w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9

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journal homepage: www.elsevier.com/locate/watres

The effect of roofing material on the quality of harvested

rainwater

Carolina B. Mendez a, J. Brandon Klenzendorf a,1, Brigit R. Afshar a,2, Mark T. Simmons b,
Michael E. Barrett a, Kerry A. Kinney a, Mary Jo Kirisits a,*
a
Department of Civil, Architectural, and Environmental Engineering, The University of Texas at Austin, 1 University Station C1786,
Austin, TX 78712, USA
b
Lady Bird Johnson Wildflower Center, The University of Texas at Austin, 4801 La Crosse Avenue, Austin, TX 78739, USA

article info abstract

Article history: Due to decreases in the availability and quality of traditional water resources, harvested
Received 7 November 2010 rainwater is increasingly used for potable and non-potable purposes. In this study, we
Received in revised form examined the effect of conventional roofing materials (i.e., asphalt fiberglass shingle,
15 December 2010 Galvalume
metal, and concrete tile) and alternative roofing materials (i.e., cool and green) on
Accepted 16 December 2010 the quality of harvested rainwater. Results from pilot-scale and full-scale roofs demonstrated
Available online 22 December 2010 that rainwater harvested from any of these roofing materials would require treatment if the
consumer wanted to meet United States Environmental Protection Agency primary and
Keywords: secondary drinking water standards or non-potable water reuse guidelines; at a minimum,
Rainwater harvesting first-flush diversion, filtration, and disinfection are recommended. Metal roofs are commonly
Roof-runoff recommended for rainwater harvesting applications, and this study showed that rainwater
Water quality harvested from metal roofs tends to have lower concentrations of fecal indicator bacteria as
First-flush compared to other roofing materials. However, concrete tile and cool roofs produced harvested
Roofing material rainwater quality similar to that from the metal roofs, indicating that these roofing materials
Potable also are suitable for rainwater harvesting applications. Although the shingle and green roofs
produced water quality comparable in many respects to that from the other roofing materials,
their dissolved organic carbon concentrations were very high (approximately one order of
magnitude higher than what is typical for a finished drinking water in the United States), which
might lead to high concentrations of disinfection byproducts after chlorination. Furthermore
the concentrations of some metals (e.g., arsenic) in rainwater harvested from the green roof
suggest that the quality of commercial growing media should be carefully examined if the
harvested rainwater is being considered for domestic use. Hence, roofing material is an
important consideration when designing a rainwater catchment.
ª 2011 Elsevier Ltd. All rights reserved.

1. Introduction harvesting is undergoing a surge in popularity in the United

States, particularly in locations where traditional, high-quality
Roof-based rainwater harvesting is the capture of rain- freshwater supplies are absent or where consumers desire to
water from a roof for potable or non-potable use. Rainwater contribute to sustainability. The United States Environmental

