83 % 49 % 102 % 68 % 88 % 110 % 88 % 55 % 132 % 54 %
Pollutant load (g/ha.ano) – 1.452 – 486.6 644.6 575.5 719.0 181.4 84.98 1.56 0.12 0.07 0.02

ND not detected
a
Med.=median
b
Min=minimum
c
Max.=maximum
d
SD=standard deviation
e
CV=coefficient of variation
f
With the exception of pollutant load, with specific units
Page 11 of 17 399
399 Page 12 of 17 Water Air Soil Pollut (2015) 226:399

Table 9 Matrix of Pearson coefficients and respective significance of relevant water quality parameters

Cond Sal Turb TSS Hard Cl− COD TOC BOD5 Fe Zn Cu Pb

Cond – 0.979** 0.14 0.08 0.392* 0.797** 0.660** 0.834** 0.706* 0.120 0.287 0.538* 0.286
Sal 0.000 – 0.145 0.13 0.405* 0.805** 0.691** 0.845** 0.695* 0.144 0.304 0.542* 0.299
Turb 0.460 0.445 – 0.699** 0.019 0.276 0.439* 0.241 0.152 0.870** 0.672** 0.121 0.653**
TSS 0.676 0.492 0.000 – −0.13 0.234 0.397* 0.171 0.124 0.865** 0.783** 0.268 0.364*
Hard 0.032 0.027 0.919 0.492 – 0.397* 0.079 −0 −0.29 −0.06 −0.11 −0.16 0.198
−
Cl 0.000 0.000 0.147 0.221 0.033 – 0.430* 0.503* 0.646* 0.403* 0.316 0.151 0.530*
COD 0.000 0.000 0.015 0.03 0.679 0.02 – 0.882** 0.565* 0.342 0.550* 0.783** 0.323
TOC 0.000 0.000 0.218 0.383 0.996 0.007 0.000 – 0.725* 0.187 0.467* 0.837** 0.338
BOD5 0.001 0.001 0.547 0.625 0.236 0.005 0.015 0.001 – 0.232 0.480* 0.538* 0.555*
Fe 0.528 0.449 0.000 0.000 0.768 0.03 0.064 0.34 0.355 – 0.780** 0.12 0.602**
Zn 0.124 0.102 0.000 0.000 0.58 0.095 0.002 0.012 0.044 0.000 – 0.525* 0.328
Cu 0.002 0.002 0.524 0.153 0.413 0.436 0.000 0.000 0.021 0.528 0.003 – −0.01
Pb 0.126 0.109 0.000 0.048 0.293 0.003 0.081 0.079 0.017 0.000 0.077 0.977 –

*p value<0.05; **p values<0.001

Two groups of water quality parameters are
highlighted in Fig. 7, one of which is the first cluster
showed in Fig. 6 related to solids and some heavy
metals.
The occurrence of the first flush phenomenon was
confirmed, especially for the pollutants associated with
particles, such as TSS and correlated pollutants, but not
so much for the dissolved pollutants, such as those
associated with salt deposition. However, this pattern
is not always observed. Figure 8 depicts some of the first
flush relations found.
The highest concentration of pollutants, according to
the present research, tends to occur when, after a long
ADP, the first moments of the event are characterized by
high intensity rainfall, inflating the first flush phenom-
enon. On the other hand, the study confirmed that above
a certain ADP level, these concentrations tend to
stabilize.

