spatio-temporal variation in trihalomethanes in new south wales
TRANSCRIPT
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Spatio-temporal variation in trihalomethanes in New SouthWales5
Richard J. Summerhayes a,e,*, Geoffrey G. Morgan a,d, Douglas Lincoln a,Howard P. Edwards a, Arul Earnest b, Md. Bayzidur Rahman c, Paul Byleveld f,Christine T. Cowie g, John R. Beard a
aUniversity Centre for Rural Health, Northern Rivers, University of Sydney, PO Box 3074, Lismore, NSW 2480, AustraliabCentre for Quantitative Medicine, Duke-NUS Graduate Medical School, SingaporecSchool of Public Health and Community Medicine, University of New South Wales, Sydney, NSW 2052, AustraliadNorth Coast Area Health Service, NSW, Australiae School of Health and Human Sciences, Southern Cross University, Lismore, NSW 2480, AustraliafWater Unit, NSW Department of Health, PO Box 798, Gladesville, NSW 2111, AustraliagRespiratory & Environmental Epidemiology, Woolcock Institute of Medical Research, 431, Glebe Point Road, Glebe, NSW 2037, Australia
a r t i c l e i n f o
Article history:
Received 16 December 2010
Received in revised form
22 August 2011
Accepted 24 August 2011
Available online 1 September 2011
Keywords:
Trihalomethanes
Chloroform
Bromodichloromethane
Drought
Disinfection by-products
Australia
Abbreviations: THMs, trihalomethanes; Tchloromethane; DBCM, dibromochlorometh5 Institution where this work was performe2480, Australia.* Corresponding author. Tel.: þ61 419249037.E-mail addresses: summerhayes.richard
[email protected] (H.P. Edwards), arhealth.nsw.gov.au (P. Byleveld), christinec@h0043-1354/$ e see front matter ª 2011 Elsevdoi:10.1016/j.watres.2011.08.045
a b s t r a c t
Aim: This paper describes the spatio-temporal variation of trihalomethanes in drinking
water in New South Wales, Australia from 1997 to 2007
Method: We obtained data on trihalomethanes (THMs) from two metropolitan and 13 rural
water utilities and conducted a descriptive analysis of the spatial and temporal trends in
THMs and the influence of season and drought.
Results: Concetrations of monthly THMs in the two metropolitan water utilities of Sydney/
Illawarra (mean 66.8 mg/L) and Hunter (mean 62.7 mg/L) were similar compared to the
considerable variation between rural water utilities (range in mean THMs: 14.5e330.7 mg/L).
Chloroform was the predominate THM in two-thirds of the rural water utilities. Higher
concentrations of THMs were found in chlorinated water distribution systems compared to
chloraminated systems, and in distribution systems sourced from surface water compared
to ground water or mixed surface and ground water. Ground water sourced supplies had
a greater proportion of brominated THMs than surface water sourced supplies. There was
substantial variation in concentration of THMs between seasons and between periods of
drought or no drought. There was a moderate correlation between heavy rainfall and
elevated concentrations of THMs.
Conclusion: There is considerable spatial and temporal variation in THMs amongst New
South Wales water utilities and these variations are likely related to water source, treat-
ment processes, catchments, drought and seasonal factors.
ª 2011 Elsevier Ltd. All rights reserved.
HM4, total THM; NSW, New South Wales; DBP, disinfection by products; BDCM, bromodi-ane.
d: University Centre for Rural Health, Northern Rivers, University of Sydney, Lismore, NSW
@gmail.com (R.J. Summerhayes), [email protected] (G.G. Morgan),[email protected] (A. Earnest), [email protected] (Md.B. Rahman), [email protected] (C.T. Cowie).ier Ltd. All rights reserved.
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 65716
1. Introduction
The provision of safe drinking water through disinfection to
remove water-borne microbiological pathogens causing
typhoid, cholera and gastroenteritis is one of the major
achievements of public (Galal-Gorchev, 1996). An unexpected
consequence of disinfection is the interaction of the disin-
fectant with natural organicmatter (NOM) in the source water
forming a range of chemicals collectively called disinfection
by-products (DBPs) (Rook, 1974).
DBP formation is not well understood but is influenced by
the presence of bromide, iodide, pH, temperature, seasonal
and climatic factors. Operational factors in water treatment
also play a role in DBP formation including residency time
within the distribution system, filtration methods used in
removal of NOM, and disinfectant type and dose (Chowdhury
et al., 2009). Trihalomethanes (THMs) were the first DBPs
discovered in 1974 and are a group of organic compounds
formed through reactions between methane (CH4) derivatives
in NOM and chlorine or chloramines (Garrido and Fonseca,
2010). Since their discovery, more than 600 different DBPs
have been reported, with THMs being the most frequently
detected compounds (Richardson et al., 2007).
In 1976, the US National Cancer Institute declared chloro-
form a carcinogen in animals and a suspected carcinogen in
humans (National Cancer Institute, 1976). Exposure to DBPs is
associated with bladder, rectal and colon cancer, ‘suggestive
of a causal inference’ (Hrudey, 2009).While some reproductive
outcomes such as small for gestational age and pre-term
births have also been associated with DBP exposure, the
current evidence is inconclusive (Grellier et al., 2010). In Aus-
tralia, DBPs are not regulated but a guideline value of 250 mg/L
for total THM is recommended and action to reduce THMs is
encouraged, while not compromising disinfection as exposure
to non-disinfected water poses substantially greater health
risk than exposure to low level THMs (NHMRC, 2004). There is
limited published data describing THMs or other disinfection
by-products in Australia. A survey of several DBPs during
1994-95 in 16 cities throughout Australia found that some
Australian drinking water supplies had high THM concentra-
tions (up to 191 ug/L) (Simpson and Hayes, 1998).
In New South Wales (NSW), Australia’s most populated
state, more than 5million residents (approximately 80% of the
population) use public drinking water as their usual source of
drinking water (Centre for Epidemiology and Research, 2002).
