water research 43 (2009) 1630–1640

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Characterisation of atmospheric deposition as a source of

contaminants in urban rainwater tanks

R. Hustona,b,d,f,*, Y.C. Chana,f, T. Gardnerc, G. Shawe,f, H. Chapmanb,g

a
School of Environment, Griffith University, Nathan Campus, 170 Kessels Road, Brisbane, Queensland 4108, Australia
b
CRC for Water Quality and Treatment, Australia
c
Queensland Department of Natural Resources and Water, Queensland, Australia
d
University of Queensland, The National Research Centre for Environmental Toxicology, Queensland, Australia
e
School of Public Health, Griffith University, Queensland, Australia
f
Australian Rivers Institute, Griffith University, Queensland, Australia
g
Smart Water Research Facility, Griffith University, Australia

article info abstract

Article history: To characterise atmospheric input of chemical contaminants to urban rainwater tanks,
Received 13 October 2008 bulk deposition (wet þ dry deposition) was collected at sixteen sites in Brisbane, Queens-
Received in revised form land, Australia on a monthly basis during April 2007–March 2008 (N ¼ 175). Water from
19 December 2008 rainwater tanks (22 sites, 26 tanks) was also sampled concurrently. The deposition/tank
Accepted 22 December 2008 water was analysed for metals, soluble anions and selected samples were additionally
Published online 3 January 2009 analysed for PAHs, pesticides, phenols, organic & inorganic carbon. Flux (mg/m2/d) of total
solids mass was found to correlate with average daily rainfall (R2 ¼ 0.49) indicating the
Keywords: dominance of the wet deposition contribution to total solids mass. On average 97% of the
Urban water total mass of analysed components was accounted for by Cl (25.0%), Na (22.6%), organic
2
Atmospheric deposition carbon (20.5%), NO
3 (10.5%), SO4 (9.8%), inorganic carbon (5.7%), PO3
4 (1.6%) and NO
2

Bulk deposition (1.5%). For other minor elements the average flux from highest to lowest was in the order of
Heavy metals Fe > Al > Zn > Mn > Sr > Pb > Ba > Cu > Se. There was a significant effect of location on flux
Rainwater of K, Sb, Sn, Li, Mn, Fe, Cu, Zn, Ba, Pb and SO2
4 but not other metals or anions. Overall the

Tank water quality resulting from the deposition (wet þ dry) was good but 10.3%, 1.7% and 17.7%
Pb of samples had concentrations of Pb, Cd and Fe respectively greater than the Australian
Lead Drinking Water Guidelines (ADWG). This generally occurred in the drier months. In
Health risk comparison 14.2% and 6.1% of tank samples had total Pb and Zn concentrations exceeding
the guidelines. The cumulative mean concentration of lead in deposition was on average
only 1/4 of that in tank water over the year at a site with high concentrations of Pb in tank
water. This is an indication that deposition from the atmosphere is not the major
contributor to high lead concentrations in urban rainwater tanks in a city with reasonable
air quality, though it is still a significant portion.
ª 2008 Elsevier Ltd. All rights reserved.

1. Introduction However, there is less published on the deposition of chemical

contaminants from the urban atmosphere, particularly in
There has been extensive research into air quality in urban Australia. In many cities worldwide drought and population
settings (Chan et al., 2000; Jordan, 2005; Lim et al., 2005). growth are putting pressure on water supplies. In Australia

* Corresponding author. Tel.: þ61 4 2874 8401.