Fig. 6 Dendrogram representing

one relevant CA for EMC water
quality parameters
Water Air Soil Pollut (2015) 226:399
Fig. 7 Variable projection on three planes corresponding to three
principal components of PCA
Based on the salt deposition rate (SDR) data obtained
at the two sites, the SDR appears to show a high corre-
lation with wind speed and direction, but mostly with
wave propagation, so that it is lower in the summer, in
spite of the favorable wind direction in the case study.
The distance to the sea, topography, ground obstacles,
and the platform altitude seem to be also relevant; e.g.,
SDR tends to decrease exponentially with distance as
asserted by Hossain and Easa (2011).
Fig. 8 Accumulated pollutant
load versus cumulative volume of
road runoff: a event 11: TSS and
salinity, b event 24: COD and
BOD5, c event 8: Fe and Zn, d
event 28: TSS and Fe
Page 13 of 17 399
The SDR in the road section is relatively significant,
with an average of 55mgCl−/m2. Figure 9 shows that
there is a sharp variation of SDR along the year.
SDR has two peaks, one in January/December and
the other one in May. Actually, around May, there are
two peaks, the second one being smaller than the first
one (according to the collected data), corresponding to
the transition between the beginning of more favorable
winds and a still significant aerosol generation at sea. In
warmer months, especially in August, SDR is lower.
As usually, some exploratory statistical techniques
were more successful than the others were. In fact, the
ACP was not as remarkable as Pearson coefficient cor-
relations and CA; moreover, based on the present re-
search, the latter seems to produce clearer conclusions.
Table 10 presents Pearson coefficients, correlating
relevant water quality parameters to meteorology and
road section parameters.
During a rainfall event, RD and RMI can represent
the wash-off energy required to leach and mobilize the
deposited pollutants; ADP may represent the available
pollutant quantity that accumulates on the highway sur-
face before the runoff occurs (Kim et al. 2005).
RD and RMI coefficients are negative, whereas that
of ADP is positive for all pollutants. This indicates that
the pollutant EMC decreases with the dilution effect
399 Page 14 of 17
Fig. 9 Variation of SDR along
the year in the study case. a
Measures in monitoring station, b
measures in meteorological
station
induced by heavy rainfall, but increases with a long
antecedent dry period due to the increased pollutant
mass that accumulates on the highway surface.
As indicated by Pearson coefficients, ADP and wind
speed during ADP (MWSADP) seem to show high
correlations with relevant pollutants.
ADP, which has been mentioned in several interna-
tional researches, e.g., Kayhanian et al. (2007), Opher
et al. (2009), has several significant correlations and
seems to be reflected mainly in pollutants associated
with dissolved or colloidal matter. The VADP is tightly
correlated with ADP, and this may explain their similar
correlation pattern.
In addition, MWSADP (parameter rarely considered
in road runoff researches) will particularly influence
(with inverse proportionality) salinity, conductivity, and
the organic matter, showing a greater correlation than RD
with some water quality parameters. DE is mainly in-
versely related with water quality parameters associated
to salinity. VE is also tightly correlated with ADP, and
this may explain their similar correlation pattern.
MAXI has an important correlation with pollutants
associated with particulate matter, especially TSS. Other
parameters—such as RMI and RIAE—did not show a
great correlation with pollutants.
Water Air Soil Pollut (2015) 226:399
None of the parameters related to meteorology or the
platform section are correlated with hardness, which is
in agreement with its exterior source.
4 Conclusions
Based on a case study, this research focused on the
distinctive quality characteristics and patterns of road
runoff in coastal areas. For that purpose, and along
3 years, an intensive monitoring program was imple-
mented in a road section near the sea, including the
measurement of various parameters related to meteorol-
ogy, road runoff hydrology, and salt deposition (which is
unique in this type of research).
In order to estimate the correlations and patterns of
different water quality parameters and variables related
to weather, road section, and salt deposition, the study
included exploratory data analysis using different tech-
niques, confirming some specific features of the inves-
tigated road runoff.
Although variable throughout the year, as confirmed
by SDR measurements, the salt deposition is significant
on the road platform, increasing the concentration of the
water quality parameters analyzed, with significant
 Water Air Soil Pollut (2015) 226:399

Table 10 Pearson coefficients correlating relevant water quality, meteorology, and road parameters

Cond Salt Turb TSS Hard Cl− COD TOC BOD5 Fe Zn Cu Pb

DEa −0.411* −0.423* −0.106 −0.034 −0.231 −0.581** −0.158 −0.118 −0.031 −0.093 −0.137 0.0755 −0.303
RD −0.384* −0.343 −0.046 0.221 0.0823 −0.26 −0.308 −0.371* −0.248 0.0998 −0.053 −0.216 −0.126
RMI −0.207 −0.161 −0.011 0.2511 0.1824 −0.053 −0.238 −0.347 −0.229 0.1312 −0.004 −0.241 −0.026
MAXI −0.064 −0.001 0.0474 0.619** −0.092 −0.092 0.1574 0.0042 −0.103 0.3126 0.3593 0.2633 −0.213
b
VE −0.413* −0.425* −0.138 −0.071 −0.239 −0.587* −0.181 −0.14 −0.023 −0.123 −0.163 0.0702 −0.33
ADP 0.562* 0.552* 0.252 0.0975 0.2359 0.521* 0.425* 0.426* 0.606* 0.251 0.3448 0.2427 0.248
VADPc 0.553* 0.541* 0.2481 0.0925 0.229 0.507* 0.414* 0.412* 0.597* 0.2448 0.3325 0.2394 0.2372
RIAE −0.13 −0.139 0.0937 −0.132 −0.145 −0.153 −0.034 −0.166 −0.075 −0.027 −0.019 −0.076 −0.168
MWSADPd −0.490* −0.473* −0.129 0.0896 −0.214 −0.195 −0.42 −0.355 −0.119 0.0636 −0.117 −0.316 −0.316

*p value <0.05
a
DE=duration of rainfall event
b
VE=vehicles during the event
c
VADP=vehicles during ADP
d
MWSADP=mean wind speed during ADP
Page 15 of 17 399
399 Page 16 of 17
amounts of seawater features, e.g., salinity, conductivity,
and chlorides.
The hardness, in contrast to its presence in seawater,
showed a lower correlation with the above parameters.
On the other hand, the concentrations of organic
matter and Cu were correlated with parameters associ-
ated with salt deposition.
Fe and Zn show high correlations to TSS while Pb
showed a very low concentration.
In the present research, many of these road runoff
pollutants seemed to be very dependent on the ADP,
while others are more dependent on MWSADP.
A statistical modeling approach is ongoing, follow-
ing techniques that have been successfully applied in
this area, such as multiple linear regression, in order to
identify and quantify the relationship between the de-
pendent variables of pollutants and EMC independent
variables associated to such processes.
Acknowledgments Part of this study was developed within a
project financed by the Portuguese National Foundation for Sci-
ence and Technology (PTDC/AMB/64953/2006).
Antunes P. thanks the Portuguese National Foundation for
Science and Technology for the Ph.D. grant (SFRH-BD-43638-
2008).
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