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4 AUTHORS:
Raktim Pal
Megharaj Mallavarapu
University of Newcastle
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Paul Kirkbride
Ravi Naidu
Flinders University
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Review
Centre for Environmental Risk Assessment and Remediation, University of South Australia, Mawson Lakes, Adelaide, South Australia 5095, Australia
CRC for Contamination Assessment and Remediation of the Environment, University of South Australia, Australia
Australian Federal Police Forensic and Data Centres, Canberra, Australia
a r t i c l e
i n f o
Article history:
Received 15 March 2012
Received in revised form 28 May 2012
Accepted 28 May 2012
Available online 21 June 2012
Guest Editors: Ravi naidu, Ming Wong
Keywords:
Illicit drug
Emerging contaminant
Wastewater
Surface water
Groundwater
Ecotoxicity
a b s t r a c t
Illicit drugs and their metabolites are the latest group of emerging pollutants. Determination of their concentration in environment (such as water bodies, soil, sediment, air) is an indirect tool to estimate the community level consumption of illicit drug and to evaluate potential ecotoxicological impacts from chronic low
level exposure. They enter the wastewater network as unaltered drugs and/or their active metabolites by
human excretion after illegal consumption or by accidental or deliberate disposal from clandestine drug laboratories. This article critically reviews the occurrence and concentration levels of illicit drugs and their metabolites in different environmental compartments (e.g., wastewater, surface waters, groundwater, drinking
water, and ambient air) and their potential impact on the ecosystem. There is limited published information
available on the presence of illicit drugs in the environment, reports are available mainly from European
countries, UK, USA, and Canada but there is a lack of information from the remainder of the world. Although
the environmental concentrations are not very high, they can potentially impact the human health and ecosystem functioning. Cocaine, morphine, amphetamine, and MDMA have potent pharmacological activities
and their presence as complex mixtures in water may cause adverse effect on aquatic organisms and
human health. However, there is no current regulation demanding the determination of occurrence of
these emerging pollutants in treated wastewater, surface water, drinking water, or atmosphere. Thus, critical
investigation on distribution pattern of this new group of emerging contaminant and their potential harmful
impact on our environment needs immediate attention.
2012 Published by Elsevier B.V.
Contents
1.
2.
3.
Introduction . . . . . . . . . . . . . . . . . . . . . . . .
The potential for distribution of illicit drugs and metabolites in
Illicit drugs in environment . . . . . . . . . . . . . . . . .
3.1.
Wastewater . . . . . . . . . . . . . . . . . . . .
3.2.
Surface water . . . . . . . . . . . . . . . . . . . .
3.3.
Groundwater and drinking water . . . . . . . . . .
3.4.
Sewage sludge . . . . . . . . . . . . . . . . . . .
3.5.
Air . . . . . . . . . . . . . . . . . . . . . . . . .
4.
Ecotoxicity of illicit drugs . . . . . . . . . . . . . . . . .
5.
Methodology used to analyse illicit drugs in environment . .
6.
Conclusion. . . . . . . . . . . . . . . . . . . . . . . . .
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . .
References . . . . . . . . . . . . . . . . . . . . . . . . . . .
. . .
water
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1080
1079
1080
1081
1081
1084
1084
1084
1084
1087
1088
1090
1090
1090
Corresponding authors at: Centre for Environmental Risk Assessment and Remediation, University of South Australia, Mawson Lakes, Adelaide, South Australia 5095, Australia.
Tel.: + 61 8 83025041; fax: + 61 883023057.
E-mail addresses: Megharaj.Mallavarapu@unisa.edu.au (M. Megharaj), Ravi.Naidu@crccare.com (R. Naidu).
0048-9697/$ see front matter 2012 Published by Elsevier B.V.