The two largest public water suppliers provide drinking water
to the Sydney/Illawarra (4.2 million people) and Hunter
(516,000 people) metropolitan areas. In rural areas, local water
utilities (largely through local government authorities)
provide drinking water. While the NSW Health Department
recommends that all water utilities collect monthly THM
samples (NSW Health, 2000), only the large metropolitan
utilities of Sydney/Illawarra and the Hunter, and a small
number of rural water utilities conduct regular THM
monitoring.
This paper describes THM concentrations throughout New
South Wales, Australia, covering large metropolitan water
utilities, as well as small to medium size rural water utilities.
Our study assesses geographic differences and temporal
trends in monthly THM data from metropolitan utilities over
several years, and rural utilities for at least one year. During
our study period,much of NSWexperienced one of the longest
droughts on record lasting nearly a decade from 1997 to 2006
(Bond et al., 2008) and we also investigated the influence of
drought on THM’s.
2. Methodology
2.1. Water utility data
We obtained data on THMs for the periods 1998 to 2004 for
Sydney/Illawarra region, 1997 to 2004 for Hunter region and
various time periods between 1997 and 2007 for the rural
water utilities summarized in Table 1.
2.1.1. Sydney/Illawarra water utility dataThe SydneyWater Corporation (SWC) supplies water from five
surface catchments to the Sydney/Illawarra metropolitan
region, covering an area of 12,700 km2. Sydney/Illawarra has
a three level hierarchical structure, with 14 delivery systems
(average area 241 km2) supplied with surface water treated at
nine water filtration plants. Each delivery system contains
from one to six distribution systems (average area 84.3 km2)
which are treated either by chloramination or chlorination.
Rechlorination occurswithin the distribution system.Water is
stored in 180 water supply zones (average area 16.4 km2)
which supply water to homeswithin the distribution systems.
Limited data was also available on a range of water quality
factors and other DBP’s including: trichloracetonitrile (5
months in 1998 covering 18% of supply zones); six haloacetic
acids (HAAs) (two periods of 12 and 7 months covering 69% of
supply zones); and three HAAs (bromoacetic-, dibromoacetic-
and tribromoacetic acids, 5months covering all supply zones).
Due to the limited duration of sampling for these DBP’s, and
the lack of comparable data from other water supplies in
NSW,we have not reported these results in detail in the paper,
but summary statistics are provided in the Supplementary
Material AeC.
There are some 3000 THM water sampling sites within the
Sydney/Illawarra distribution systems. Monthly monitoring is
generally conducted at these sites on a three to six-monthly
rotational cycle with a minimum of 3e6 sites operating
within each distribution system (SWC, 2002). Monthly THM
data from all available monitoring sites within each supply
zonewas averaged to obtain zone/month THM concentrations
for each month in the study period.
2.1.2. Hunter water utility dataThe Hunter Water Corporation supplies the Hunter metro-
politan region via nine water distribution systems covering an
area of 5400 km2. Six distribution systems received surface
water and three received ground water for most of the study
period although prior to 2003 blending of surface and ground
waters from different sources occurred at various time
periods for three distribution systems normally supplied by
surface water. After 2003 two distribution systems, previously
supplied by groundwater, were continuously augmentedwith
Table 1 e Characteristics of NSW metropolitan and rural water utilities included in the study.
Water Utility WaterSource
DisinfectantProcess
Treatment Process(Catchment characteristics)
Approx.pop. (2002)
Number ofsamples
Study Period(months of data)
Sydney/
Illawarra
Surface Chlorinateda Filtration, flocculation,
coagulation, lime.
600,000 5341 Jan 1998eDec 2004 (84)
Chloraminated 3,600,000
Hunterb Surface Chlorinated Filtration, coagulation,
flocculation, sedimentation,
powdered activated
carbon (PAC)
452,000 863 Jan 1997eDec 2004 (96)
Ground Chlorinated Aeration, lime, coagulation,
filtration
60,000
Rural
Utilities
1 Surface Chlorinated Filtration, coagulation,
sedimentation, PAC
4000 28 Feb 2003eNov 2003 (9)
2 Surface Chlorinated Filtration, flocculation,
sedimentation,
21,000 156 Nov 1997eDec 2005 (89)
3 Surface Chlorinated Filtration, coagulation,
flocculation, sedimentation
160,000 72 Nov 2003eJan 2004 (8)
4 Surface Chlorinated Filtration 26,000 314 Jan 2001eMay 2007 (62)
5 Surface Chlorinated No treatment 65,000 508 Jan 2001eDec 2004 (54)
6 Surface
blended
Chlorinated Lime, aeration 2000 61 Jan 2001eMay 2006 (61)
7 Surface Chlorinated Coagulation, flocculation,
sedimentation
20,000 30 Jul 2001eJan 2004 (30)
8ac Ground Chloraminated Direct filtration, aeration,
coagulation, flocculation,
dissolved air flotation
4500 1378 Dec 2000eMay 2006 (63)
8bc Surface Chlorinated Filtration, coagulation,
flocculation, sedimentation
11,000 660 Dec 2000eMay 2006 (66)
9 Surface Chlorinated Direct filtration 21,000 85 Jan 2000eOct 2006 (80)
10 Surface Chlorinated Direct filtration, coagulation,
flocculation, sedimentation
53,000 43 Jun 2001eAug 2005 (40)
11 Surface Chlorinated Filtration, dissolved air
flotation, flocculation
74,000 1610 Jan 2000-Apr 2006 (61)
12 Surface Chlorinated Filtration, flocculation 8000 43 FebeDec 2003 (11)
13 Surface Chlorinated Filtration, coagulation,
flocculation, sedimentation
135,000 159 Mar 1999eJan 2006 (86)
a In Sydney/Illawarra, 4 of the 33 distribution systems changed disinfection from chlorination to chloramination in June 2003.
b In Hunter, two distribution systems using ground water were augmented with ground and surface waters from other sources after 2003, and
prior to 2003, some systems supplied with surface water were occasionally augmented with blended ground and surface waters from other
sources.
c Water utility 8 includes a chloraminated distribution system with ground water supply (8a) and a chlorinated distribution system with
a surface supply. Data for 8a should be treated with caution as majority of values were below <5 mg/L detection limit.