E-mail address: r.huston@griffith.edu.au (R. Huston).
0043-1354/$ – see front matter ª 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.watres.2008.12.045
 water research 43 (2009) 1630–1640
a change in government policy combined with rebates has seen
a large number of urban households installing rainwater tanks.
Tank owners often use the water for drinking even where
treated water is available though it is not advised by water
authorities. The percentage of owners drinking tank water has
been reported as 60% in the Sunshine Coast (Lukin et al., 2005)
and in a recent study in Brisbane it varied with the demo-
graphic being 1%, 15% and 92% for greenfield, retrofit and peri
urban tank owners respectively (Gardiner et al., 2008).
However, roof runoff has been shown to contain elevated
heavy metals such as Pb and Zn with differences noted
between urban, industrial and rural sites (Thomas and Greene,
1993), with the roof often acting as a source of metals (Chang
et al., 2004). Tank water Pb also exceeds Australian Drinking
Water Guidelines (2004) in some cases (Chapman et al., 2006).
Government and water authorities are concerned that urban
and industrial air pollution may adversely affect the water
quality in urban tanks through both wet and dry deposition of
contaminants (CRC for Water Quality and Treatment, 2005;
Gardner et al., 2004). However limited data exists on the rela-
tive contribution of atmospheric deposition. Before control
measures are considered it is necessary to characterise the
input of atmospheric deposition to the chemical water quality
of urban tanks. This paper examines the current atmospheric
deposition of chemicals in a sub-tropical urban environment in
Brisbane, Australia. The deposition of contaminants is
compared with tank water concentrations at 13 sites sampled
at the same time and location. Location effects on fluxes of
deposited contaminants are also examined.
2. Materials and methods
2.1. Local climate and meteorology
Greater Brisbane is a sprawling city of just under 2 million
people (ABS, 2006) in a sub-tropical climate. It is heavily reliant
on cars and trucks with transport estimated to generate 60%
or more of the air pollution (EPA, 2004). It has a domestic and
international airport, shipping port and oil refineries near the
mouth of the Brisbane River and some light industry in several
industrial precincts. The median annual rainfall of 1138 mm is
typically predominately in spring and summer, though the
sampling period had an unusual extended drought followed
by heavy rains toward the end of the sampling. The total
rainfall for the period was 86% of median rainfall for the last
75 years (Bureau of Meteorology, Archerfield station) with 5
out of the 12 months having less than 50% of median rainfall
for that month (see Supplementary information, appendix 1).
Average minimum and maximum temperatures are between
20–30  C and 10–20  C for summer and winter respectively and
average humidity ranges from 45 to 72% being lowest in
winter and highest in the summer. Winds are typically a land
breeze from the south–southwest in the mornings and change
in the afternoons to an east–northeast sea breeze (ABM, 2008).
2.2. Sampling
Sampling of wet plus dry atmospheric deposition with
continuously open containers, known as bulk deposition (BD),
1631
was conducted at 12 households and 4 Environmental
Protection Agency (EPA) air pollution monitoring sites on
a monthly basis from April 2007 to March 2008. Sites were
spread across greater Brisbane, Queensland, Australia (Fig. 1).
The samplers were based on the Australian standard for dust
deposition (AS/NZS 3580.10.1, 2003). They consisted of 4 L
amber glass bottles and clear glass funnels (15–18 cm diam-
eter) pre-cleaned in a laboratory dishwasher then soaked in
8% nitric acid for several days and finally rinsed thoroughly
with MilliQ water and air dried. Teflon stoppers were used to
hold the funnels in place and treated the same for cleaning. As
the aim was to mimic the microbial and physical environment
in a tank no antimicrobial agent was used and each bottle was
completely wrapped with aluminium foil to exclude light and
prevent algal growth. Samplers were deployed with clear
surrounding airspace at a height of 2 m in yards behind
private houses or at 4 m for EPA sites. They were deployed for
33 days on average. Funnels were rinsed with 100 mL MilliQ
water prior to removal and sample transport to the laboratory.
Bottles were stored at 4  C in the dark until processing which
was usually within two weeks.
The total sample volume was determined gravimetri-
cally. As the total solids concentrations averaged <0.04 mg/
mL and did not exceed 0.26 mg/mL there was no adjust-
ment for increased density associated with solids and 1 g
was assumed to equal 1 mL of rainfall. Average daily rain-
fall (mm/d) was calculated by the volume collected (cm3)/
surface area of the funnel (cm2)/number of days deployed
(d)  10 (mm/cm). Evaporative losses were measured as
10 mL/8 d during March 2008 and estimated as <10% in 88%
of samples (median volume collected ¼ 1700 mL). Previous
research has shown BD samplers to correlate well with rain
gauges (Rossini et al., 2005). Tank water was sampled
directly into 4  5 mL polypropylene tubes (Sarstedt), one
container for each analysis, as close to the tank outlet as
possible and before any filter systems present and where
possible before any pump. Sites were spread across Bris-
bane with 13 locations having both tank water and BD
sampled concurrently.
2.3. Chemical analysis
2.3.1. Total solids analysis
Total solids were determined gravimetrically by difference in
mass after evaporating a well-mixed aliquot of 250–350 mL of
BD sample at 105  C in a clean dry beaker (Method 2540 B)
(Eaton et al., 2005). Beakers were cooled and stored in a des-
sicator before weighing.
2.3.2. Organic analysis
Organic analysis was undertaken by Queensland Health
Scientific Services (an NATA registered laboratory) which use
a reporting limit (RL) approximately five times the detection
limit of the method. Approximately 1 L of sample was liquid–
liquid extracted with dichloromethane and then analysed by
GC/MS. Surrogates and internal standards were used for
quality control. This organic analysis included 122 herbicides
and pesticides, 17 PAHs and 16 phenolic compounds. Pesti-
cides and herbicides are not listed due to space but the PAHs
and phenolic compounds analysed are presented in Table 1.
1632 water research 43 (2009) 1630–1640

Fig. 1 – Bulk Deposition Sampling sites.