doi:10.1016/j.scitotenv.2012.05.086
1080
1. Introduction
Drug abuse is a global problem with signicant direct or indirect
adverse impacts on human health and social welfare (Grifths et al.,
2008; Sloan, 2008; Rieckermann and Christakos, 2008; EMCDDA,
2007). Illicit drugs are those for which nonmedical use is prohibited
by the national or international laws (Hall et al., 2008). Illicit drugs
fall into the categories of opioids, cocaine, cannabis, amphetaminetype substances (ATSs), and ecstasy-group substances (Hall et al.,
2008; UNODC, 2007). ATSs (largely amphetamine and methamphetamine) and ecstasy (3,4-methylenedioxymethamphetamine (MDMA))
currently demand the most attention by law enforcement agencies
(Grifths et al., 2008; EMCDDA, 2007; Logan, 2001). Globally, ATSs and
ecstasy are the second most commonly consumed illicit drugs after cannabis, and they are attractive to clandestine laboratory operators due to
the easy availability of the precursor chemicals and their ease of
manufacturing (EMCDDA, 2008; UNODC, 2008a). Although some notable exceptions have occurred in some critical areas, the global markets
for almost every kind of illicit drug showed signs of overall stabilization
in 20052006, in terms of cultivation, production or consumption
(UNODC, 2008b, 2007). However, the use of ATSs continued to exceed
that of heroin and cocaine combined (UNODC, 2008a), and millions of
individuals are reported to be current users of ATS drugs. In fact,
human use of these psychoactive substances is virtually universal
(Grifths et al., 2008).
The methods of administration of illicit drugs are generally oral,
intranasal (snorting powder), by needle injection, or by inhaling
smoke (EMCDDA, 2008; NIDA, 2008). Our environment is the ultimate destination for all these compounds following their metabolism
in the human body and/or accidental or deliberate disposal of illicit
drugs and associated compounds. In common with legal pharmaceuticals, a large proportion of the administered drug may be excreted as
the parent compound and/or metabolites, through human urine and
faeces, and discharged directly into the sewage system (Castiglioni
et al., 2007; Al-Rifai et al., 2007; Roberts and Thomas, 2006; Zuccato
et al., 2005; Daughton, 2001). Additionally, clandestine chemicals
(e.g., drugs, their precursors, by-products, etc.) are also illegally buried in soil, disposed of into sinks and toilets to nd their way into
sewerage systems and public wastewater treatment facilities, or
dumped in public solid waste facilities (Janusz et al., 2003; Scott et
al., 2003). These chemicals undergo diverse processes after their release into the environment, such as sorption, degradation, leaching,
and transport in surface runoff, and interactions with soils, sediments,
groundwater, surface water, with potential implications for humans
and wildlife. Some of the illicit drugs are comparatively more polar
than the pollutants of historic concern and not readily sorbed to
sub-soils, or other materials low in organic matter, and may enter
the surface or ground waters (Jones-Lepp et al., 2004). Cannabinoids
are highly hydrophobic and are found bound to sewage sludge solids
(Daz-Cruz et al., 2009). We reported the degradation pattern of certain parent drugs, precursor, and manufacturing by-products in soil
and their impact on soil microbiological properties (Pal et al., 2011,
2012; Janusz et al., 2003; Scott et al., 2003). Methamphetamine was
found to be relatively persistent with half-life values in soil up to
502 days (Pal et al., 2011).
The term emerging pollutants has been dened as substances that
are not presently known to cause impairments in water systems but
have characteristics such as the ability to bioaccumulate, persistence
in the environment, and toxicity that suggest that they could impact
the integrity of water (Boles and Wells, 2010). Illicit drugs (both plant
derived and synthetic drugs) are the latest group of emerging pollutants
identied in the aquatic environment demanding attention (Boleda et
al., 2009; Kasprzyk-Hordern et al., 2010). These compounds may have
potent pharmacological and biological activities and their presence in
surface waters even at low concentrations, together with the residues
of many therapeutic pharmaceuticals and other organic compounds,
may lead to unexpected pharmacological interactions causing toxic effects to aquatic organisms. In addition, they may cause a wide variety
of environmental and health problems (Zuccato et al., 2008;
Castiglioni et al., 2007; Al-Rifai et al., 2007; Pomati et al., 2006). Analysis
of illicit drugs in wastewater and surface water by means of mass spectrometry and the occurrence of these compounds in environmental waters have been reviewed by Castiglioni et al. (2008) and Postigo et al.
(2008a), respectively. However, the current state of knowledge on the
concentrations, frequency, and geographic distribution patterns of illicit
drugs in the environment (especially water bodies and ambient air) as
reported from various parts of the world has not yet been encapsulated
in a review article.
