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Environment International
journal homepage: www.elsevier.com/locate/envint
Review article
a r t i c l e
i n f o
Article history:
Received 9 February 2016
Received in revised form 24 March 2016
Accepted 24 March 2016
Available online 20 April 2016
Keywords:
Sewage
Removal efciency
Organic contaminant
Endocrine disrupting compound
Pharmaceutical and personal care product
Meta-analysis
a b s t r a c t
Trace organic contaminants (TrOCs), such as endocrine disrupting compounds (EDCs) and pharmaceuticals and
personal care products (PPCPs), represent global threats to aquatic animals and ecosystems. A major source of
TrOCs in the aquatic environment is via the discharge of treated sewage, so there is an urgent need to evaluate
the comparative efciencies of the most widely used sewage treatment technologies as regards elimination of
these compounds from wastewater. To address this need, 976 published articles were compiled focusing on estimates of removal (%) for 20 common environmental TrOCs, from ve major sewage treatment technologies:
conventional activated sludge (CAS), oxidation ditch (OD), membrane bioreactor (MBR), ponds and constructed
wetlands (PCW), and trickling biological lters (TBF). A quantitative meta-analysis was performed to compare
standardized relative removal efciencies (SREs) of the compounds amongst these technologies, and where possible potential sources of heterogeneity were considered (e.g., ow rates and chemical sorption potential). The
results indicate that the most widely used CAS treatment and the less common TBF provide comparatively
poor overall removal of common organic micropollutants. Membrane bioreactors appear to be capable of achieving the greatest overall removal efciencies, but the sustainability and economic viability of this option has been
questioned. Treatment with OD systems may be more economical while still achieving comparatively high removal efciencies, and the analysis revealed OD to be the best option for targeting highly potent estrogenic
EDCs. This study offers a unique global assessment of TrOC removal via leading sewage treatment technologies,
and is an important step in the identication of effective options for treating municipal sewage.
2016 Elsevier Ltd. All rights reserved.
Contents
1.
2.
3.
Introduction . . . . . . . . . . . . . . . . . . . . .
Methods . . . . . . . . . . . . . . . . . . . . . . .
Results and discussion . . . . . . . . . . . . . . . .
3.1.
Overview of data collection . . . . . . . . . . .
3.2.
Comparing SREs and controlling for heterogeneity.
4.
Conclusions . . . . . . . . . . . . . . . . . . . . .
Acknowledgements . . . . . . . . . . . . . . . . . . . .
References . . . . . . . . . . . . . . . . . . . . . . . .
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1. Introduction
Trace Organic Contaminants (TrOCs), such as endocrine disrupting
compounds (EDCs) and pharmaceutical and personal care products
(PPCPs), are now widely considered as emerging threats to aquatic
Corresponding author at: Smart Water Research Centre, Building G51, Grifth
University, QLD 4222, Australia.
E-mail address: s.melvin@grifth.edu.au (S.D. Melvin).
http://dx.doi.org/10.1016/j.envint.2016.03.031
0160-4120/ 2016 Elsevier Ltd. All rights reserved.
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183
184
185
185
185
187
188
188
animals and ecosystem health (Boxall et al., 2012; Brausch and Rand,
2011; Kaplan, 2013; Pal et al., 2010; Stuart et al., 2012). Many representative TrOCs have been shown to elicit a range of adverse toxicological
effects in aquatic wildlife, often at environmentally relevant sub-lethal
concentrations (Godoy et al., 2015; Pereira et al., 2015). The discharge
of treated sewage is a primary source of such contaminants in the
aquatic environment (Jasinska et al., 2015; Kaplan, 2013; la Farr
et al., 2008). Ensuring the protection of aquatic ecosystems and the
preservation of global biodiversity therefore demands sewage
184
3) the primary source of wastewater was domestic sewage, and 4) percentage removal was reported for clearly identied organic contaminant(s). When percentage removal was not directly reported, studies
were still included provided removal (R) could be calculated based on
concentrations at the inuent and efuent (Eq. (1)).
R %
C Influent C Effluent
100
C Influent
SRE
x
The average SRE for each treatment option (for each contaminant)
was calculated and analysed for signicant differences in the average
SREs (of all contaminants) using randomizations without replacement.
This approach is well suited for investigating differences in betweenstudy effect sizes (Adams et al., 1997; Gurevitch and Hedges, 1999),
and has been effectively applied to analyse similarly structured datasets
exploring ecological and toxicological processes (Melvin and Houlahan,
2012; Melvin and Wilson, 2013). The randomizations were performed
using MS Excel (Microsoft, Inc.), by calculating the absolute differences
in the average of all SREs amongst the 5 treatment technologies, and
then randomly reassigning the data to the different groups and
recalculating the differences. 10,000 permutations of the data were performed to determine the probability of randomly observing differences
in standardized removal amongst re-sampling groups that were greater
than or equal to those reported for the different treatment technologies,
using = 0.05 as the signicance threshold.