2.3.3. Metal analysis lower for most elements analysed compared with many
Metals analysis (29–30 metals, see Table 4 for list) was based earlier studies using ICP-optical emission spectrometer or
on US EPA method 200.8 for acid soluble trace elements in atomic absorption spectrometer instruments. Water was of
water using Inductively Coupled Plasma-Mass Spectrometer low turbidity so tank water and BD samples were acidified
(ICP-MS). ICP-MS has detection limits 1–2 orders of magnitude directly with nitric acid (4.9 ml sample þ 0.1 ml HNO3) then
0.1 ml of internal standard solution was added to all samples
including calibration standards, blanks and Certified Refer-
ence Material (CRM – TM23.3, lot 305, National Water Research
Table 1 – PAHs and phenolics analysed. Institute, Environment Canada). Internal standards used were
PAHs Phenolics Sc, Ge, Y, Rh, Tb, Au at 10 mg/L for all apart from Au which was
2 mg/L. A mixed environmental calibration stock was
Benzo[g,h,i]perylene Phenol
purchased (Choice Analytical, Thornleigh, Sydney, NSW, 2120)
Dibenz[a,h]anthracene 2-Chlorophenol
to which were added individual standards for Li, Al, Bi and Sr.
Indeno[1,2,3-cd]pyrene 2-Methylphenol
Benzo[e]pyrenea 4-Methylphenol The Standards were mixed and diluted in 2% nitric acid to
Benzo[a]pyrene 2-Nitrophenol 1000 mg/L then diluted further each month from this stock. An
Perylenea 2,4-Dimethylphenol Agilent 7500cs ICP-MS was used for analysis. Interference
Benzo[bþk]fluorantheneb 2,4-Dichlorophenol corrections were used for In, Cd, Mo and V and Pb concen-
Chrysene 2,6-Dichlorophenol tration was based on the sum of the counts from all isotopes.
Benz[a]anthracene 4-Chloro-3-methylphenol
Arsenic is normally corrected for Cl interference, however it
Pyrene 2,4,6-Trichlorophenol
Fluoranthene 2,4,5-Trichlorophenol
was found to have more reliable values without interference
Anthracene 2,4-Dinitrophenol corrections because of the relatively low chloride concentra-
Phenanthrene 4-Nitrophenol tions in rainwater. Analysis with and without interference
Fluorene 2,3,4,6-Tetrachlorophenol corrections was run for comparison.
Acenaphthene 2-Methyl-4,6-dinitrophenol
Acenaphthylene Pentachlorophenol
2.3.4. Anion analysis
Naphthalene
A total of eight soluble anions (F, Cl, NO   2
2 , Br , NO3 , SO4 ,
Benzo-b-naptho(1,2-d )thiophenea 3 2
Cyclopenta[c,d]pyrenea PO4 and C2O4 ) were analysed without prior filtration via Ion
chromatography on a Dionex LC20 instrument. The chroma-
a Only analysed in tank water samples.
tography consisted of a 2 mm internal diameter AS4A_SC
b Analysed as combined as they were not chromatographically
column with an AG4A-SC guard column and anion self-
resolved.
regenerating suppressor run at 50 mA. Eluent flow was 0.5 mL/
 water research 43 (2009) 1630–1640
min of 1.8 mM sodium carbonate/1.7 mM sodium bicarbonate.
Electrical conductivity was used for detection and determined
via a Dionex CD-20.
2.3.5. Total organic and inorganic carbon analysis
Total, inorganic and organic carbon were analysed by
combustion-infrared detection with an Elementar liqui TOC
analyser. Organic carbon was obtained by subtraction of
inorganic from total fractions. External calibration of organic
carbon and inorganic carbon fractions used potassium
hydrogen phthalate and sodium carbonate/bicarbonate as
calibration standards.
2.4. Quality control
A BD field blank (capped bottle of milliQ water) was filled and
deployed at one site for the collection period for most months.
One BD sampling was duplicated at a randomly selected site
each month. Laboratory replicates of several tank water and
BD samples were analysed each month. Laboratory blanks
were analysed every 10–20 samples. The method detection
limit (MDL) was defined as mean þ 3  standard deviation
using all laboratory blanks (N ¼ 75–91) for the year, after
exclusion of outliers (defined as >3 standard deviations). The
MDL for Na, Mg, Ca and K was 100, 40, 200, 40 mg/L respectively
and 100 mg/L for all anions. Fe and Al had MDLs of 30 mg/L and
5 mg/L respectively while all other elements averaged 0.37 mg/L
(range 0.1–2 mg/L). Median pooled relative standards devia-
tions (RSDs) of replicates were 17.5% (range 3.6–62.7%) and
5.9% (range 0–33.1%) for BD and tank water samples respec-
tively with higher RSDs where most samples were near
detection limits. A Certified Reference Material (CRM) of trace
elements in water was analysed with each analytical run on
the IPC-MS (TM23.3, lot 305, National Water Research Insti-
tute, Environment Canada). In general 95–100% of results over
the year were within two standard deviations of the certified
value for all elements except Fe and Sr. The certified Fe
concentration was below the MDL. The non-certified (indica-
tive) values for other elements also compared well to those
listed in the CRM.
Occasional contamination of the field blank with nitrate
was found and this may indicate insufficient rinsing with
milliQ water, therefore results for nitrate should be inter-
preted with caution. However, the average concentration and
variation of nitrate in BD (1.17  1.24 mg/L) were comparable
to that in rainwater tanks (1.59  1.44 mg/L). Rainwater tank
samples were collected directly into polypropylene tubes that
had not been soaked in nitric acid so did not have contami-
nation issues. As field blanks were not open to the atmosphere
there would have been no bacterial activity to consume any
residual nitrate (Dammgen et al., 2005), unlike BD samplers,
and hence values were not corrected using field blanks.
2.5. Data processing
All data values below the MDL were recoded at 1⁄2 the MDL for
calculation of descriptive statistics and flux. One sample
result each for Ni, Cd and Pb and five for V and Cr were
excluded from analysis due to likely contamination after
examination of box plots of log-transformed values and the
1633
robust methods based on the median absolute deviation
detailed in Miller (1993). Some positive bias in average flux
values for F, PO3 
4 , Br , C2O4
2
is expected where most
samples were below detection limits. Flux of elements was
calculated using the concentration, volume collected, area of
funnel and number of days deployed to give a value in mg/m2/
d. Mean annual flux was based on the mean of all monthly
fluxes. F, SO2 
4 , Cl , Na and Mg fluxes showed a normal
distribution while all other fluxes displayed a log-normal
distribution. Statistical analysis of fluxes was based on the
unchanged data for F, SO2 
4 , Cl , Na and Mg and the log value
for all other fluxes (Fowler et al., 1998; Gilbert, 1987). Levene’s
statistic was used for testing homogeneity of variance and
where significant differences existed post hoc analysis used
Tamhane’s T2. All other post hoc analysis used the Tukey test.
Mean and standard deviations of groups are calculated from
the transformed data when used then converted back to
normal (Fowler et al., 1998). Significance level was set at
P < 0.05. Where the majority of samples were below detection
limit the compound was excluded from statistical analysis.
Average results are reported as mean  1 standard deviation
unless otherwise stated. Methods for reconstructing the total
mass were based on Chan et al. (2000) and references therein.
Briefly the total solids mass was reconstructed from the
analytical results by estimating the mass of crustal matter, sea
salt, ammonium sulfate, organic carbon, smoke, lead bromide
and nitrates. Crustal matter was based on the Al, Fe, Ca and Si
content with Si estimated from Al as it was not analysed
directly. Sea salt was based on Na, ammonium sulfate on
sulfate, soot and organic matter were pooled and assumed to
be all organic matter and based on total organic carbon, smoke
was based on non-soil K and lead bromide the sum of lead
plus bromide. Nitrates were based on direct measurement.
Volume weighed annual mean concentrations were calcu-
lated from the total mass of compound deposited over the
year divided by the total rainfall collected at the site over the
year.
3. Results
3.1. Organic compounds
Of the 155 organic compounds analysed in BD at 16 sites in
December 2006 there were few that were above the parts per
trillion detection limit. Typically only 1 or 2 sites had some
organic compounds detected with concentrations near the
detection limit. As such, the maximum concentration rather
than the mean is shown. With the mass adoption of rainwater
tanks in urban Australia and some people drinking tank water
(Gardiner et al., 2008) concentrations of measured compounds
in BD were compared with the 2004 Australian Drinking Water
Guidelines (ADWG) to assess if there was any potential health
risk (Table 2). For many compounds ADWG have two
concentrations, the first is the guideline level which is based
on instrumental detection limits and the view that the
compound should not be present in drinking water, and
where applicable, a health guideline value (usually much
higher) using the acceptable daily intake (ADI) based on
exposure, dose response and health effects (ADWG, 2004) is
1634 water research 43 (2009) 1630–1640