Water bodies can be considered to be the most susceptible environmental matrices for contamination by illicit drugs and associated compounds, just as they are for legal pharmaceuticals and personal care
products (PPCPs) after their ingestion and excretion, external application, or disposal (Daughton, 2001). Illicit drugs have also the potential
to escape to the atmosphere, but their determination has not attracted
attention. Illicit drugs are suspected to promote long term ill health
effects even when present at low concentrations in the ambient air
(Cecinato et al., 2010). Information on the worldwide prevalence of
illicit drugs is a prerequisite to identify and foster timely plans on
safe and appropriate control measures to prevent their spread in
the environment and to protect human and ecological health. The
aim of this review is to develop a critical overview of the occurrence
and concentrations of the different groups of illicit drugs in aquatic
systems (waste and surface waters) and ambient air worldwide
and their potential ecotoxicological impact on the environment.
2. The potential for distribution of illicit drugs and metabolites in
water
Illicit drugs and their metabolites are continuously discharged into
wastewaters due to human excretion after legal or illegal consumption
or occasional direct disposal of clandestine laboratory wastes into sewage systems (Gonzlez-Mario et al., 2012; Boles and Wells, 2010).
After their consumption, drugs are excreted unaltered and/or as metabolites in urine, faeces, saliva, and sweat and the process of excretion occurs consistently even when illicit drugs are administered via different
methods injecting, smoking, snorting, swallowing and so forth
(Verster, 2010; Vazquez-Roig et al., 2010; Prichard et al., in press). The
proportion of consumed drugs excreted unaltered and as their metabolites in urine and faeces can be summarized as follows: cocaine
(unaltered (19%); benzoylecgonine (3554%); ecgonine methyl ester
(3249%)); amphetamine (unaltered 3040%), methamphetamine
(unaltered 4362%); MDMA (unaltered 65%); heroin (excreted as morphine 42.5%); and THC (unaltered 6590% through faeces and 1025%
through urine) (van Nuijs et al., 2011a; Boles and Wells, 2010;
Gheorghe et al., 2008; Bischoff, 2007). Chiaia et al. (2008) and van
Nuijs et al. (2009a,b) reported that in urine, a large proportion (80%)
of cocaine can be accounted for in the form of benzoylecgonine and
ecgonine methyl ester with both excreted at higher concentration
than cocaine. Amphetamine group compounds are primarily excreted
as the intact drug (Boles and Wells, 2010) but the excretion rate can
change with the pH of urine of that particular user, route of intake,
and dose (van Nuijs et al., 2011a). Although amphetamine and methamphetamine are excreted mostly as unaltered drugs, metabolites of
these drugs are also excreted and several additional metabolites may
form during sewage treatment processes (Boles and Wells, 2010).
The residues of illicit drugs found in consumers' urine that enter
the sewage network with wastewater are only partially removed by
STPs (Zuccato and Castiglioni, 2009). In urine drugs are generally
detected in the ppm range, but in wastewater and surface waters
their concentration is much lower at ppb levels (Verster, 2010).
The decrease in concentration of illicit drugs and their metabolites
in sewage efuents and surface waters depend on the technologies
1081
1082
Table 1
Concentration of cocainics, opioids, and cannabinoids in wastewater.
Compound
Country
Study site
Study period
Concentration (ng L 1)
Inuent
Cocaine
Italy
Switzerland
Italy/Switzerland
Spain
Belgium
UK