* Corresponding author. Tel.: þ1 512 232 7120; fax: þ1 512 471 0592.
E-mail address: kirisits@mail.utexas.edu (M.J. Kirisits).
1
Present address: Geosyntec Consultants, 3600 Bee Caves Road, Suite 101, Austin, TX 78746, USA.
2
Present address: CH2M Hill, 12377 Merit Drive, Ste. 1000, Dallas, TX 75251, USA.
0043-1354/$ e see front matter ª 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.watres.2010.12.015
2050 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9
Nomenclature
cm centimeter
CFU colony forming unit
 %
degree angle
 PAH
C degrees Celsius
DOC dissolved organic carbon
FC fecal coliform
h hour
km kilometer
L liter
MCL maximum contaminant level
mg/L microgram per liter
mS/cm microsiemens per centimeter
mg-N/L milligram of nitrogen per liter
mg/L milligram per liter
Protection Agency (USEPA) does not regulate the water quality
of residential rainwater harvesting systems in the U.S., but
some state and local agencies do issue voluntary water quality
guidelines for residential rainwater harvesting systems (e.g.,
Texas Rainwater Harvesting Evaluation Committee, 2006). The
quality of harvested rainwater is of great importance because it
is increasingly used for domestic purposes.
Several types of chemical contaminants have been found in
harvested rainwater including heavy metals (Förster, 1999; Lee
et al., 2010), polycyclic aromatic hydrocarbons (PAHs) (Förster,
1998, 1999), pesticides (Zobrist et al., 2000), and herbicides
(Bucheli et al., 1998). Microorganisms also are present in roof-
runoff, and fecal indicator bacteria and potentially pathogenic
bacteria and protozoa have been detected (Ahmed et al., 2008).
The type of roofing material used for the catchment can
affect the quality of harvested rainwater. Nicholson et al.
(2009) compared harvested rainwater quality among six roof
types: galvanized metal, cedar shake, asphalt shingle, two
types of treated wood, and green (i.e., vegetated). The galva-
nized metal, asphalt shingle, and green roofs neutralized the
acidic rainwater to a greater extent than did the other roofing
materials. The treated woods yielded the highest copper
concentrations (mg/L range), and the galvanized metal yiel-
ded the highest zinc concentrations (mg/L range), as com-
pared to the mg/L concentrations of these metals from the
other roofing materials. Van Metre and Mahler (2003) found
galvanized metal roofs to be a source of particulate zinc and
cadmium and asphalt shingle roofs to be a source of partic-
ulate lead and potentially mercury. Kingett Mitchell Ltd.
(2003) found higher zinc concentrations in rainwater har-
vested from painted galvanized iron roofs that showed
evidence of weathering as compared to those in excellent
condition. Despins et al. (2009) found that harvested rain-
water quality from steel roofs was superior to that from
asphalt shingle roofs, particularly with respect to turbidity,
total organic carbon, and color.
Most studies to date have focused on examining conven-
tional roofing materials, such as galvanized metal, for rain-
water harvesting. Green roofs are increasingly being installed
for their stormwater retention characteristics, and both green
and cool roofs (made of reflective roofing material) are being
installed for their energy conservation potential; however,
mL milliliter
mm millimeter
NTU nephelometric turbidity unit
percent
polycyclic aromatic hydrocarbon
PVC polyvinyl chloride
SMCL secondary maximum contaminant level
SVOC semi-volatile organic compound
a significance level
m2 square meter
TC total coliform
TDS total dissolved solids
TSS total suspended solids
USEPA United States Environmental Protection Agency
VOC volatile organic compound
neither has been widely considered for rainwater harvesting.
To our knowledge, only one study has analyzed harvested
rainwater quality from a green roof (Nicholson et al., 2009),
and it was examined in the context of non-potable use.
The objective of the current study was to thoroughly
examine the effect of roofing material on the quality of har-
vested rainwater (untreated, except for the use of a first-flush
diverter) from the standpoint of suitability for domestic use.
Five co-located pilot-scale roofs were used to compare har-
vested rainwater quality among conventional roofing mate-
rials (i.e., asphalt fiberglass shingle, Galvalume
metal, and
concrete tile) and alternative roofing materials (i.e., cool and
green). This is the first study to extensively compare harvested
rainwater quality (20 water quality parameters) among these
conventional and alternative roofing materials. In addition, the
quality of the rainwater harvested from the asphalt fiberglass
shingle and Galvalume