Table 2 – Concentrations of organics above reporting level Table 3 – Concentrations of organics above reporting level
in Bulk Deposition samples. in tank water samples.
Compounds No. RL Max. ADWG Compounds No. RL Max. ADWG
>RL Conc. (health) >RL conc. (health)

PAHs 0.01a (BaP) Phenols

Pyrene (mg/L) 1 0.01 0.01 10 4-Methylphenol (mg/L) 1 0.24 0.7 na
Fluoranthene (mg/L) 1 0.01 0.01 10
PAHs 0.01a (BaP)
Anthracene (mg/L) 1 0.01 0.039 1
Anthracene (mg/L) 1 0.01 0.013 1
Acenaphthylene (mg/L) 1 0.01 0.014 10
Naphthalene (mg/L) 2 0.01 0.054 10
Phenolics (mg/L)
Herbicides
Phenol (mg/L) 2 0.25 0.8 na
Diuron (mg/L) 2 0.01 0.79 30
4-Methylphenol (mg/L) 1 0.25 0.83 na
Simazine (mg/L) 1 0.01 0.01 0.5 (20)
2-Nitrophenol (mg/L) 2 0.25 0.57 na
Terbutryn (mg/L) 1 0.01 0.01 1 (300)
Pentachlorophenol 1 0.25 0.44 0.01 (10)
(mg/L) (#) Levels in brackets refer to the guideline level based on health
criteria. RL ¼ reporting limit. na ¼ not applicable, i.e. no guideline
Herbicides (mg/L)
set. N ¼ 15 tanks sampled in July 2007.
Ametryn (mg/L) 1 0.01 0.01 5 (50)
a ADWG values for PAHs other than BaP are not given but are
Atrazine (mg/L) 11 0.01 0.03 0.1 (40)
calculated here based on toxic equivalency factors relative to BaP
Diuron (mg/L) 5 0.01 0.05 30
(Nisbet and Lagoy, 1992).
Simazine (mg/L) 3 0.01 0.02 0.5 (20)

(#) Levels in brackets refer to the guideline level based on health

criteria. RL ¼ reporting limit. na ¼ not applicable, i.e. no guideline
set. N ¼ 16 sites sampled in Dec 2006.
a ADWG values for PAHs other than BaP are not given but are
calculated here based on toxic equivalency factors relative to BaP
(Nisbet and Lagoy, 1992).
given. For organic compounds the only sample exceeding the
ADWG was for pentachlorophenol and this was still well
below the health guideline, which as stated, is based on actual
health risk. Pentachlorophenol is commonly used as a wood
preservative. There were no obvious local sources. A low level
of herbicides was the most common finding, particularly
atrazine, simazine and diuron in both BD and tanks. Atrazine
is commonly detected at background and urban sites with the
presence at background sites indicating long-range transport
(Majewski et al., 2000).
To compare with organics found in BD, a group of 15 tanks
were also sampled in July 2007 and the water analysed for the
same set of organic compounds with 2 additional PAHs
a linear fashion (see Fig. 2). This is largely due to the increase
of the water-soluble components NaCl, carbon, nitrates and
sulphates adding to the mass of solids deposited with rain
(Table 4). The regression equation suggests a background
deposition flux of 32 mg/m2/d which equates to the average
dry deposition for all seasons and locations. The concentra-
tion of TS decreased exponentially with increasing rainfall
indicating a dilution effect. This is in agreement with other
studies which have found a decrease in concentrations of ions
or heavy metals with increasing rainfall (Alastuey et al., 2001;
Hou et al., 2005). This is because washout (below cloud scav-
enging) is a major mechanism by which contaminants are
incorporated in rainfall (Hou et al., 2005). Most of this washout
occurs with the first few mm of rainfall (Alastuey et al., 2001)
with further rain diluting contaminants already washed out.
Reconstructed mass concentration was significantly
correlated with experimental total solids concentration but
300