185
Fig. 1. Average removal (%) of the studied TrOCs amongst the various treatment
technologies. Boxplots display interquartile range, median (horizontal line), min and
max (whiskers), and average (+) of the 20 compounds included in the nal dataset.
was achieved in studies reporting contaminant removal using MBR systems, although this technology also exhibited the greatest heterogeneity (Fig. 3a). The cause of increased heterogeneity in MBR systems was
not immediately apparent, but closer inspection revealed very poor
comparative removal of the synthetic musk tonalide using this technology (Table 1). The literature search only identied a single removal estimate for tonalide using MBR treatment (Supplementary Table 1),
raising the possibility that anomalous outcomes for poorly studied compounds could introduce bias into the analysis. This is somewhat comparable to the phenomenon known as availability bias, where outcomes in
meta-analyses are inuenced by the selective inclusion of the most
readily accessible literature (Rothstein et al., 2006).
Therefore, the SRE values for each compound was weighted based on
the number of data points available for each treatment technology
(Eq. (3)), where, n is the number of removal estimates obtained for
each specic treatment technology, and N is the total number of data
points for that contaminant.
SRE0
SRE n
N
Analysis of the weighted data found CAS to be less effective than all
other treatment technologies (Fig. 3b). It is important to recognize that
the number of data points available for any given treatment technology
does not necessarily provide a strong indication of the reliability of a
study, and the true comparative removal efcacies therefore likely fall
Table 1
Average weighted Standardized Removal Efciencies (SRE) for each of the studied TrOCs amongst the 5 major treatment technologies. Bolded values indicate the treatment technology
with the highest SRE for each compound.
Sorption
Compound
Log Kow
CAS
MBR
OD
PCW
TBF
Low
Caffeine
Metoprolol
Sulfamethoxazole
Trimethoprim
17-Estradiol
Bisphenol A
Carbamazepine
Ethinylestradiol
Estriol
Estrone
Ibuprofen
Ketoprofen
Naproxen
Propranolol
Diclofenac
Galaxolide
Gembrozil
Nonylphenol
Tonalide
Triclosan
0.1
1.9
0.9
0.9
4.0
3.3
2.5
3.7
2.5
3.1
3.9
3.1
3.2
3.5
4.5
5.4
4.8
5.8
5.8
4.8
0.039
0.239
0.003
0.226
0.100
0.028
0.011
0.071
0.036
0.106
0.087
0.153
0.034
0.059
0.129
0.150
0.090
0.144
0.072
0.052
1.182
0.054
0.157
0.017
0.013
0.063
0.019
0.011
0.046
0.043
0.036
0.018
0.055
0.031
0.125
0.004
0.050
0.071
0.006
0.080
0.001
0.594
0.002
0.017
0.001
0.016
0.080
0.070
0.021
0.127
0.090
0.052
0.011
0.013
0.026
0.042
0.033
0.035
0.028
0.028
0.058
0.071
0.461
0.011
0.138
0.035
0.168
0.050
0.019
0.016
0.043
0.087
0.013
0.116
0.091
0.001
0.077
0.188
0.216
0.156
0.119
0.077
0.066
0.257
0.002
0.038
0.002
0.029
0.007
0.004
0.007
0.060
0.010
0.005
0.000
0.006
0.030
0.030
0.021
0.019
0.033
0.058
0.017
0.055
0.156
Medium
High
186
somewhere between the unweighted (Fig. 3a) and weighted (Fig. 3b)
data. Nevertheless, this clearly demonstrates that 1) the most widely
used sewage treatment technology globally appears to provide the
poorest comparative removal of a range of important TrOCs, and
2) more research is necessary to evaluate treatment technologies
other than CAS. This is of further importance because it illustrates the
risk of uncertainty that is associated with making conclusions based
on individual studies, and demonstrates how consideration of a broader
dataset allows stronger conclusions to be made.
In meta-analyses, it is important to consider and account for as many
sources of heterogeneity as possible, as this lends strength when
interpreting results and forming overall conclusions (Higgins and
Thompson, 2002). In the present study, the impact of hydraulic ow
rate and the lipophilicity (Kow) of the studied compounds were evaluated as potential sources of heterogeneity. A pH dependent octanolwater partition coefcient (Dow) can often be calculated provided Kow
and the acid dissociation constant of the compound is known (pKa),
and this can also serve as a robust indicator of sorption potential (Supplementary Table 2). However, it was not possible to consider this as a
possible source of heterogeneity, due to incomplete reporting of water
quality characteristics amongst the included studies.