roofing materials was compared
between the pilot-scale roofs and full-scale residential roofs.
2. Materials and methods
2.1. Study sites
This study was conducted in Austin, Texas, where the mean
annual rainfall is 856 mm (National Oceanic and Atmospheric
Administration, 2010). The pilot-scale roofs were constructed
at the Lady Bird Johnson Wildflower Center (Austin, TX), and
the full-scale residential roofs were located within 42 km of
the pilot site.
2.2. Pilot-scale roofs
The conventional pilot-scale roofs, constructed in 2009, were
made of asphalt fiberglass shingle (GAF-Elk, Wayne, NJ),
Galvalume
(55% aluminum-zinc alloy coated steel, United
States Steel Corporation, Pittsburgh, PA), or concrete tile
(MonierLifetile, Irvine, CA) (Fig. 1A). They were angled 18.4
from the horizontal, with a footprint area of 2.8 m2. The alter-
native pilot-scale roofs, constructed in 2007 as described by
Simmons et al. (2008), were an unfertilized (type E) green roof
(Fig. 1B) and an acrylic-surfaced, 2-ply atactic polypropylene
 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9 2051

Fig. 1 e Pilot-scale roofs (A) from left to right: asphalt fiberglass shingle, metal, concrete tile, (B) green, and (C) cool.

modified bituminous membrane cool roof (Fig. 1C); these low- sampler, first-flush bottle, and first and second tanks were
slope roofs were angled 1.2 from the horizontal, with a foot- analyzed in triplicate for pH, conductivity, total coliform
print area of 3.4 m2. All of the pilot-scale roofs faced north. (TC), fecal coliform (FC), turbidity, total suspended solids
(TSS), dissolved organic carbon (DOC), and nine metals
2.3. Full-scale residential roofs (dissolved þ particulate): aluminum, arsenic, cadmium, chr-
omium, copper, iron, lead, selenium, and zinc. Nitrate and
Three full-scale residential roofs were sampled: a 12-year-old nitrite were measured once for each sample. For the fourth
Galvalume
roof (22 from the horizontal, footprint area of rain event, samples from the ambient sampler and first-flush
4.3 m2), a 5-year-old asphalt fiberglass shingle roof (23 from bottle were analyzed for pesticides and PAHs.
the horizontal, footprint area of 4.3 m2) and another 5-year-old Rainwater harvested from the full-scale roofs was sampled
asphalt fiberglass shingle roof (18 from the horizontal, foot- during three rain events in 2009: February 9, February 11, and
print area of 5.3 m2). All of the full-scale roofs faced north. March 11. For all three rain events, the ambient sampler, first-
flush bottle, and first and second tanks were analyzed in tripli-
cate for TC, FC, TSS, DOC, lead, and zinc. The pH, conductivity,
2.4. Rainwater sampling devices
turbidity, nitrate, and nitrite were measured once for each
sample. For the first rain event, samples from the ambient
A sampling insert (7.6-cm inner-diameter potable-quality
sampler and first-flush bottle were analyzed for a suite of volatile
polyvinyl chloride (PVC) pipe cut lengthwise in half) was placed
and semi-volatile organic compounds (VOCs and SVOCs).
in the gutters of the conventional pilot-scale and full-scale
At the end of each rain event, samples were transported to
roofs. The sampling insert drained to a passive collection
the laboratory for analysis. The pH, conductivity, TC, FC,
system consisting of a 2-L glass bottle to collect the “first-flush”
turbidity, and TSS were analyzed immediately upon arrival at
and two 10-L polypropylene tanks in series (Fig. 2). The first-
the laboratory. The pH was measured with a combination
flush volume was designed according to the Texas Water
electrode and meter (Model 920A, Orion Research Inc., Boston,
Development Board guidelines, which state that the first-flush
should divert a minimum of 38 L for every 93 m2 of collection
area (Texas Water Development Board, 2005). For the alterna-
tive pilot-scale roofs, the drainage system described in
Simmons et al. (2008) emptied to the aforementioned passive
collection system. The first-flush bottle and tanks in the passive
collection system filled sequentially during a rain event, with
excess rainfall exiting the system through an overflow spout
(Fig. 2). A 46-cm inner-diameter polyethylene funnel attached to
a 10-L polypropylene tank was used as an ambient sampler to
collect rainwater without roof exposure; the cover on the funnel
was removed up to 24 h prior to a rain event, so some atmo-
spheric deposition was possible. Between rain events, the
sampling devices were washed and rinsed, and the collection
bottle and tanks were autoclaved. Rainfall was measured with
a rain gauge, and the sampled events had rainfalls between
25 mm and 38 mm at the pilot-scale and full-scale sites.