(cyclopenta[cd]pyrene and benzo[b]naptho[2,1-d]thiophene)

that are markers for petrol and diesel traffic respectively (IPCS,
Total solids flux (mg/m²/d)

1996). Even fewer compounds were above detection limits for R² = 0.49
the tank water and none above the guideline levels (Table 3). 200
Based on these results and those of the earlier survey work it
was decided that further analysis of organics not be under-
taken for this project. However, detection of herbicides and
pesticides in deposition is generally greatest during the
100
application period (Grynkiewicz et al., 2003) so the sampling
period in this project is not sufficient to represent annual
deposition.

3.2. Inorganics 0
0 2 4 6 8 10 12
Total rainfall collected in BD sampler
3.2.1. Total solids flux, concentration, rainfall and for month - expressed as (mm/d)
reconstructed mass
The flux of total solids (TS) increased significantly (P < 0.05, Fig. 2 – Bulk Deposition flux of total solids vs total rainfall
R2 ¼ 0.49) with the average daily rainfall for the month in collected for month (expressed as mm/d).
 water research 43 (2009) 1630–1640 1635

solids determination due to inherent errors in the method

Table 4 – Average flux of measured mass in descending %
of total. (Eaton et al., 2005).
Additionally comparison of mass reconstruction results
Chemical N > Min Max Mean s.d % of total
from aerosol samples collected on filters may not be directly
DL (mg/ (mg/ (mg/ (mg/ mass
m2/d) m2/d) m2/d) m2/d) applicable to deposition because of their very different
particle size and composition (Lim et al., 2006). Metals of
Cl 173 206.11 22915.47 6507.67 4423.28 21.9
crustal origin (Fe, Al, Si) are found mostly in the coarse particle
Na 175 202.23 19890.79 5880.36 3588.16 19.8
fraction (>2.5 mm) and can constitute a large part of urban
Organic 117 212.13 45252.61 5342.65 6211.08 17.9
carbon aerosol while anthropogenic metals are mostly in the fine
NO 3 172 22.48 22122.55 2740.85 2636.47 9.2 particle fraction (Chan et al., 2008; Sillanpää et al., 2006; Yi
SO2
4 173 146.12 9054.66 2547.51 1420.06 8.6 et al., 2006). Though the majority of Cr, Cu, Ni, Pb and Zn mass
Inorganic 112 24.08 15962.85 1480.32 2147.80 5.0 in ambient air may be associated with particles <6 mm, the dry
carbon deposition of these metals is dominated by particles >10 mm
Ca 165 126.91 6899.04 1397.73 1184.09 4.7
(Lim et al., 2006; Sakata and Marumoto, 2004). It is likely that
K 168 25.38 6101.41 910.95 943.26 3.1
larger particles also dominate the dry deposition of crustal
Mg 175 75.39 2400.47 847.34 484.10 2.8
PO3
4 74 7.77 15864.16 527.14 1444.36 1.8 metals such as Al, Fe and Si as crustal sources are usually in
NO 2 99 7.77 9603.97 423.43 820.01 1.4 the courser aerosol. Particle size analysis of selected BD
Al 173 4.67 2107.90 310.59 383.89 1.04 samples supports the dominance of larger particles in depo-
Fe 142 16.78 1535.68 275.27 277.20 0.92 sition as the mean modal particle size was 18.5 mm.
F 39 7.77 570.17 159.85 105.72 0.54 The relative importance of dry versus wet deposition to the
Br 1 7.77 570.17 156.69 109.13 0.53
overall flux is dependant on the rainfall and analyte, with dry
C2O24 0 7.77 570.17 156.06 109.25 0.52
Zn 171 2.97 191.60 45.53 36.32 0.15
deposition dominating annual flux in more arid environments
Mn 175 2.59 124.30 16.06 18.83 0.054 and for some elements such as Cr, As, Mn, V, Cu, Ni Cd and Pb
Sr 170 0.83 47.89 8.55 8.35 0.029 (Azimi et al., 2003; Sakata et al., 2008). While dry deposition
Ba 167 0.41 33.77 7.27 5.35 0.024 may be dominated by >10 mm particles, wet deposition has
Pb 122 0.11 47.13 5.92 7.46 0.020 been calculated to favour finer particle constituents (Kaupp
Cu 120 0.33 25.47 5.52 4.80 0.019
and McLachlan, 1999). Studies suggest rain scavenges the 2–
Cr 117 0.11 70.68 1.81 6.08 0.006
10 mm aerosol size range most efficiently followed by the
Se 14 0.08 5.70 1.76 1.32 0.006
Ni 82 0.12 5.96 1.03 1.01 0.003 <0.1 mm while the 0.1–2 mm particles are the least efficiently
As 107 0.06 29.98 0.97 2.46 0.003 scavenged (Zhang and Vet, 2006).
V 107 0.17 4.22 0.90 0.78 0.003
Co 79 0.05 7.79 0.72 1.47 0.002 3.2.2. Major and minor components of deposition flux
Sb 55 0.02 2.65 0.50 0.47 0.002 The contribution to the flux of all analysed components is
Mo 5 0.02 1.71 0.48 0.33 0.002
listed in Table 4 in decreasing percentage of total mass ana-
Li 84 0.04 6.20 0.37 0.55 <0.001
lysed. Sea salt is the major component with organic carbon,
Sn 64 0.01 3.40 0.35 0.44 <0.001
Cd 33 0.01 9.56 0.32 0.99 <0.001 nitrates, sulphates and inorganic carbon cumulatively
Bi 1 0.03 0.57 0.18 0.11 <0.001 explaining 82.4% of the total mass of analysed components.
This is in agreement with urban deposition and aerosol
All units in mg/m2/d. N > DL ¼ number of samples with concentra-
characteristics of coastal cities which list sea salt, carbon
tions above method detection limit (MDL). Concentrations below
MDL were recoded at 1⁄2 MDL for calculation of flux. (elemental or particulate organic matter), sulfate, nitrates and
ammonium ions the dominant compounds (Deboudt et al.,
2004; Sillanpää et al., 2006). The sea salt flux being significantly
this on average only accounted for 32% of the total solids correlated with rainfall (P < 0.01, R2 ¼ 0.4) is supported by
measured (P < 0.05, R2 ¼ 0.44). In this study, the Si and soil modelling where dry deposition only accounts for approxi-
concentrations were estimated from the Al and Fe concen- mately 30% of the removal of sea salt from the atmosphere
trations. The silicates in soil require hydrofluoric acid for (Henzing et al., 2006). The other major components of flux in
digestion (Eaton et al., 2005). Elements such as Fe and Al decreasing order are Ca > K > Mg > PO3 
4 > NO2 . The presence
3
incorporated in these minerals may be underestimated in our of PO4 may be an indication of bird faeces contamination in
analysis due to the incomplete digestion. Conko et al. (2004) the BD samplers (Dammgen et al., 2005). The terrestrial
also reported only partial dissolution of crustal elements with elements Al and Fe are the greatest in the minor components
direct acidification of samples. They estimated a 2- to 7-fold accounting for approximately 1% of the analysed mass though
increase in wet deposition using total acid digestion compared as mentioned are probably underestimated here. The other
with direct acidification. In this study the low percentage of significant minor elements in decreasing order are
total solids mass explained by the reconstructed mass is Zn > Mn > Sr > Ba > Pb > Cu > Cr > Se > Ni similar to a study in
probably from an underestimation of crustal matter due to Northern France (Deboudt et al., 2004). All other elements had
this. This deduction is supported by the relative mass of the an average flux of less than 1 mg/m2/d. Ag, Be, Hg, Th, Tl, U and
reconstructed soil fraction in this study being noticeably lower C2O24 were also analysed but below the MDL in all samples
than other urban aerosol mass closure studies (e.g. 8% and are thus not presented in Table 4.
compared to 22% of total mass) (Sillanpää et al., 2006). There The fluxes of many of the heavy metals measured in Bris-
may also be a minor systematic overestimation in the total bane are comparable to those in other cities as shown in Table
1636 water research 43 (2009) 1630–1640