The differences in ow rates observed amongst the various treatment technologies could be expected to have a signicant inuence
on removal efciencies, although this may not hold true for all
treatment systems (Dong et al., 2011). Nevertheless, in light of the pronounced differences in the proportion of data pertaining to the different
treatment technologies (i.e., signicantly more studies related to CAS
systems), hydraulic loading rate was controlled for as a potential source
of heterogeneity in the global dataset. Roughly 30% of studies did not report sewage ow rate, making mathematical correction (i.e., weighting
data based on ow rate) a tenuous approach. Since the average ow rate
reported for CAS systems was notably greater than the ow to all other
treatment options (Fig. 2), a subgroup analysis was performed
(Borenstein and Higgins, 2013) using only those CAS studies with reported ow rate less than or equal to 65,000 m3/day. Unfortunately,
there was no mechanism to effectively adjust the lower ow rates commonly reported for PCW systems. However, if ow truly represents an
important source of heterogeneity, re-analysis after exclusion of a
large proportion of CAS studies would be expected to yield a dramatically different outcome.
This was not the case, and the overall results of the subgroup analysis were highly comparable with that observed with the full unweighted
global dataset (Fig. 4a). This suggests that differences in ow rates
amongst studies are not a major factor inuencing comparative SREs
amongst the 5 treatment technologies. For consistency, the SREs of the
subgroup data were weighted based on the number of available removal estimates for each treatment option, and this again revealed a
similar pattern to the full weighted data set (Fig. 4b). To clarify, the
fact that ow rate was not found to be a major source of heterogeneity
in the present study does not mean that this is not an important factor
inuencing chemical removal amongst different approaches to sewage
treatment. However, the goal of the present meta-analysis is to provide
a broad comparison of contaminant removal efciencies amongst different types of sewage treatment systems, and it is somewhat outside of
the scope of the present dataset to explore removal mechanisms.
Another potential source of heterogeneity could relate to differences
in sorption coefcients (Kow) of the studied compounds. Numerous researchers have indicated that sorption is a key factor inuencing chemical removal during wastewater treatment (Cirja et al., 2008; Luo et al.,
2014; Rogers, 1996), although it has also been suggested that sorption
may be far less important than other factors (Andersen et al., 2005).
While there is some evidence suggesting similar sorption capacity between CAS and MBR treatment systems (Cirja et al., 2008), differences
in Kow were nevertheless explored as a potential source of heterogeneity in the global dataset. This was again achieved by performing subgroup analysis, this time by splitting the full dataset into three groups
Fig. 3. Standardized Removal Efciencies (mean 95 CI) for a) for the full unweighted
dataset (SRE), and b) with data weighted by the number of removal estimates available
for each of the various treatment option (SRE).
Fig. 4. Standardized Removal Efciencies (mean 95 CI) for a) for the subgroup analysis
with CAS loading rates b 65.000 m3/day (SRE), and b) with data weighted by the number
of removal estimates for each treatment option (SRE).
Fig. 2. Average reported loading rates to the different treatment systems (m3/day) from
the full global dataset. Dashed line indicates the 65,000 m3/day cut-off for inclusion in
the related sub-group analysis.
Fig. 5. Standardized Removal Efciencies (mean 95 CI) of TrOCs with a) low (Log
Kow b 2.5), b) medium (2.5 Log Kow 4) and c) high (Log Kow N 4) sorption potential.
187
4. Conclusions
Choosing the most effective sewage treatment technology for any
given situation requires careful consideration of various environmental,
economic, and social implications. The present study addresses the
identied need for research assessing the comparative removal efciencies of various leading sewage treatment technologies, but does not
consider economic or social aspects. One important outcome from the
analysis is the observation that CAS treatment systems are ostensibly
the least-effective options for removing EDCs and PPCPs from wastewater. Considering that CAS systems are also not considered to be costeffective, this highlights the need to identify effective solutions to improve global sewage treatment. The results reveal that MBR systems
may offer the highest level of removal of organic contaminants. However, issues with membrane fouling continue to present difculties
and raise operational expenditures, and unless practical solutions are
identied the benets of MBR treatment may not outweigh the costs.
A wide range of chemical characteristics, operational parameters,
and various other factors can inuence the removal of organic contaminants from sewage. Due to inconsistencies in reporting, it was unfortunately not possible to effectively control for all possible sources of
heterogeneity through the analysis of the data. Nevertheless, several
factors known to inuence chemical removal were controlled for
(i.e., ow rate and sorption potential) with no major impact on the
overall conclusions of the study. It can therefore be concluded that
MBR systems exhibit marginally greater overall removal for a range of
contaminants, compared to other leading treatment options. However,
a consideration of construction and operational costs, relative toxicities
of different contaminants, and the induced environmental threat associated with the high energy consumption of advanced treatment
(e.g., MBR) are all important when evaluating the benets of different
treatment technologies. While this falls outside the scope of the present
analysis, this study provides a rst of its kind comparative assessment of
leading sewage treatment technologies, and is therefore an important
contribution to discussions surrounding the identication of effective
options for the elimination of important TrOCs from wastewater.
188
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