2.5. Sampling and analytical methods

Rainwater harvested from the pilot-scale roofs was sampled

during four rain events in 2009: April 18, June 11, July 23, and
September 11. For the first three rain events, the ambient Fig. 2 e Schematic of the sampling device.
2052 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9
MA). Conductivity was measured with a conductivity meter
(Model CDM 230, Radiometer Analytical, Lyon, France). TC was
measured according to method 9222B (American Public Health
Association, 1998) with m-Endo broth (Millipore, Billerica, MA),
and FC was measured according to method 9222D (American
Public Health Association, 1998) with m-FC agar (Difco,
Detroit, MI). Turbidity was measured with a turbidimeter (Model
2100A, Hach, Loveland, CO). TSS was measured according to
method 2540B (American Public Health Association, 1998).
Samples for the remaining analytes were preserved for
later analysis. Samples for nitrate and nitrite analysis were
stored at 4  C and analyzed within 48 h with Test 0 N Tube
Reactor/Cuvette Tubes (Hach, Loveland, CO); nitrate was
measured with the NitraVer
X reagent set, and nitrite was
measured with the NitriVer
3 reagent set according to the
manufacturer’s instructions. Samples for DOC analysis were
stored at 4  C after addition of reagent grade phosphoric acid;
DOC was measured with an Apollo 9000 Combustion Analyzer
(Tekmar-Dohrmann, Cincinnati, OH). Samples for metal
analysis were preserved with trace metal grade nitric acid.
For the pilot-scale study, metal concentrations were mea-
sured by inductively coupled plasma-mass spectrometry
(Model 7500ce, Agilent Technologies, Inc., Tokyo, Japan). For
the full-scale study, metal concentrations were measured by
graphite furnace atomic absorption spectroscopy (Model
AAnalyst 600, PerkineElmer, Waltham, MA).
At the end of the February 9 and September 11, 2009 rain
events, samples were delivered to DHL Analytical (Round
Rock, TX) for the analysis of organic compounds. Pesticides
were measured according to method 8081A (USEPA, 1996a);
SVOCs and PAHs were measured according to method 8270C
(USEPA, 1996b); VOCs were measured according to method
8260B (USEPA, 1996c).
2.6. Statistical analysis
The nonparametric Mann-Whitney test was used to make
comparisons among the data because of the small number of
rainfall events and the inability to show that the water quality
Fig. 3 e Average pH (panel A) and conductivity (panel B) for the pilot-scale events: ( ) Quality of the first-flush, ( )
Quality after the first-flush (average of tank 1 and tank 2),  USEPA secondary drinking water standard range for pH
(6.5e8.5), - - - Ambient sampler. One standard deviation is shown.
data could be characterized by a normal distribution. A
significance level of a ¼ 0.1 was used.
Since the consumer often diverts the first-flush water from
use, the discussion in this study generally focuses on the
quality of the rainwater harvested after the first-flush (i.e.,
tanks 1 and 2 in Fig. 2). The quality of the rainwater harvested
after the first-flush was compared to the quality of the first-
flush, to the quality of rainwater captured by the ambient
sampler, to the U.S. drinking water standards, and to the U.S.
non-potable urban water reuse guidelines. Finally, the quality
of the rainwater harvested after the first-flush was compared
among the roofing materials.
3. Results and discussion
3.1. pH and conductivity e pilot-scale roofs
The average pH of rainfall collected in the ambient sampler
was 6.1, and all of the harvested rainwater samples from the
pilot-scale roofs were in the near-neutral range (Fig. 3A). For
all of the pilot-scale roofs except the metal roof, the pH of the
rainwater harvested after the first-flush was significantly
higher than that in the ambient sampler ( p-values < 0.048).
Similarly, other studies have reported an increase in pH from
ambient rainwater to harvested rainwater (Kingett Mitchell
Ltd., 2003). The pH of the rainwater harvested after the first-
flush for the tile roof was significantly higher than those of the
other pilot-scale roofs ( p-values < 0.021). This was expected
due to the alkaline nature of concrete and is consistent with
other studies (Kingett Mitchell Ltd., 2003). The average pH of
the rainwater harvested after the first-flush for all pilot-scale
roofs met the USEPA secondary drinking water standard range
of 6.5e8.5 (Fig. 3A) and the non-potable urban water reuse
guideline range of 6.0e9.0 (USEPA, 2004).
The average conductivity of rainfall collected in the amb-
ient sampler was 34 mS/cm (Fig. 3B), which is in the typical
range for ambient rainwater (Yaziz et al., 1989; Lee et al., 2010).
For the green roof only, the conductivity of the rainwater
 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9
harvested after the first-flush was significantly higher than
that in the ambient sampler ( p-value ¼ 0.012). The conduc-
tivity of the rainwater harvested after the first-flush for the
green roof also was significantly higher than those for the
other pilot-scale roofs ( p-values < 0.013); this was expected
due to mineral dissolution as the rainwater passed through
the growing media of the green roof. For the shingle, metal,
and cool pilot-scale roofs, the conductivity of the first-flush
was significantly higher than that of the rainwater harvested
after the first-flush ( p-values < 0.024).
Conductivity and total dissolved solids (TDS) are corre-
lated, although a specific correlation was not prepared in this
study. Using the correlation of Singh and Kalra (1975) between
conductivity and TDS in mountain streams, the average,
estimated TDS of rainwater harvested after the first-flush for
all pilot-scale roofs met the USEPA secondary maximum
contaminant level (SMCL) for TDS, which is 500 mg/L.
3.2. TC and FC e pilot-scale roofs
The harvested rainwater was assessed using TC (Fig. 4A) and
FC (Fig. 4B) as indicators of microbial quality.
For the shingle, tile, and cool pilot-scale roofs, the TC
concentration of the first-flush was significantly higher than
that of the rainwater harvested after the first-flush ( p-
values < 0.024), but the TC concentration from the metal and