Table 5 – Comparison of fluxes with other cities.

Reference Location As Cd Cr Cu Pb Zn THM
(mg/m2/d) (mg/m2/d) (mg/m2/d) (mg/m2/d) (mg/m2/d) (mg/m2/d) (mg/m2/d)

This study Brisbane (BD) 0.97 0.32 1.8 5.5 5.9 45.5 94#
Rossini et al. (2005) Venice (BD) 0.9 0.4 2.7 11.8 9.9 79.5
Sakata et al. (2008) Tokyo Bay (wet þ dry) 7.9 1.1 17.4 44.8 26.9 –
Azimi et al. (2005) Paris (BD) – – – – – – 282.2
Sabin et al. (2005) Los Angeles – – 1.3 9.3 5.5 39.7
(wet þ dry)
Lim et al. (2006) Los Angeles (dry) – – 4.6 21 19 120
Wu et al. (2006) Taiwan (dry) – – 11.2 21.9 56.0 109.0

BD ¼ bulk deposition sample, wet þ dry ¼ sum of separate wet and dry deposition samples, dry ¼ dry deposition only, THM – Total Heavy
Metals ¼ Sum Ba, Cd, Co, Cr, Cu, Ni, Mn, Pb, Sb, Sr, V, Ti and Zn fluxes, # – excluding Ti.

5 and are generally at the lower end of the scale. The study by
Sakata et al. (2008) in Tokyo Bay uses separate wet and dry
deposition samplers, the later using recirculated water, so
may be biased to higher dry deposition rates compared with
other sampling methods (Chu et al., 2008).
3.2.3. Effect of location on flux of metals
There was a statistically significant effect of location on the
annual mean daily flux of some elements and anions (see
Table 6). Specifically Li, Mn, Fe, Pb and SO2
4 were significantly
higher in city/heavy traffic/industrial sites compared to outer
suburban sites. Ba, Zn and Cu showed significant differences
in flux between sites in the order of city/heavy traffic/indus-
trial > inner suburban/traffic > outer suburban sites. Mean
daily flux of Sb and Sn was significantly higher in city/heavy
traffic/industrial sites but there was no significant difference
between inner or outer suburbs. Mean daily flux of K was
significantly lower in inner suburban sites compared to city/
high traffic/industrial or outer suburban sites as was the flux
of smoke after mass reconstruction (non-soil K). The mean
daily flux of crustal matter, sea salt and lead bromide using
the reconstructed mass was not significantly different
between site classes. Mean daily ammonium sulfate flux was
significantly higher in the inner city compared to outer sites,
with inner suburban/traffic sites midway between the two but
not significantly different from either. Elevated Zn and Cu in
deposition have been attributed to vehicles in urban envi-
ronments (Conko et al., 2004) and both Zn and Sb have been
proposed as marker elements for motor vehicle exhaust
emissions (Huang et al., 1994). Zn is also a component of tire
wear (Councell et al., 2004). Elevated atmospheric deposition
of heavy metals in the city centre compared to outer areas has
been found by other studies (Azimi et al., 2005). The elevated
zinc and antimony in higher traffic areas point toward the
importance of motor vehicles as a source of contaminants in
deposition.