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 6 5717
blended surface and ground water from different sources
(HWC, 2004). A fixed sampling site is located within each
distribution system towards the extremities of the systems,
providing distribution/month THM values.
2.1.3. Rural water utility dataWe surveyed all 106 utilities in rural NSW requesting infor-
mation and data on DBPs and water quality parameters.
Ninety-four rural water utilities (89%) responded to the survey
and 27 (26%) indicated they collected some data on THMs. We
received data on THMs from 25 (24%) rural water utilities of
which 13 (12%) had sufficient THM data to be included in our
analysis. Five of these rural utilities supplied additional
monitoring data on a range of other water quality parameters,
however these data covered limited durations and were
insufficient to assess seasonal trends and geographic differ-
ences and in keeping with the objectives of the paper are not
reported in detail, although they are briefly summarised in the
Supplementary Material A.
The size and complexity of rural water utilities varies, and
THM sampling varied from one-off short term sampling
periods to routine quarterly or monthly sampling covering
various time periods between 1997 and 2007 (see Table 1). All
sampling was conducted at random sites throughout the
distribution systems. Water utility #6 provided data only on
THM4 from sample points within the distribution system. A
separate one-month survey in utility #6 including post-
treatment samples indicated that chloroform comprised
approximately 86% and BDCM 13% of the THM4 concentration
entering the distribution system (these survey data not
included in the final analysis but are provided in
Supplementary Material D). Rural utility #8 includes a distri-
bution system which is chloraminated and mainly sourced
from ground water, and a chlorinated distribution system
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 65718
sourced from surface water. We designated the two distribu-
tion systems as #8a and #8b respectively for reporting. The
source water, disinfection, treatment types, number of THM
samples and sampling period for each of the water utilities
included in our analysis are shown in Table 1.
We included only those rural water utilities with monthly
monitoring data covering all four seasons in at least one year
(DecembereFebruary ¼ summer, MarcheMay ¼ autumn,
JuneeAugust¼winter and SeptembereNovember¼ spring) so
that seasonal variation could be assessed. For each rural water
utility with sufficient data to be included in the study we
averaged available monthly THM concentrations to obtain
utility/month concentrations.
2.1.4. Trihalomethane monitoringWater samples were analysed for THMs by Sydney Water
Corporation laboratories using Standard Methods for the
Examination of Water and Waste Water (20th Ed.), Method
6200B (modified) and USEPA Method 8260 (modified) (APHA-
AWWA-WPCF, 1998; USEPA, 2008); in the Hunter Water
Corporation based on the USEPA standard Method 8260
(USEPA, 2008) and in rural water utilities using the Standard
Methods for the Examination of Water andWasteWater (18th
ed) Method 6232 (APHA-AWWA-WEF, 1992). Further details of
the analytical techniques are provided in the Supplementary
Material E.
Multiple values below the detection limit were recorded
within each water utility over the study period. The limit of
detection for individual THMs was usually <1 mg/L, with
occasional higher limits of detection reported. We used
a similar approach to other studies and substituted samples
flagged as below the detection limit with two-thirds of the
detection limit value, which is the approximatemean of a log-
normal distribution (Whitaker et al., 2003). Bromoform was
found to be below the detection limit more than 75% of the
time across most utilities (metropolitan and rural), and
therefore we examined bromoform only as part of total
brominated THMs (BrTHM) and the sum of the four trihalo-
methanes (THM4) (percentage of observations below detec-
tion values provided in Supplementary material F).
2.2. Rainfall data
Data on rainfall was obtained from the Sydney Catchment
Authority, and the Australian Bureau of Meteorology website
(Bureau Of Meteorology, 2010). Data on monthly drought
status for NSW districts containing the water utilities was
obtained from the NSW Department of Primary Industries,
with each month classified as ‘no drought’, ‘marginal’ or
‘drought’. Drought status is defined by a number of criteria
including monthly rainfall, temperature, frost and evapora-
tion, poor pasture biomass, soil moisture and livestock.
Marginal conditions include rainfall for the previous 3months
within or below average for the three month rainfall decile
and surface water supplies less than 50% of normal for the
time of year. Drought conditions include rainfall for the
previous 6 months within or below average for the 6-month
rainfall decile and surface water supplies less than 30% of
normal for the time of year (NSW Department of Primary
Industries, 2010).
2.3. Statistical analysis
We produced a range of descriptive statistics using log
transformed THM concentrations due to the skewed THM
distribution and back-transformed the results for reporting.
Differences in themeans for season and drought periods were
assessed using KruskaleWallis tests. Correlations between
THMs and rainfall lagged up to one month were conducted
using the Spearman correlation coefficient. The selection of
a one month lag is based on a 30e40 day residency time for
Prospect Reservoir in the Sydney/Illawarra supply (Hamilton
et al., 1995). Data management was conducted in Excel
(version 2003) and Access (version 2003) and all statistical
analyses were conducted using SAS version 9.1.3 (SAS Insti-
tute Inc., Cary North Carolina USA).
3. Results
3.1. Spatial variation
Table 2 summarises descriptive statistics for individual THMs
and THM4 concentrations in treated water for all the selected
NSW water utilities. The mean THM4 concentrations in Syd-
ney/Illawarra (66.8 mg/L) and Hunter are similar (62.7 mg/l).
Water treated by chlorination in Sydney/Illawarra had higher
mean THM4 concentrations (81.1 mg/L) than water treated by
chloramination (50.8 mg/L). The Prospect South delivery
system in Sydney/Illawarra switched from chlorination to
chloramination in July 2003 and the mean monthly chloro-
form concentration decreased substantially from 59.5 mg/L
during the chlorination period (1998 to mid-2003) to 23.0 mg/L
( p < 0.001) during the chloramination period (mid-
2003e2004). In the Hunter, chlorinated surface water had
higher mean THM4 concentrations (74.4 mg/L) than chlori-
nated ground water (36.1 mg/L). From 2003, Hunter augmented
two ground supplies and three surface supplies continuously
with blended ground and surface waters in response to
drought conditions. The mean THM4 in the ground water
supplies increased from 17.9 to 40.6 mg/L with augmentation
and from 66.4 to 74.2 mg/L in the surface supplies.