green pilot-scale roofs did not change significantly from the
first-flush to the subsequent tanks ( p-values ¼ 0.131 and 0.179,
respectively). For all of the pilot-scale roofs, the TC concentra-
tion of the rainwater harvested after the first-flush was statis-
tically indistinguishable from that in the ambient sampler
( p-values > 0.131). According to the USEPA primary drinking
water standards, no more than five percent of samples in
a month are allowed to be positive for TC; all of the pilot-scale
roofs violate this standard because they showed measurable TC
in the first-flush and subsequent tanks for all rain events.
For the shingle, metal, tile, and cool pilot-scale roofs, the
FC concentration of the first-flush was significantly higher
than that of the rainwater harvested after the first-flush
( p-values < 0.083). For all of the pilot-scale roofs except the
metal roof, the FC concentration of the rainwater harvested
Fig. 4 e Geometric mean of TC (panel A) and FC (panel B) for the pilot-scale events: ( ) Quality of the first-flush, ( ) Quality
after the first-flush (average of tank 1 and tank 2), - - - Ambient sampler. One geometric standard deviation is shown.
2053
after the first-flush was statistically indistinguishable from
that in the ambient sampler ( p-values > 0.179). According to
the USEPA primary drinking water standards, if two consec-
utive samples have TC and at least one of them has FC (or
Escherichia coli), then the system has an acute maximum
contaminant level (MCL) violation; all of the pilot-scale roofs
violate this standard. Only the rainwater harvested after the
first-flush from the metal roof meets the non-potable urban
water reuse guidelines (USEPA, 2004), which state that FC
should not exceed 14 colony forming units (CFU)/100 mL in
any sample.
Our data are consistent with the literature, which shows
detectable TC and FC in harvested rainwater (Yaziz et al., 1989;
Simmons et al., 2001). The use of these traditional indicator
bacteria might cause the underestimation of the risk of
waterborne disease to the rainwater consumer (Lye, 2002;
Ahmed et al., 2008). Nonetheless, based on the TC and FC
concentrations in the rainwater harvested after the first-flush,
most of the pilot-scale roofs produced water that did not meet
potable and non-potable guidelines. Thus treatment is needed
if the guidelines are to be met.
Due to filtration of the rainwater through the substrate
layer, we expected the pilot-scale green roof to consistently
yield the lowest concentrations of indicator bacteria in har-
vested rainwater, but this was not always the case. For
instance, while the first two rain events showed no detectable
FC in the rainwater harvested from the green roof, the third
rain event showed a spike in FC (330 CFU/100 mL) in the
rainwater harvested after the first-flush. The third rain event
also showed a spike in TC concentrations from the green roof
but no spikes in TSS or turbidity (data not shown). The other
pilot-scale roofs did not have similar contaminant spikes in
the third rain event; thus, the reason for the spike in indicator
bacteria concentrations in this event from the green roof is
unclear at this time. On a per-event basis, the green roof most
often showed the best water quality with respect to indicator
bacteria among the roofing materials, but the potential for
spikes in indicator bacteria concentrations from the green
roof should be investigated further.
For the pilot-scale metal roof, the FC concentration of the
rainwater harvested after the first-flush was significantly
2054 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9
lower than that in the ambient sampler ( p-value ¼ 0.083). The
TC and FC concentrations of the first-flush from the metal roof
were significantly lower than those for the cool, shingle, and
tile roofs ( p-values < 0.001). Similarly, Yaziz et al. (1989)
showed that the concentration of indicator bacteria in rain-
water harvested from metal roofs was lower than that from
concrete tile roofs. One possible reason for this trend is that
low emissivity materials, like metals, have higher surface
temperatures in sunlight (Bretz et al., 1998), which might
have inactivated a fraction of the indicator bacteria. Another
possible reason for this trend is that heavy metal exposure
can decrease cellular viability (Teitzel and Parsek, 2003), so
contact with the metal roofing material might have inacti-
vated a fraction of the indicator bacteria.
3.3. Turbidity and TSS concentrations e pilot-scale roofs
Turbidity (Fig. 5A) and TSS concentrations (Fig. 5B) were
measured for the pilot-scale roofs.
For all of the pilot-scale roofs, the turbidity of the first-flush
was significantly higher than that of the rainwater harvested
after the first-flush ( p-values < 0.083). The turbidity of the
first-flush from the metal and cool pilot-scale roofs was
significantly higher than those for the shingle, tile, and green
pilot-scale roofing materials ( p-values < 0.001). This was
expected because the metal and cool roofs visually had the
smoothest surfaces, and Egodawatta et al. (2009) noted that
particulate matter washes off from smoother surfaces more
rapidly than it does from rougher surfaces. For the tile, cool,
and green pilot-scale roofs, the turbidity of the rainwater
harvested after the first-flush was statistically indistinguish-
able from that in the ambient sampler ( p-values > 0.131). The
turbidity of the rainwater harvested after the first-flush for the
green roof was lower than that for the shingle, metal, and tile
pilot-scale roofs but indistinguishable from that of the cool
pilot-scale roof ( p-values < 0.078); thus, the green roof
produced the highest quality rainwater with respect to
turbidity.
According to the USEPA primary drinking water standards,
for systems using conventional or direct filtration, turbidity
Fig. 5 e Average turbidity (panel A) and TSS concentrations (panel B) for the pilot-scale events: ( ) Quality of the first-flush,
( ) Quality after the first-flush (average of tank 1 and tank 2),  USEPA filtered system guideline (1 NTU), - - - Ambient
sampler. One standard deviation is shown.
must never be above 1 nephelometric turbidity unit (NTU),