3.2.4. Concentrations of metals in BD compared to ADWG

Table 6 – Annual mean daily flux of elements at site ADWG recommended levels were used as a maximum limit
categories. to assess potential health risk of consuming collected
deposition. It was found that Pb, Cd and Fe concentrations
Compound Outer Inner City/heavy
Suburban suburban/ traffic/light in BD exceeded the ADWG in 10.3%, 1.7% and 17.7% of
traffic industrial samples respectively. However, this was generally in drier
months when there was little wet deposition and hence no
Mean S.D. Mean S.D. Mean S.D.
dilution. This dilution effect is also reflected in the decline
K (mg/m2/d) 0.57a,b 2.70 0.43b 2.31 0.71a 3.02 of TS concentrations with increasing rainfall. In an empty
Li (mg/m2/d) 0.21a 2.01 0.23a,b 2.28 0.33b 2.14 tank the concentrations in rainfall may be significant, but
Mn (mg/m2/d) 9.08a 2.10 9.60a,b 1.97 14.65b 2.57
the volume of water collected during low rainfall periods
Fe (mg/m2/d) 157.1a 2.34 197.2a,b 2.22 255.1b 2.18
would mean it is easily diluted with any water already in
Cu (mg/m2/d) 2.69a 2.33 3.86b 2.16 5.91c 2.03
Zn (mg/m2/d) 21.52a 2.06 31.18b 1.69 57.34c 1.95 a tank. It is worth mentioning that the Fe guideline is based
Sb (mg/m2/d) 0.29a 2.39 0.33a 2.00 0.49b 2.34 on the taste threshold rather than health issues. When the
Ba (mg/m2/d) 3.35a 2.06 5.48b 1.79 8.58c 2.27 mean volume weighed concentrations over the year are
Pb (mg/m2/d) 2.14a 4.08 2.54a,b 3.57 4.18b 3.19 examined, the risk from consumption of heavy metals in
Sn (mg/m2/d) 0.17a 2.49 0.17a 2.71 0.29b 3.10 water from urban atmospheric deposition is small, as all
PO2 2
4 (mg/m /d) 0.19a,b 2.93 0.16a 2.51 0.30b 4.17
sites were below the ADWG. The concentrations of heavy
SO2 2
4 (mg/m /d) 2.21a 1.30 2.41a,b 1.26 2.95b 1.56
metals in deposition found in this study are comparable to
All mean and S.D. values calculated from log normal transformed others (Table 7). Annual volume weighed means reported
data and reconverted to normal values except for SO2
4 which was here are lower than the mean or median values used by
normally distributed and analysed untransformed. All units in mg/
some authors due the dilution effect of higher rainfall
m2/d excluding K, SO2 3 2
4 and PO4 which are in mg/m /d. Significant
periods decreasing the impact of small volumes of concen-
differences between groups indicated by superscripts (a, b, c).
trated deposition.
 water research 43 (2009) 1630–1640 1637

Table 7 – Mean (±S.D.) annual BD concentrations of heavy metals compared to other urban deposition studies.
Reference/metal Concentration of heavy metals in mg/L

As Cd Cr Cu Ni Pb Zn
a,d
Muezzinoglu and Cizmecioglu (2006) – 3.1 (1.6) 17.2 (8.6) 19.7 (25) 7.4 (2.6) 7.0 (4.1) 186.4(225.5)
Conko et al. (2004) a,c,e 0.10 (0.19) 0.06 (0.01) 0.17 (0.09) 0.76 (1.2) 0.27 (0.32) 0.47 (0.55) 4.4 (3.4)
(Deboudt et al. 2004) a,d – 12.4 (10) – 89.0 (120.7) – 580.2 (600.9) 1425 (2582.9
This study b,a,e,f 0.3 (0.3) 0.1 (0.1) 0.7 (1.0) 2.0 (0.9) 0.4 (0.1) 2.1 (0.7) 16.4 (10.1)

a Wet deposition.
b Bulk deposition.
c Annual volume weighed mean.
d Mean concentration.
e Suburban.
f Urban.