The majority of the rural water utilities reporting in the
study use chlorination, one system used chloramination
together with chlorination. Rural NSW water utilities gener-
ally use surface water, with some using ground water or
a blend of ground and surface waters. During the study period
there was large variability in the monthly mean THM4
concentration in treated water between rural water utilities.
The THM4 concentration of the rural utility with the
minimum (#8a: 15 mg/L) and maximum (#6: 331 mg/L) monthly
concentrations were substantially different compared to the
remaining 11 utilities which ranged from of 63.7 mg/L to
189.1 mg/L, although this trimmed range still represents a 3
fold difference in monthly THM4 concentrations.
Chloroform is the main component of total THM in chlo-
rinated (66%) and chloraminated (59%) surface water in Syd-
ney/Illawarra. Chloroform is also themain component of total
THM in chlorinated surface water in the Hunter (60%) and in
most rural utilities with the exception of utilities #2 (29%), #3
Table 2 e Concentrations of trihalomethanes in treated drinking water in water utilities in New South Wales.
Water Utility N Mean THM4 Chloroform BDCM DBCM
Min P95 Max Mean Min Max Mean Min Max Mean Min Max
Metropolitan
Sydney/Illawarra 563 66.8 22.7 114.6 196.7 40.1 4.5 162.5 16.5 3.0 46.0 7.1 0.7 27.3
Chloraminated 278 50.8 22.7 81.3 199.0 28.3 9.0 88.0 14.2 3.0 39.0 5.8 0.7 31.0
Chlorinated 340 81.1 25.0 127.0 196.7 50.7 4.5 162.5 18.6 5.7 46.0 8.1 0.8 27.3
Hunter 72 62.7 10.1 105.2 114.6 35.2 0.7 96.3 15.2 0.7 31.2 9.1 0.9 24.9
Ground 18 36.1 10.1 74.3 74.3 16.0 0.7 46.8 8.3 0.7 20.8 5.9 2.8 9.2
Blended 30 72.6 14.7 106.4 134.0 33.4 1.0 78.3 20.7 0.7 34.3 15.2 3.7 27.0
Surface 48 74.4 30.1 105.2 131.0 44.5 20.5 96.3 18.1 3.1 30.0 10.0 0.9 24.0
Rural Utilities
1a 9 189.1 67.5 290.7 290.7 104.8 29.7 190.1 48.8 22.5 94.1 19.8 4.7 76.3
2 89 114.9 21.0 231.0 346.0 33.6 2.0 172.0 32.5 4.5 104.7 32.7 2.8 128.5
3 8 81.7 65.4 102.3 102.3 29.5 13.3 47.9 24.9 20.6 31.2 16.6 6.9 24.7
4 62 106.1 21.1 170.2 245.4 45.0 16.8 108.8 26.8 0.7 56.7 16.0 0.7 56.7
5 54 73.4 23.8 120.1 122.3 48.2 13.9 90.0 16.5 6.3 24.2 5.7 2.7 10.3
6a 61 330.7 63.0 501.0 586.0 na na na na na na na na na
7 30 87.5 22.7 147.3 213.7 72.8 3.0 200.0 11.9 3.0 20.0 1.4 1.0 2.0
8a 63 14.5 13.1 17.8 23.6 4.4 3.3 11.2 3.4 3.3 5.4 3.3 2.5 4.1
8b 66 102.2 44.9 145.4 221.2 63.9 22.2 159.2 25.6 8.2 51.3 9.1 3.3 25.3
9 80 99.3 39.0 157.9 180.0 46.8 12.0 112.8 33.4 12.0 57.0 17.9 8.0 56.0
10 42 63.8 13.3 86.3 120.0 34.1 3.3 68.0 16.2 3.3 39.0 9.5 1.0 32.0
11 61 63.7 18.4 102.3 128.9 33.0 5.7 86.6 16.6 3.8 32.2 9.2 3.3 32.0
12a 11 138.5 52.3 286.0 286.0 87.1 17.3 155.0 31.3 13.3 78.0 12.3 1.3 48.0
13 86 94.9 2.7 152.7 229.0 54.5 0.7 110.0 26.7 0.7 76.0 11.1 0.7 64.0
All values in mg/L ¼ micrograms per litre, N ¼ number of observations, Min ¼ minimum, P95 ¼ 95th percentile, Max ¼ maximum, na ¼ not
available.
Sydney/Illawarra mean: mean of annual zone means.
Hunter mean: mean of annual distribution system means.
Rural water utilities mean: mean of monthly utility means.
Water utility 8 includes a chloraminated distribution systemwith groundwater supply (8a) and a chlorinated distribution systemwith a surface
supply. Data for 8a should be treated with caution as majority of values were below <5 mg/L detection limit.
Water utility 6 only has data for THM4.
a Utilities with 95th percentile THM4 concentrations above the Australian National Drinking Water Guideline value of 250 mg/L.
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 6 5719
(36%) and in the ground water sources in the Hunter (56%) and
#8a (30%) which had higher proportions of brominated THMs.
3.2. Rainfall
Fig. 1 illustrates the temporal variation in Sydney/Illawarra
chloroform and brominated THM concentrations and mean
monthly rainfall. Prior to October 1998 brominated THM
concentrations were generally higher than chloroform, then
decreased until mid 1999 and have since remained relatively
constant. Chloroform concentrations decreased steadily from
mid-1998 but showed considerable variability, and from late
2003 concentrations were similar or lower than brominated
species. Several peaks and troughs in chloroform concentra-
tion coincidewith heavy rainfall events.We found amoderate
correlation between overall monthly THM4 and rainfall (lag
one month, r ¼ 0.35, p < 0.01) for the Sydney/Illawarra, with
higher correlations within some of the five Sydney/Illawarra
catchments (Blue Mountains/Cascade catchment: r ¼ 0.57,
p < 0.001; Upper Nepean/Illawarra catchment r ¼ 0.47,
p < 0.001).