Benzoylecgonine
Ireland
France
Croatia
USA
Canada
Italy
Switzerland
Italy/Switzerland
Spain
Germany
Belgium
UK
Ireland
France
Croatia
USA
Canada
Australia
Belgium
Italy
Switzerland
Italy/Switzerland
Cagliari
Latina
Cuneo
Varese
Milan
WWTPs at Florence
Lugano
STPs at Bern, Basel, Geneva, Lucern, Zurich
42 different towns in NE-Spain
Catalonia in NE-Spain
STPs located at east coast
7 different STPs
STP that gives service only to penal complex
WWTP in Castelln province
5 STPs located in NW Spain
STPs located in NW Spain
STP at Almera
WWTPs in Flanders
11 different WWTP
30 different WWTP
37 different WWTP
41 different WWTP
WWTP in Brussel-Noord
WWTP Brussels
Cilfynydd
WWTP Cilfynydd
WWTP Coslech
Ringsend, Shanganagh, Leixlip, Navan
WWTP at different suburbs of Paris
WWTP at city of Zagreb
WWTPs around US
WWTPs serving three Canadian cities
Cagliari
Latina
Cuneo
Varese
Milan
WWTPs at Florence
Lugano
STPs at Bern, Basel, Geneva, Lucern, Zurich
42 different towns in NE-Spain
Catalonia in NE-Spain
STPs located at east coast
7 different STPs
STP that gives service only to penal complex
WWTP in Castelln province
5 STPs located in NW Spain
STPs located in NW Spain
STP at Almera
STP in Vila-Seca
12 German STPs
WWTPs in Flanders
11 different WWTP
30 different WWTP
37 different WWTP
41 different WWTP
WWTP in Brussel-Noord
WWTP Brussels
Cilfynydd
WWTP Cilfynydd
WWTP Coslech
Ringsend, Shanganagh
WWTP at different suburbs of Paris
WWTP at city of Zagreb
WWTPs around US
WWTPs serving three Canadian cities
Metropolitan WWTPs in South Australia
11 different WWTP
Milan
Lugano
2004
Feb 2006
Jul 2006Jun 2007
Mar 2006
JulOct 2009
Apr 2006Jan 2007
AprSep 2006
Jul 2007
Oct 2007Jul 2008
Jun 2008Jan 2009
JunJul 2008
Feb 2011
MayJun 2010
Feb 2006Sept 2007
Aug 2007Jan 2008
20072008
20072008
20072008
Feb 2008
Mar 2009Jan 2010
Nov 2006
MarSep 2009
Oct 2008Aug 2009
2004
Feb 2006
Jul 2006Jun 2007
Mar 2006
JulOct 2009
Apr 2006Jan 2007
AprSep 2006
Jul 2007
Oct 2007Jul 2008
Jun 2008Jan 2009
JunJul 2008
Feb 2011
MayJun 2010
Nov 2009
Mar and Nov 2005
Feb 2006Sept 2007
Aug 2007Jan 2008
20072008
20072008
20072008
Feb 2008
Mar 2009Jan 2010
Nov 2006
MarSep 2009
Oct 2008Aug 2009
Apr 2009Oct 2009
Aug 2007Jan 2008
Feb 2006
Mar 2006
83
76
120
42
421.4
50
218.4
248
2001000c
44700c
79
592
384d
128
608
163
179
474
205
126
189
153
218
346
329
526
521
207
489
4.8282c
52d
235
209823c
640
420
750
390
1132.1
127
547.4
604
2001000d
97500c
810
2149
1310d
556
4750
907
447
2541
78
753
375
485
510
603
831
645
1229
992
1082
290
64849c
178d
1131
2872624c
52
89
36.6
18.8
436.6c
Efuent
Reference
no.a
[1]
b 0.99(LOQb)
10.7
b 15(LOQ)
1100d
17
57
16.8d
540
52
26.55
171
149
128
b 1(LOQ)
93.3
1.25.3c
25d
b 20(LOQ)530c
b 0.92(LOQ)
100.3
96
11500c
216
155
115d
3425
407
189
1010
914
49
1597
1091
13
26.5
7.9149c
79d
62775c
b 0.56(LOQ)
7.5
[2]
[3]
[2]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[26]
[27]
[28]
[12]
[13]
[14]
[15]
[16]
[14]
[29]
[17]
[18]
[18]
[19]
[20]
[30]
[21]
[22]
[1]
[1]
[1]
[1]
[2]
[3]
[2]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[26]
[27]
[28]
[31]
[23]
[12]
[13]
[14]
[15]
[16]
[14]
[29]
[17]
[18]
[18]
[19]
[20]
[30]
[21]
[22]
[24]
[13]
[2]
[2]
[5]
1083
Table 1 (continued)
Compound
Norbenzoylecgonine
Norcocaine
Cocaethylene
Morphine
Country
Spain
USA
Italy
Switzerland
Italy/Switzerland
USA
Italy
Switzerland
Italy/Switzerland
Spain
Italy
Switzerland
Italy/Switzerland
Germany
Spain
6-Acetylmorphine
Ireland
Croatia
Italy
Switzerland
Italy/Switzerland
Spain
Morphine-3-D-glucuronide
Methadone
Belgium
Croatia
Italy
Switzerland
Italy
Switzerland
Italy/Switzerland
Germany
Spain
Belgium
EDDP
Croatia
USA
Italy
Switzerland
Italy/Switzerland
Spain