and 95% of samples in one month must be less than or equal
to 0.3 NTU. According to the non-potable urban water reuse
guidelines (USEPA, 2004), the average turbidity in a 24-h period
should be less than or equal to 2 NTU and turbidity should not
exceed 5 NTU at any time. All samples of rainwater harvested
after the first-flush from the pilot-scale roofs violate these
standards.
The TSS data showed very similar trends to the turbidity
data. For example, the TSS of the rainwater harvested after
the first-flush for the green roof was lower than those for the
other pilot-scale roofs ( p-values < 0.047); thus, the green roof
produced the highest quality rainwater with respect to TSS.
No primary or secondary drinking water standards exist for
TSS. The non-potable urban water reuse guidelines state that
TSS should not exceed 5 mg/L (USEPA, 2004); the rainwater
harvested after the first-flush for all pilot-scale roofs often
exceeded this standard.
Based on the turbidity and TSS concentrations in the
rainwater harvested after the first-flush, all of the pilot-scale
roofs produced water that did not meet potable and non-
potable guidelines. Thus, treatment is needed if the guidelines
are to be met.
3.4. Nitrate and nitrite concentrations e pilot-scale roofs
Nitrate (Fig. 6A) and nitrite (Fig. 6B) concentrations were
measured for the pilot-scale roofs.
For the shingle, metal, and tile pilot-scale roofs, the average
nitrate concentration of the first-flush was significantly higher
than that of the rainwater harvested after the first-flush
( p-values < 0.082). For all of the pilot-scale roofs, the average
nitrate concentration of the rainwater harvested after the first-
flush was statistically indistinguishable from that in the
ambient sampler ( p-values > 0.25). Elevated nitrate levels were
not expected in the rainwater harvested from the green roof
because no fertilizers were applied to the green roof, and plants
and soil biota can consume nitrate. All samples of the rain-
water harvested after the first-flush for all pilot-scale roofs met
the USEPA MCL for nitrate (10 mg-N/L), consistent with the
 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9
Fig. 6 e Average nitrate (panel A) and nitrite (panel B) concentrations for the pilot-scale events: ( ) Quality of the first-flush,
( ) Quality after the first-flush (average of tank 1 and tank 2),  USEPA MCLs for nitrate (10 mg-N/L) and nitrite (1 mg-N/L),
- - - Ambient sampler. One standard deviation is shown.
findings of Nicholson et al. (2009) for asphalt fiberglass shingle,
metal, and green roofs.
The average concentration of nitrate in the first-flush from
all of the pilot-scale roofs was greater than the average nitrate
concentration in the ambient sampler (Fig. 6A), which is likely
due to dry deposition of nitrate onto the roof surfaces (Förster,
1998). The nitrate concentrations in the first-flush increased
from 4 to 8 antecedent dry days and then either reached
a plateau or continued to increase from 8 to 14 antecedent dry
days (Fig. 7), supporting the hypothesis that dry deposition
contributes to nitrate levels in harvested rainwater.
For all of the pilot-scale roofs, the average nitrite concen-
tration of the first-flush was significantly higher than that of
the rainwater harvested after the first-flush ( p-values < 0.083).
For the metal, cool, and green pilot-scale roofs, the average
nitrite concentration of the rainwater harvested after the first-
flush was statistically indistinguishable from that in the
ambient sampler ( p-values > 0.25), and the shingle and tile
pilot-scale roofs produced nitrite concentrations in the rain-
water harvested after the first-flush that were just slightly
higher than ambient ( p-values < 0.083). All samples of the
rainwater harvested after the first-flush for all pilot-scale roofs
met the USEPA MCL for nitrite (1 mg-N/L).
3.5. DOC concentrations e pilot-scale roofs
DOC concentrations were measured for the pilot-scale roofs
(Fig. 8). For the metal and cool roofs, the average DOC concen-
tration of the first-flush was significantly higher than that of the
rainwater harvested after the first-flush ( p-values < 0.048). For
the metal, tile, and cool pilot-scale roofs, the average DOC
concentration of the rainwater harvested after the first-flush
was statistically indistinguishable from that in the ambient
sampler ( p-values > 0.33). Conversely, for the shingle and green
pilot-scale roofs, the average DOC concentration in the rain-
water harvested after the first-flush was significantly higher
than that in the ambient sampler ( p-values < 0.012). In fact,
the shingle pilot-scale roof showed a significant increase in
DOC concentration from rainwater in the first-flush tank to
the rainwater harvested after the first-flush ( p-value < 0.012).
The green roof showed statistically significant higher DOC
2055
concentrations in the rainwater harvested after the first-
flush as compared to all of the other pilot-scale roofs ( p-
values < 0.047). Given the nature of the roofing materials, the
shingle and green pilot-scale roofs were expected to be sources
of organic matter. Asphalt fiberglass shingles are noted for
producing colored water (Despins et al., 2009). Berndtsson et al.
(2009) hypothesized that the elevated DOC concentrations
observed in green roof-runoff come from the soil organic matter
and from decay of the vegetation. DOC also might be produced
by soil bacteria colonizing the green roof. The DOC concentra-
tions in the rainwater harvested after the first-flush for the
shingle and green roofs were elevated as compared to the DOC
concentration of a typical, finished drinking water in the U.S.
(w2.5e3.5 mg/L).
Although DOC does not have an MCL, it is a precursor for
regulated disinfection byproducts (e.g., trihalomethanes and
haloacetic acids). To reduce disinfection byproduct formation,
the Stage 1 Disinfectants/Disinfection Byproducts Rule
mandates that water systems that treat with disinfectants
other than ultraviolet light must reduce the total organic
carbon of the water by 15e50%, where the percentage is based
Fig. 7 e Effect of antecedent dry days on average nitrate