Fig. 2 shows the temporal variation in chloroform, bromi-
nated THMs and rainfall in the Hunter region. Chloroform
concentrations are generally higher than brominated THMs,
with occasional large peaks in chloroform and brominated
THMs from2001.We found no correlation in theHunter region
between rainfall (lag one month) and mean THM concentra-
tion in distribution systems supplied by ground water, and
a moderate correlation in distribution systems supplied by
surface waters (r ¼ 0.59, p < 0.01).
We generally foundmoderate correlations between rainfall
and THM4 concentrations in the rural utilities located in sub-
tropical coastal floodplains including utilities #11 (r ¼ 0.30,
p < 0.02), #8b (r ¼ 0.58, p < 0.001) and #5 (0.67, p < 0.001). We
generally found little correlation with mean monthly rainfall
(lag 1 month) and THM in the other rural utilities (data not
shown).
3.3. Drought
We examined the difference in the concentration in THMs in
periods of drought compared to marginal and no drought and
the results are summarised in Table 3. Sydney/Illawarra was
in drought for 18 months (21.4%) of the 84 month study period
and continuously in marginal drought from September 2002
until mid-2007. There was a consistent significant decrease in
mean THM4 concentrations during drought months
compared to non-drought (THM4: 52.6ug/L compared to
0.0
20.0
40.0
60.0
80.0
100.0
120.0
0
10
20
30
40
50
60
70
80
90
Mea
n M
onth
ly C
atch
men
t R
ainf
all (
mm
)
Mea
n M
onth
ly C
hlor
ofor
m a
nd B
rom
inat
ed T
HM
C
once
ntra
tion
(ug
/L)
BrTHM Chloroform Rainfall
Fig. 1 e Temporal variation in Sydney/Illawarra monthly chloroform and brominated THM concentration and monthly
rainfall.
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 65720
75.9ug/L, p < 0.001), and this was reflected in chloroform and
BDCM, while DBCM concentration increased. The majority of
sampling for HAAs in Sydney/Illawarra occurred in a non-
drought period, however three HAAs (bromoacetic-;
dichloroacetic- and trichloroacetic acids) showed significant
decline during drought compared to no drought consistent
with reductions in THMs, except DBCM (see Supplementary
Material C).
Hunter was in drought for 19months of the 96month study
period and only the blended distribution systems showed
a significant THM4 decrease during drought compared to no
drought (THM4: 69.8 mg/L compared to 46.4 mg/L, p < 0.05), re-
flected in chloroform, BDCM and DBCM. THM concentrations
0
10
20
30
40
50
60
70
80
90
100
Mea
n M
onth
ly C
hlor
ofor
m a
nd B
rom
inat
ed T
HM
C
once
ntra
tion
(ug/
L)
chloroform BrTHM Rainfall
Fig. 2 e Temporal Variation in Hunter monthly chloroform and
rainfall (mm).
in rural water utilities during drought periods compared to
non-drought periodswere extremely variable. Five rural water
utilities that were in drought continuously for 12 months or
longer experienced significantly reduced chloroform concen-
trations compared to periods of no drought (#2, #4, #9, #10 and
#13), and these same utilities experienced significantly
increased DBCM concentrations.
3.4. Seasonal variation
We found considerable seasonal variability in mean THM4
concentrations between locations and these results are sum-
marised in Table 4. In Sydney/Illawarra there was a significant
0
50
100
150
200
250
300
350
400
450M
ean
Mon
thly
Cat
chm
ent
Rai
nfal
l (m
m)
brominated THM (BrTHM) concentration and monthly
Table 3 e Mean monthly trihalomethane concentrations during drought compared to no drought and marginal drought, NS water utilities.
Water Utility Time (months THM4 Chloroform BDC DBCM
NoDroughtn (%)
Marginaln (%)
Droughtn (%)
NoDroughtMean
MarginalMean
DroughtMean
NoDroughtMean
MarginalMean
DroughtMean
NoDroughtMean
Margi alMea
DroughtMean
NoDroughtMean
MarginalMean
DroughtMean
Sydney/Illawarra 50 (59.5) 16 (19.1) 18 (21.4) 75.9 51.1 52.6** 49.0 27.5 27.6** 17.7 13. 14.1** 6.6 7.4 8.0**
Chloramination 59.4 37.0 36.5** 36.0 17.4 16.5** 16.1 11. 11.4** 5.3 6.3 6.6**
Chlorination 87.2 66.7 67.8** 57.8 38.7 37.9** 18.8 16. 16.7** 7.5 8.7 9.4**
Hunter 60 (62.5) 17 (17.7) 19 (19.8) 58.4 73.6 66.4* 33.2 41.6 35.4 13.9 18. 17.0 8.2 10.7 10.6
Ground 31.5 56.1 50.2** 12.5 22.9 20.7** 6.8 16. 14.4** 5.9 11.6 9.8**
Blended 69.8 70.6 46.4* 36.7 35.4 19.0** 20.0 19. 11.6* 11.5 12.1 9.9
Surface 72.3 84.2 80.6* 46.4 54.5 47.5 16.1 18. 20.0** 8.4 9.5 11.2*
Rural Utilities
2 26 (27.1) 19 (19.8) 51 (53.1) 149.9 97.6 113.5* 55.6 36.8 25.3* 32.6 32. 30.9 32.4 23.2 36.6*
3 1 (12.5) 4 (50.0) 3 (37.5) 67.4 86.7 88.8 14.3 30.8 39.4 22.7 26. 26.7 20.2 21.9 17.2
4 10 (16.1) 5 (8.10) 47 (75.8) 151.2 134.5 103.8* 92.3 92.9 41.0* 21.8 30. 31.2 5.8 11.6 22.2*
5 24 (44.4) 16 (29.6) 14 (25.9) 74.8 81.3 82.6 49.2 56.9 57.7 17.7 17. 17.6 7.2 6.7 7.2
6 23 (37.7) 20 (32.8) 18 (29.5) 287.5 379.3 331.9** a a a a a a a a a
7 12 (40.0) 6 (20.0) 12 (40.0) 86.0 89.2 88.1 74.3 74.3 70.6 9.1 12. 14.8** 1.3 1.6 1.5
8b 24 (36.4) 7 (10.6) 35 (53.0) 97.1 108.8 105.9 56.8 70.9 68.9 26.8 26. 25.3 10.1 8.3 8.7
9 29 (36.2) 16 (20.0) 35 (43.8) 100.4 97.3 100.3 54.8 40.5 43.7* 32.5 34. 33.6 12.7 20.2 21.1**
10 10 (25.0) 7 (17.5) 23 (57.5) 63.7 56.9 67.5 48.3 29.5 30.6* 9.5 15. 19.7* 2.6 8.7 13.0**
11 38 (62.3) 15 (24.6) 8 (13.1) 63.4 69.0 71.9 33.5 39.7 34.0 16.9 18. 18.6 9.6 8.8 14.8
12 - (0.0) 1 (09.0) 10 (91.0) na 157.9 143.1 na 135.0 94.1 na 20. 33.8 na 1.3 14.1
13 47 (54.7) 22 (25.6) 17 (19.8) 83.9 112.7 104.5* 50.7 67.5 48.5* 22.9 33. 31.3* 9.4 10.4 18.7*
* Significant at p < 0.05 level.