Belgium
9-tetrahydrocannabinol
Ireland
Croatia
Italy
Switzerland
Italy/Switzerland
Spain
Study site
Study period
JunJul 2008
Feb 2006
Mar 2006
WWTPs around US
Milan
Lugano
Feb 2006
Mar 2006
Jul 2007
Oct 2007Jul 2008
Jul 2008
Feb 2006
Jul 2006Jun 2007
Mar 2006
JulOct 2009
12 German STPs
WWTP
WWTPs in NE-Spain
STPs located at east coast
7 different STPs
STP that gives service only to penal complex
5 STPs located in NW Spain
STPs located in NW Spain
STP at Almera
STP in Vila-Seca
Catalonia in NE-Spain
Swords, Navan
WWTP at city of Zagreb
Milan
Lugano
STPs at Bern, Basel, Geneva, Lucern, Zurich
7 different STPs
STP that gives service only to penal complex
WWTP Brussels
WWTP at city of Zagreb
Milan
Lugano
Milan
Lugano
STPs at Bern, Basel, Geneva, Lucern, Zurich
WWTP
WWTPs in NE-Spain
STP that gives service only to penal complex
Catalonia in NE-Spain
STP at Almera
STPs located in NW Spain
11 different WWTP
WWTP Brussels
WWTP at city of Zagreb
WWTPs around US
Milan
Lugano
STPs at Bern, Basel, Geneva, Lucern, Zurich
MarJul 2007
MarMay 2007
Jun 2008Jan 2009
AprMay 2007
MayJun 2010
Feb 2011
Aug 2007Jan 2008
Mar 2009Jan 2010
MarSep 2009
Feb 2006
Mar 2006
JulOct 2009
WWTPs in NE-Spain
STP that gives service only to penal complex
Catalonia in NE-Spain
STP at Almera
STPs located in NW Spain
11 different WWTP
WWTP Brussels
Ringsend, Swords, Leixlip, Navan
WWTP at city of Zagreb
Milan
Lugano
MarMay 2007
Jun 2008Jan 2009
AprMay 2007
MayJun 2010
Feb 2011
Aug 2007Jan 2008
Mar 2009Jan 2010
Nov 2006
MarSep 2009
Feb 2006
Mar 2006
WWTPs in NE-Spain
Catalonia in NE-Spain
STPs located in NW Spain
7 different STPs
MarMay 2007
AprMay 2007
Feb 2011
Oct 2007Jul 2008
Feb 2011
MayJun 2010
Nov 2009
AprMay 2007
Nov 2006
MarSep 2009
Feb 2006
Mar 2006
JulOct 2009
Concentration (ng L 1)
Inuent
Efuent
290
75.2
13.7
4.3
436.6c
19.5
11.5
5.9
436.6c
78.3
18.1d
150
83.3
12.3
204.4
1007
80200c
310d
300d
54.1
91.8
94.4d
1346
137
21
152
90
25.5278
287d
11.8
10.4
38
510c
2.7d
63
13
12d
2.5
18.1
11.6
49.7
112
1090c
88d
12.7
4704
3.41531
45
28.7
19.1
54
55d
33.7
19.8
91.3
315
1090c
19.7
9262
3.31029
138
40.44
36.8
109
136d
62.7
91.2
6090c
63.8
11.3127
126
18.0d
b 1.92(LOQ)
0.7
b 0.95(LOQ)
0.2
3.6
1.5d
80
b 3.95(LOQ)
55.4
929
40d
25d
51
20.5
46.4d
102
73
545
1281.1
663
53d
b 5.3(LOQ)
b 5.3(LOQ)
b 5(LOQ)
1.8d
b 0.63(LOQ)
b 0.63(LOQ)
9.1
36.2
65
87d
11.4
3.4732
18
17.6
36d
22.6
72.1
294
22.4
2.71150
64
27.45
82.5
124d
b 1.75(LOQ)
7.2
39.2
4.2d
32.2
7.9d
Reference
no.a
[11]
[21]
[2]
[2]
[5]
[21]
[2]
[2]
[5]
[8]
[9]
[11]
[2]
[3]
[2]
[4]
[5]
[23]
[33]
[25]
[8]
[9]
[10]
[26]
[27]
[28]
[31]
[32]
[19]
[30]
[2]
[2]
[4]
[5]
[9]
[10]
[29]
[30]
[2]
[2]
[2]
[2]
[4]
[5]
[33]
[25]
[10]
[32]
[28]
[27]
[13]
[29]
[30]
[21]
[2]
[2]
[4]
[5]
[25]
[10]
[32]
[28]
[27]
[13]
[29]
[19]
[30]
[2]
[2]
[5]
[25]
[32]
[27]
[9]
1084
of cocaine and benzoylecgonine in surface waters was reported at relatively higher concentrations from Spain, Belgium, and Italy. The concentrations of amphetamine and MDMA were recorded higher in the
surface waters from Spain while methamphetamine was higher in
USA. Although the concentrations of different drugs and their metabolites in surface waters are in the few nanogram per litre range, their
possible effects on wildlife and human health cannot be disregarded
especially on vulnerable populations (Valcrcel et al., 2012). The concentrations of some illicit drugs in natural waters occur at similar
level to other emerging contaminants (e.g., psychiatric drug carbamazepine and the anti-inammatory diclofenac) leading to their inclusion in the list of priority substances of the European Union
Water Framework Directive (Gonzlez-Mario et al., 2010).