3.2.5. Concentrations of metal in urban rainwater tanks described in order to focus control measures. This was
compared to ADWG attempted with a case study of a newly installed tank with
The tank water concentrations demonstrate that tanks will a known history of no overflow during the first 11 months of the
not always have water meeting the ADWG (2004), particularly study period. Hence the majority of rainfall during the study
where there are major local sources or other inputs such as was mixed into the tank with minimal loss, approximating the
from roof materials. In fact, when tank water concentrations volume-weighed concentration in BD at the site. The volume-
are examined, Pb and Zn exceed the ADWG in 14.2% and 6.1% weighed concentration was calculated cumulatively for each
of samples respectively. Of these metals, Pb has the most month and plotted against the tank water concentration
potential for serious health effects, particularly where chil- measured at the same time and location. This cumulative
dren are drinking the water due to the permanent develop- event mean concentration of Pb in BD compared to the
mental neurological effects (Goyer, 1993). Consumption of Pb concentration in tank water at site 1# (Fig. 4). This is a volume
contaminated tank water has been shown to contribute to weighed average lead concentration (total deposited lead/total
elevated blood-Pb levels in children in Port Pirie, a town volume water deposited) in BD at the site at the given time
affected by lead smelter emissions (Body, 1986). In this study point. The important point in this diagram is that the BD
most samples of tank water had some detectable Pb but the concentrations are always less than the tank water concen-
majority were 2 mg/L (Fig. 3). However the range of concen- trations. Additionally, analysis of sludge from selected tanks
trations exceeding the ADWG was large, with 84.7 mg/L being shows further Pb is contained in the sludge. For example the Pb
the highest concentration of Pb in tank water in this study. concentration in sludge was 184 mg/g compared to a mean
water concentration of 0.5  0.8 mg/L from the same tank. This
3.2.6. Atmospheric deposition relative to tank is in agreement with Magyar et al. (2007) who found high
water concentrations concentrations of heavy metals in sludge of urban tanks. Hence
The relative importance of atmospheric deposition as a source Pb concentrations in the water represent a fraction of the total
of heavy metals, particularly Pb, to urban tanks needs to be Pb in a tank. The implication for the case study is that there are
major sources of Pb to the tank other than atmospheric depo-
sition. This site had a tile roof with 0.25 m2 of unpainted lead
Australian Drinking Water Guideline concentration

250

50
200
Number of samples

Lead concentration (µg/L)

40
150
30

100
20

Tank water concentration

50 10

BD volume weighed average

0 0
sampled
May-07

Aug-07

Nov-07

Mar-08
Dec-07
Sep-07

Feb-08
Oct-07
Jun-07

Jan-08
Jul-07
<=

10

12

14

16

18

>

Date
-4

-6

-8

-1

20
-1

-1

-1

-2
2

-1
0

0
4

Pb concentration (µg/L)
Fig. 4 – Comparative lead concentrations in tank water
Fig. 3 – Distribution of lead concentration in rainwater tank and bulk deposition (cumulative volume weighed mean)
samples. at site 1#.
1638 water research 43 (2009) 1630–1640
flashing on the roof catchment supplying the tank and is the
likely source of additional lead in the tank water (Magyar et al.,
2008). This is similar to Rocher et al. (2004) who found increased
Pb flux in runoff from a slate roof with lead flashing compared
to atmospheric deposition at the same site. When the 13 sites
where both tank water and BD were monitored 9 tanks had
a median Pb concentration near the annual volume weighed Pb
concentration in BD. Four tanks had concentrations far
exceeding the BD with three of the four tanks having Pb
flashing on the roof. However, one tank with a high median Pb
concentration did not have Pb flashing on the roof. This tank
was sampled at an unused tap positioned very close to the
bottom and probably had more sludge in the water sample
contributing to the elevated Pb. Apart from lead flashing, old
paint and Pb stabilised PVC drain pipes are other potential
sources of Pb (Al-Malack, 2001; Lasheen et al., 2008; Weiss et al.,
2006).
4. Conclusion
This study demonstrates atmospheric deposition does
contribute to contaminants in rainwater in an urban envi-
ronment. It shows that there is an increase in the
contaminant flux in traffic/industrial areas compared to
outer suburbs with marker elements implicating traffic as
a major contributor. Rainwater collected in urban areas
where air pollution is significant must consider the impact
of pollution on the water quality. Despite the measurable
effect of urban activity on contaminant flux, for a sub-
tropical city of nearly 2 million people the chemical water
quality of urban rainwater over annual time periods could
still be considered as potable. However, the quality of water
collected in a tank may not reflect that of the rainwater,
with Pb exceeding drinking water guidelines most
commonly. This is due to input of contaminants from other
sources such as roof materials. A probabilistic health risk
using the distribution of Pb concentrations in tank water
coupled with tank owner’s consumption patterns is needed
to assess if there is a likely impact on the health of the
general population. In this study atmospheric deposition is
not the major source of Pb in tanks with high concentra-
tions as indicated by comparison with the annual volume
weighed concentrations in rainfall collected at the same
sites. The exact source of this lead in tank water is not
proven in this study. Lead flashing is potentially the source
in the case study shown. The application of multivariate
receptor modelling tools and Pb isotope ratios to identify
and quantify the sources of Pb in tank water is currently
underway. Identification of the source(s) of Pb in tank water
is necessary for targeting control measures for an otherwise
good quality water source. Lastly, the impact of Pb in sludge
and the partitioning between sludge and the water column
needs further study to assess the usefulness of removing
sludge for decontamination. A device that discards the
initial runoff from the roof (first flush device) may reduce
sludge build up and improve water quality somewhat for
particulate Pb but is unlikely to result in sufficient reduction
of soluble Pb (Gardner et al., 2004).
Acknowledgments
This study was supported by the CRC for Water Quality and
Treatment, a Smart State grant from the Queensland
Government and The National Research Centre for Envi-
ronmental Toxicology. We would like to thank the
Queensland EPA for use of their air monitoring stations for
sampling.
Supplementary data
Supplementary data associated with this article can be found,
in the online version, at doi:10.1016/j.watres.2008.12.045.
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