concentrations in first-flush samples from the pilot-scale
roofs: dCd Shingle, dBd Metal, d;d Tile, d6d Cool,
d-d Green,  USEPA MCL for nitrate (10 mg-N/L).
2056 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9
Fig. 8 e Average DOC concentrations for the pilot-scale
events: ( ) Quality of the first-flush, ( ) Quality after the
first-flush (average of tank 1 and tank 2), - - - Ambient
sampler. One standard deviation is shown.
on the total alkalinity and source water total organic carbon
concentration. Thus, systems with high source water total
organic carbon concentrations (>8 mg/L) must decrease the
total organic carbon by 30e50%. Given the particularly high
DOC concentrations in the rainwater harvested after the first-
flush from the shingle and green roofs, it is quite possible that
the concentrations of disinfection byproducts formed in these
waters would violate the primary drinking water standards. If
the water is used for non-potable purposes, the consumer also
might come into contact with these disinfection byproducts by
inhalation, since many of them are volatile (e.g., chloroform).
3.6. Metal concentrations e pilot-scale roofs
The average concentrations of cadmium, chromium, and
selenium in the rainwater harvested after the first-flush for
each pilot-scale roof were at least an order of magnitude below
the corresponding primary drinking water standard (data not
shown); these metals are not discussed further. Data for the
remaining metals (aluminum, arsenic, copper, iron, lead, and
zinc) are shown in Fig. 9.
In general, the average concentration of each metal in the
first-flush was significantly higher than that in the rainwater
harvested after the first-flush at a 10% significance level. The
notable exception to this is the green roof, where the metal
concentrations (except for lead) in the first-flush were statis-
tically indistinguishable from those in the rainwater har-
vested after the first-flush at a 10% significance level.
In general, the average concentration of each metal in the
rainwater harvested after the first-flush was significantly
less than or statistically indistinguishable from that in the
ambient sampler at a 10% significance level, with three
notable exceptions. First, the rainwater harvested after the
first-flush from the tile and green roofs had arsenic and
lead concentrations that were significantly higher than those
in the ambient sampler ( p-values < 0.083). Second, the rain-
water harvested after the first-flush from the metal, tile, and
green roofs had zinc concentrations that were significantly
higher than those in the ambient sampler ( p-values < 0.083).
The elevated arsenic, lead, and zinc found in the rainwater
harvested from the green roof are hypothesized to have come
from the growing media, which suggests that the quality of
commercial growing media must be carefully examined if the
harvested rainwater is being considered for domestic use.
Third, the rainwater harvested after the first-flush from the
shingle roof had copper concentrations that were significantly
higher than that in the ambient sampler ( p-value ¼ 0.012) and
those from all of the other pilot-scale roofs ( p-values < 0.001),
suggesting that the shingle roof is a source of copper. This is
consistent with the study of Nicholson et al. (2009), which
showed that rainwater harvested from asphalt fiberglass
shingle roofs contained more copper than did rainwater har-
vested from galvanized metal or green roofs. In other studies,
elevated copper in roof-runoff was attributed to atmospheric
deposition due to vehicles (Van Metre and Mahler, 2003) and
copper fittings (Förster, 1999), but those sources were not
present at our pilot-scale site.
The concentration of each metal in the rainwater harvested
after the first-flush was compared to the appropriate USEPA
primary and secondary drinking water standards or action
levels (Fig. 9). None of the pilot-scale roofs violated the primary
standards or action levels for the rainwater harvested after the
first-flush (i.e., arsenic, copper, and lead). However, aluminum
(Fig. 9A) and iron (Fig. 9D) concentrations in the rainwater
harvested after the first-flush often exceeded the secondary
standards. All of the pilot-scale roofs violated the aluminum
SMCL of 200 mg/L in the rainwater harvested after the first-flush.
Only the green pilot-scale roof did not violate the iron SMCL of
300 mg/L in the rainwater harvested after the first-flush.
Zinc concentrations in the rainwater harvested after the
first-flush from all roofing materials were at least one order of
magnitude below the zinc secondary drinking water standard
(Fig. 9F). Previous studies have shown that galvanized metal
roofs (Kingett Mitchell Ltd., 2003; Nicholson et al., 2009) or
painted galvanized metal roofs in less-than-excellent condition
(Kingett Mitchell Ltd., 2003) yield high concentrations of zinc
(mg/L) in harvested rainwater. Conversely, painted galvanized
metal roofs in excellent condition and Zincalume
(55%
aluminum-zinc alloy coated steel, which is the same compo-
sition as Galvalume
) roofs yield lower concentrations of zinc
(mg/L) in harvested rainwater (Kingett Mitchell Ltd., 2003),
similar to our data from the Galvalume
roof. This is consistent
with the work of Sullivan and Worsley (2002), who found that
the presence of aluminum in alloy-coated steel roofs increases
the corrosion resistance as compared to uncoated galvanized
roofs, thereby decreasing the zinc concentration in roof-runoff.
In terms of primary standards and action levels for metals
in drinking water, all of the pilot-scale roofs produced
acceptable quality water. The green pilot-scale roof produced
the best quality water in terms of secondary standards, as its
aluminum and iron concentrations in the rainwater harvested
after the first-flush were the lowest as compared to the other
pilot-scale roofs.
3.7. Water quality ranges e comparing full-scale and
pilot-scale roofs
Previous studies have shown that variation in roof-runoff
quality is attributable to the age of the roof, presence of over-
hanging vegetation, wind direction, and proximity to local
 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9 2057