** Significant at p < 0.001 level, na e no data were available Means are reported in mg/L.
Water utility #12 was in marginal or drought only.
Water utilities #1 and #8a not shown as utility #1 was continuously in drought during the study period and water utility #8a values were below thre old and showed no variation between themeans.
a Water utility #6 reported THM4 data only.
water
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Table 4 e Seasonal variation in the mean trihalomethane concentration in water utilities in New South Wales.
Summer Mean THM4 Autumn Mean Winter Mean Spring Mean Summer-Winter Difference (%)
Sydney/Illawarra 69.9 72.6 64.3 60.3 þ5.6 (9.0)
Chloramination 54.8 58.0 54.0 52.0 þ0.8 (1.5)
Chlorination 80.0a,byy 79.3a,byy 71.9 69.8 þ8.1 (11.3)
Hunter 60.8 66.8 60.5 62.5 þ0.3 (0.5)
Ground 34.2 39.6 39.5 39.8 5.3 (15.5)
Blended 43.1a,cy 74.8 66.7 63.1 23.6 (54.8)
Surface 75.4 80.6 77.4 71.5 þ2.0 (3.0)
Rural Utilities
1 233.7 183.6 165.4 189.3 þ68.3 (41.3)
2 146.0ay 112.3 90.9 104.8 þ55.1 (60.6)
3 82.0 66.2 90.2 79.7 8.2 (9.1)
4 110.8 122.5a,y 87.4 86.0 þ23.4 (26.8)
5 89.7ayy 85.5ay 46.2 62.0 þ43.5 (94.2)
6 340.9 313.8 324.3 345.1 þ16.6 (5.1)
7 80.5 96.9 77.1 97.8 þ3.4 (4.4)
8b 124.1ayy 107.0ay 79.8 91.3 þ44.3 (56.5)
9 97.6 102.2 99.5 97.7 1.9 (1.9)
10 64.1 70.7 60.1 64.2 þ4.0 (6.7)
11 72.1ay 67.3 48.7 58.1 þ23.4 (48.0)
12 212.5 129.2 89.5 126.1 þ123.0 (137.4)
13 93.7 92.0 97.3 94.7 3.6 (3.7)
Means and difference between summer and winter means are reported in mg/L.
y significant at the p < 0.05 level.
yy significant at the 0.001 level.
Water utility 8a values were below threshold and showed no variation between the means.
a Difference in means compared to winter.
b Difference in means compared to spring.
c Difference in means compared to autumn.
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 65722
increase ( p < 0.001) in mean THM4 concentration in chlori-
nated water during summer (mean 80.0 mg/L) compared to
winter (mean 71.9 mg/L) and spring (69.8 mg/L), but therewas no
difference in chloraminated distribution systems. In the
Hunter THM4 concentrations in blended water increased
significantly ( p < 0.05) by 23.6 mg/L in winter compared to
summer, while therewas generally a small increase in surface
and ground water concentrations. There was substantial
variation in the seasonality of THM4 concentrations between
rural water utilities. Ten of the 13 rural water utilities had
higher mean THM4 concentrations in summer compared to
winter ranging in increases of 4e123 mg/L, and this increase
was significant ( p < 0.05) in four utilities.
4. Discussion
4.1. Spatial variation
We found the concentration of THM4 and speciation to be
similar for the Sydney/Illawarra (THM4 ¼ 67 mg/L, 60% chlo-
roform) and Hunter (THM4 ¼ 63 mg/L, 56% chloroform)
metropolitan water utilities.
We found considerable variation in THM concentrations
and speciation between rural water utilities, with mean
monthly THM4 concentrations ranging from 15 to 331 mg/L
(29e86% chloroform). The THM4 concentration of the rural
utility with the minimum (#8a: 15 mg/L) and maximum (#6:
331 mg/L) in the rangewere substantially different compared to
the remaining 11 utilities and suggests that the factors influ-
encing THM4 concentrations in utilities #8a and #6 are
substantially different to the other 11 rural utilities. Differ-
ences in geography and catchment characteristics may
contribute to variation in THM concentrations throughout
NSW. Utilities in the semi-arid floodplains in the far-west of
the State (#1, #2 and #12) had higher THM4 concentrations
(range of means: 114e189 mg/L) compared to other water
utilities (range of means: 15e106 mg/L) with the exception of
water utility #6 (mean 331 mg/L) which is in a sub-tropical
coastal floodplain area. The 95th percentile for THM4
concentration for three rural water supplies was above the
Australian guideline value of 250 mg/L (Table 2) suggesting
these utilities need to implement strategies to reduce THM
concentrations (NHMRC, 2004).
The Australian guideline value for THM4 of 250ug/L is
higher than a number of other developed countries including
United Kingdom, Japan (100 mg/L), USA (80 mg/L) France
(30 mg/L) and Germany (10m/L) (Rizzo et al., 2005). The large
variation in mean THM4 in rural NSW is similar to that re-
ported in a survey of DBPs in North Virginia, USA prior to the
introduction of the 1979 interim Disinfection By-Product Rule
of <100 mg/L (USEPA, 1979) which found mean THM4
concentrations of 249 mg/L (range 40e531 mg/L) in 1975e76 and
173 mg/L (range 43e889 mg/L) in 1976e77 (Hoehn and Randall,
1979). In a study in Turkey, where THMs are not regulated,
mean THM4 concentrations of 159 mg/L and 129 mg/L were
reported (Rizzo et al., 2005). Similar large variation has also
been found in rural communities in Alberta, Canada during
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 6 5723
Autumn 2000 with mean THM3 (excluding bromoform)
ranging from 44m/L to 210m/L (Charrois et al., 2004).
THM4 levels in NSW utilities were generally higher than
levels found in countrieswhere THMs are regulated. A 1988-89
survey reported median THM4 value of 39 mg/L for 35 utilities
across the USA (Krasner et al., 1989). A survey of 113 systems
in North Carolina in 2004-05 reported an average THM4 of
40.8 mg/L. In the United Kingdom, a study of data from 1992 to
1996 reported mean THM4 concentrations of 46 mg/L (Keegan
et al., 2001).
Chloroform generally comprised the majority of the total
THM in treated surface water in NSW (52%e86%). The domi-
nation of brominated THMs in treated ground water in the
Hunter (56%) and rural utility #8a (70%) is likely due to the
coastal aquifers having higher levels of bromide compared to
the surface supplies (Kampioti and Stephanou, 2002). The
surface water supplies of utility #3 (64% brominated THMs)
lies in a coastal floodplain area which may be affected by
saltwater intrusion; while utility #2 (71% brominated THMs)
lies in an ancient sea-bed which has been noted to have high
bromide concentrations (Richardson, 2005).
Chloraminated systems generally had lower THM4
concentrations (utility #8a mean THM4 14.5 mg/L, Sydney
mean THM4 50.8 mg/L) than chlorinated systems. A change
treatment from chlorination to chloramination in a delivery
system in Sydney resulted in a 159% reduction in THM4.
Bougeard et al. (2010) in a 2008 study in the United Kingdom
reported a 92% reduction in THM4 with a shift in disinfection
from chlorination to chloramination.
A major strength of this study lies in the large number of
observations covering a lengthy time period, incorporating
periods of long-term drought, drought-free periods and heavy
rainfall events. While we were only able to access THM data on
a small proportion of the total number of rural NSWwater util-
ities the surveyed utilities cover a wide range of geographic and
climatic regions encountered across the Australian continent.
4.2. Seasonal variation
We found substantial seasonal variation in THM4 concentra-
tions in chlorinated water in Sydney/Illawarra and in many of
the rural NSW water utilities, with generally higher concen-
trations in summer/autumn and lower concentrations in
winter, especially in semi-arid locations in the far-west of NSW
(utilities #1, #2 and #12). The groundwater supplied systems in
the Hunter showed little THM variation between seasons and
these results are consistent with overseas studies. A Canadian
survey of THMs showed amore than two-fold variation during
summer and winter in chlorinated systems (62.5 mg/L
compared to 33.5 mg/L) and chloraminated systems (32.8 mg/L
compared to 13.7 mg/L), however in groundwater supplies there
was little variation between seasons (Williams et al., 1995).
Another study in China in 2003 found THM levels to be 50 mg/L
in autumn and around 10 mg/L in spring in chloraminated
waters and noted variations in different organic matter
concentrations and in the dynamics of algae/plankton
production in the different seasons (Chen et al., 2008).
Summer is considered the most challenging period for
treating water and maintaining water quality and the
magnitude of seasonal fluctuations may be dependent on the
water source (McGuire and Meadow, 1988).
4.3. Rainfall
Several peaks and troughs in chloroform concentration coin-
cide with heavy rainfall events in Sydney/Illawarra. One such
event was the rains in mid 1998 that broke a drought lasting
from 1992 to 1998 and resulted in large inflows of contami-
nants and organic matter into the Sydney/Illawarra catch-
ment (Cox et al., 2003). The moderate correlations found
between rainfall and THM reported in our results are consis-
tentwith the correlations found in aNorth Virginia, USA study
(Hoehn and Randall, 1979). Heavy drought breaking rainfall is
associatedwith high turbidity, increased inflows, soil leaching
of NOM and microbiological contamination from degraded
catchments (Stein, 2000).
4.4. Drought
Droughts lasting several months to several years are a regular
feature of the Australian environment. Much of NSW experi-
enced one of the longest droughts on record lasting nearly
a decade from 1997 to 2006 (Bond et al., 2008). Sydney and parts
of NSW experienced drought from 1992 to 98 with a significant
wet period in mid-1998, then entered into drought again from
2002 until early 2011. During this period the Sydney catchment
storage (2 million megalitres) fell from 91% in 2000 to 32.5% in
mid-2007, in some rural catchments water levels fell below
30%, whereas the Hunter maintained a storage capacity above
60% by augmenting its water supply from 2002 with ground
and surface water from additional sources in response to
drought conditions (HWC, 2004). Inflows into major river
systems in NSW were some of the lowest on record and some
floodplains and wetlands had not been flooded during the
decade of drought (Murphy and Timbal, 2008).
While the effects of drought were variable, Sydney/Ill-
awarra and five of the 13 rural utilities experienced consistent
decrease in chloroform and an increase in DBCM during
drought periods. The effect of drought was also evident in
both chlorinated and chloraminated water as illustrated by
decreased chloroform concentrations in the Prospect South
distribution system during periods of drought when the
system was chlorinated and when it changed to being chlor-
aminated. The blended water distributions systems in the
Hunter showed decreased THM concentrations during
drought periods, while the ground and surface water systems
showed increased THM concentration.