Fig. 9 e Average total aluminum (panel A), arsenic (panel B), copper (panel C), iron (panel D), lead (panel E), and zinc (panel F)
concentrations for the pilot-scale events: ( ) Quality of the first-flush, ( ) Quality after the first-flush (average of tank 1 and
tank 2),  USEPA primary or secondary drinking water standards or action levels: aluminum (200 mg/L), arsenic (10 mg/L),
copper (1300 mg/L), iron (300 mg/L), lead (15 mg/L), and zinc (5000 mg/L). - - - Ambient sampler. One standard deviation is
shown.

sources (Förster, 1999; Kingett Mitchell Ltd., 2003; Evans et al., shingle roofs at a concentration of 3 mg/L; benzyl alcohol also
2006). In contrast to the pilot-scale roofs, our full-scale roofs was detected in the first-flush from the same shingle roof at
were older, had overhanging vegetation, and were located a concentration of 0.20 mg/L. These compounds are both
closer to local emission sources (e.g., chimneys and traffic). unregulated in drinking water. Our lack of detection of PAHs
Despite these differences, the qualities of the rainwater in harvested rainwater is consistent with Van Metre and
harvested after the first-flush from the pilot-scale and full- Mahler (2003), who observed that metal and shingle roofing
scale roofs were remarkably similar (Table 1). Consistent with materials are not a source of PAHs but that PAHs come from
the pilot data, the rainwater harvested after the first-flush atmospheric deposition. Our lack of detection of pesticides in
from the full-scale metal roof had average TC and FC
concentrations that were significantly lower than those from
both full-scale shingle roofs ( p-values < 0.09). Also consistent
with the pilot data, the TC, FC, turbidity, and TSS in the
Table 1 e Water quality parameters
rainwater harvested after the first-flush for the full-scale roofs
(minimumemaximum) of the rainwater harvested after
do not meet the USEPA primary drinking water standards nor the first-flush for the pilot-scale and full-scale roofs.
the non-potable urban water reuse guidelines. Similar to the
Parameter Metal Shingle
pilot data, the average nitrate and nitrite concentrations in the
rainwater harvested after the first-flush for the full-scale roofs Pilot-scale Full-scale Pilot-scale Full-scale
were well below the USEPA MCLs. pH 6.0e6.8 5.4e6.3 6.7e6.9 5.8e6.5
Conductivity 9e56 18e60 18e57 20e102
(mS/cm)
3.8. VOCs, SVOCs, PAHs, and pesticides e pilot- and
TC (CFU/100 mL) 117e770 64e173 177e1367 102e353
full-scale roofs FC (CFU/100 mL) <1e8 37e127 9e87 73e253
Turbidity (NTU) 7e30 5e35 8e24 6e23
The first-flush samples and ambient rain samples from one TSS (mg/L) 20e87 10e50 12e54 20e150
rain event were analyzed for PAHs and pesticides for the pilot- Nitrate (mg-N/L) 0.0e2.0 0.4e4.1 0.0e1.8 0.3e4.7
scale roofs and for a larger suite of VOCs and SVOCs for the Nitrite (mg-N/L) 0.01e0.03 0.01e0.05 0.01e0.04 0.01e0.06
DOC (mg/L) 2e11 4e13 10e15 5e31
full-scale roofs. In the pilot-scale study, no pesticides or PAHs
Lead (mg/L) 0.3e2.3 2.1e5.8 0.4e1.2 0.7e8.6
were detected. In the full-scale study, 2,4-dinitrophenol was
Zinc (mg/L) 77e362 18e23 8e85 1e15
detected in the first-flush of the metal roof and one of the
2058 w a t e r r e s e a r c h 4 5 ( 2 0 1 1 ) 2 0 4 9 e2 0 5 9
harvested rainwater is likely related to surrounding land-use,
where major pesticide applications are absent.
4. Conclusions
Conventional roofing materials (i.e., asphalt fiberglass shingle,
Galvalume
metal, and concrete tile) and alternative roofing
materials (i.e., cool and green) were examined for their suit-
ability to harvest rainwater for domestic use. pH, conductivity,
TC, FC, turbidity, TSS, nitrite, nitrate, DOC, metals, VOCs, and
SVOCs were measured in harvested rainwater. The following
conclusions were drawn:
 Rainwater harvested from any of the tested roofing mate-
rials would require treatment if the consumer wanted to
meet the USEPA primary and secondary drinking water
standards or the USEPA non-potable water reuse guidelines.
In particular, the rainwater harvested after a first-flush
consisting of a minimum of 38 L for every 93 m2 of collection
area from the asphalt fiberglass shingle, metal, concrete
tile, and cool roofs would need treatment for TC, FC,
turbidity, aluminum, and iron to meet the drinking water
standards. The rainwater harvested after the first-flush
from the green roof would need treatment for TC, FC,
turbidity, and aluminum. Thus, at a minimum, first-flush
diversion, filtration, and disinfection are recommended to
meet current USEPA standards/guidelines. However, since
the quality of ambient rainwater varies by location, we
caution that rainwater harvested in other locations might
exceed standards/guidelines for different water quality
parameters than those observed in this study.
 While metal roofs are commonly recommended for rain-
water harvesting applications, the metal roofs examined in
this study did not produce clearly superior harvested rain-
water quality as compared to the other roofing materials.
Concrete tile and cool roofs also appear to be good candi-
dates for rainwater harvesting catchments, given the overall
similarity in harvested rainwater quality among those three
materials.
 The DOC concentrations in rainwater harvested from the
shingle and green roofs are very high (i.e., approximately
one order of magnitude higher than that of a typical,
finished drinking water in the U.S.) and could lead to high
concentrations of disinfection byproducts. The formation of
trihalomethanes and haloacetic acids, two classes of regu-
lated disinfection byproducts in drinking water, should be
assessed after disinfecting harvested rainwater with chlo-
rine. The elevated DOC concentrations observed in the
rainwater harvested from the shingle and green roofs in our
short-term study suggest that other roofing materials (e.g.,
metal, tile, and cool) might be preferable for rainwater
harvesting applications when chlorine is the disinfectant of
choice.
 The rainwater harvested from the metal roof showed lower
concentrations of fecal indicator bacteria than did the other
roofing materials. This might be due to the low emissivity of
metal, resulting in higher surface temperatures on the roof.
 The concentrations of some metals (e.g., arsenic) in rain-
water harvested from the green roof suggest that the quality
of commercial growing media should be carefully examined
if the harvested rainwater is being considered for domestic
use.
 Concentrations of most of the tested water quality param-
eters decreased as a result of diverting a first-flush of at least
38 L for every 93 m2 of collection area. While the depth of
rainfall to be diverted is a subject of debate, a first-flush
device can provide some improvement in water quality.
Acknowledgments
We are grateful to several sources of funding for this work: the
Texas Water Development Board (contract number
0804830855), Texas AgriLife Research (subcontract number
570464), the National Science Foundation (Graduate Research
Fellowship to C.B. Mendez), and the American Water Works
Association and CH2M Hill (Holly A. Cornell Scholarships to
B.R. Afshar and C.B. Mendez). We thank Dr. Sanjeev Kalaswad
and Mr. Jorge Arroyo from the Texas Water Development
Board for their input on this project and Mr. David Phillips (Ja-
Mar Roofing) for donating the materials and labor for
construction of the pilot-scale roofs. We also thank Mr.
Charles Perego, Dr. Steve Windhager, Dr. Cindy Menches, Dan
Hemme, Jeffrey Stump, Brett Buff, and David Stump for their
assistance on the project.
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