Our findings in NSW are broadly similar to a UK study that
also that found decreases in chloroform concentration in
water supplies during drought (Whitaker et al., 2003). A study
in Greece showed a lower mean chloroform concentration
during an intense drought period (2.27 mg/L) compared to no
drought (10.22 mg/L) and an increased mean DBCM concen-
tration (drought 13.76 mg/L; no drought 1.38 mg/L) from
increased bromide through saltwater intrusion and ground
water augmentation (Kampioti and Stephanou, 2002). A North
Virginia, UAS study reported a large variation in THMs during
a period of no drought from 1975 to 76 (mean THM4 249 mg/L)
compared to severe drought from June 1976 to November 1977
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 65724
(mean THM4 173 mg/L). Themean concentration of chloroform
decreased from 246 to 152 mg/L in the drought compared to no
droughtwhile a small increase in BDCM from 19 to 21 mg/Lwas
reported (Hoehn and Randall, 1979). Drought can cause long-
term variations in DBP formation and the 1997-98 US Infor-
mation Collection rule survey found that long-term seasonal
factors such as drought, flood, hurricanes may account for
seasonal variation in water quality both in the source water
and in the distribution system although this was not assessed
in detail (McGuire et al., 2002).
Our results support previous findings that seasonal and
long-term effects of drought can have complex effects on the
nature and presence of NOM resulting in either an increase or
decrease in NOM which may in turn affect the nature and
concentration of THMs, suggesting that the effects of drought
may be catchment specific (Williamson et al., 1999). Algal
blooms, common in Australian waters may also play a large
role during warmer months and periods of low rainfall. Algal
blooms have been correlated with THM levels and regarded as
an important precursor for DBP production (Hoehn and
Randall, 1979; Chen et al., 2008). Although we had no data on
algae levels, algal blooms occurred in several rural water
utilities in coastal floodplain/estuarine areas (utilities #3, #6,
#13) and sub-tropical coastal areas (#11, #8b) during warmer
months and periods of low rainfall and drought. The
concentration of chloroform in all these surface supplied
distribution systemswas higher during drought periods. Rural
utility #6 suffered a number of major algal blooms during the
study period and recorded the highest concentrations of
THM4 amongst the study locations.
A decrease in organic matter can occur during drought due
to reduced run-off from catchments and inflows, which can
lead to lower turbidity and settling of sediments and organic
matter (Bond et al., 2008; Murphy and Timbal, 2008). Degra-
dation of organic matter over time during lengthy dry periods
and slower travel time of water compared to wet events can
also reduce organics in the water (Personal communication
Sydney Catchment Authority 2011). Drought can also influ-
ence groundwater quality due to declines in aquifer levels and
increased salinity causing bromide concentrations to rise
which can affect THM speciation (Krasner et al., 1994).
While there is much speculation on the effects of climate
change on drinking water quality (Bates et al., 2008), increases
in the frequency and extent of drought affected areas and
flooding from drought breaking rains are expected in south
eastern Australia (ABS, 2008; Dore, 2005). Water treatment
authorities respond to the higher risk of microbial contami-
nation of the raw source water during or shortly after heavy
rainfall by using higher disinfectant concentrations which in
turn can promote THM formation (Eikebrokk et al., 2004).
Changes in climatic factors related to climate change are
likely to create additional operational challenges for water
utilities in Australia, particularly in rural areas of NSW with
limited resources (Hurst et al., 2004; Soh et al., 2008).
5. Conclusion
We found considerable variation in THM concentration
between rural water utilities in NSW with some utilities
experiencing elevated concentrations above current national
THM4 guideline values indicating that these utilities require
action to reduce THM’s, while not compromising disinfection.
We obtained THM data from a small proportion of rural NSW
water utilities and our results suggests that elevated THM4
concentrations may occur in water utilities across rural NSW,
and rural Australia. THM concentrations in the chloraminated
systems in Sydney and the one rural utility were generally
lower than the chlorinated water supply systems.
We found considerable variation in THM’s between and
within utilities associated with extended drought periods
experienced during our study, with some utilities showing
decreases in chloroform and BDCM and increases in DBCM.
While we generally found higher concentration of THMduring
the warmer compared to cooler months the overarching
influence of drought on THMsmakes it difficult to identify the
principal drivers. Unfortunately our data lacked detailed data
on NOM, algae and catchment characteristics and inflows
which may help understand the possible drivers for these
variations.
The Australian Drinking Water Guidelines are currently
under review and at this time no change has been proposed to
the guideline value of 250 mg/L for THM4 (NHMRC, 2009). The
Guidelines note that a high concentration of THM4 is a good
indicator that other DBPs may be present. However data on
the occurrence, nature and concentrations of other DBPs are
scarce due to the lack of comprehensive survey data in NSW
and Australia. We recommend improved monitoring and
reporting of DBP’s and the collection of good data on catch-
ment characteristics and treatment to enable the assessment
of contributing factors to elevated concentrations of DBPs,
especially in rural Australia.
Competing financial interests
None identified.
Acknowledgements
The authors would like to acknowledge the following organi-
sations and individuals for their work on this manuscript:
Dr Mark Angles, Dr Peter Cox, Dr Vicky Whiffin, Mr David
Holland from Sydney Water Corporation and Adam Lovell
fromWater Services Association of Australia for expert advice
on the Sydney/Illawarra water utility.
Mr Bruce Cole andMs PamO’Donoghue fromHunterWater
Corporation for expert advice on the Hunter water utility,
Mr Peter Littlejohns from the Sydney Catchment Authority
for expert advice on drought effects in Sydney catchments in
NSW.
We also thank Dr Nel Glass and Dr Stephen Kermode from
Southern Cross University, Ms Therese Dunn and Mr Paul
Houlder for their valuable contributions to this manuscript.
We wish to acknowledge the support from the Australian
Research Council Linage Grant (LP0348628) and the Network
for Spatially Integrated Social Science. This work is part of
a PhD thesis by Richard Summerhayes.
wat e r r e s e a r c h 4 5 ( 2 0 1 1 ) 5 7 1 5e5 7 2 6 5725
Appendix. Supplementary material
Supplementary data associated with this article can be found
in the online version, at doi:10.1016/j.watres.2011.08.045.
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