3.3. Groundwater and drinking water
A major concern about the presence of illicit drugs and metabolites in the environment is that drinking water treatment plants
(DWTPs) cannot adequately treat surface or groundwater before it
is supplied as drinking water to the community (Boleda et al., 2009;
Valcrcel et al., 2012). At present there is little information dealing
with the presence of illicit drugs and metabolites in drinking water;
a few recent reports from Spain deal with this issue (Huerta-Fontela
et al., 2008b; Boleda et al., 2009, 2011; Valcrcel et al., 2012) and
groundwater (Jurado et al., 2012) as presented in Table 5.
The case study on Barcelona urban groundwater showed relatively
higher frequencies of detection and concentrations for cocaine,
MDMA, and methadone among different chemical classes of drugs
and metabolites (Jurado et al., 2012). The removal efciency in conventional drinking water treatment showed complete removal for almost all the illicit drugs and metabolites with few exceptions for
benzoylecgonine, methadone, and EDDP (Huerta-Fontela et al.,
2008b; Boleda et al., 2009). However, cocaine, benzoylecgonine,
methadone and its metabolite EDDP were frequently detected in tap
water (Boleda et al., 2011; Valcrcel et al., 2012).
3.4. Sewage sludge
The illicit drugs in sewage sludge, bio-solids, and sediments have
received little attention. First reports on the presence of amphetamine (5300 g kg 1) in sewage sludge of Austria were reported
by Kaleta et al. (2006) and methamphetamine (4 g kg 1 dry
weight) in the bio-solids from Los Angeles, USA by Jones-Lepp and
Stevens (2007). Sorption of illicit drugs in sediments was rst
reported by Wick et al. (2009), the sorption coefcients (Kd,
L kg 1) of morphine and methadone were recorded at 12 and 76. Although there is no report on the occurrence of cannabinoids in sewage sludge, they are likely to be found bound to sewage sludge due
to their high human consumption rate and high hydrophobicity
(Daz-Cruz et al., 2009).
3.5. Air
Illicit drugs have the potential to escape to the ambient air in powder
form during consumption (e.g., cocaine) or handling and as smoke during consumption (e.g., cannabis, methylamphetamine or heroin)
Note to Table 1:
a
Reference no.: [1] Zuccato et al. (2005), [2] Castiglioni et al. (2006), [3] Mari et al. (2009), [4] Berset et al. (2010), [5] Castiglioni et al. (2007), [6] Huerta-Fontela et al. (2008a),
[7] Huerta-Fontela et al. (2007), [8] Postigo et al. (2008b), [9] Postigo et al. (2010), [10] Postigo et al. (2011), [11] Bijlsma et al. (2009), [12] Gheorghe et al. (2008), [13] van Nuijs
et al. (2009a), [14] van Nuijs et al. (2009d), [15] van Nuijs et al. (2009c), [16] van Nuijs et al. (2009b), [17] Kasprzyk-Hordern et al. (2008), [18] Kasprzyk-Hordern et al. (2009),
[19] Bones et al. (2007), [20] Karolak et al. (2010), [21] Chiaia et al. (2008), [22] Metcalfe et al. (2010), [23] Hummel et al. (2006), [24] Irvine et al. (2011)), [25] Boleda et al.
(2007), [26] Gonzlez-Mario et al. (2010), [27] Gonzlez-Mario et al. (2012), [28] Bueno et al. (2011), [29] van Nuijs et al. (2011b), [30] Terzic et al. (2010), [31] Pedrouzo
et al. (2011), [32] Boleda et al. (2009), [33] Wick et al. (2009).
b
Limit of quantication.
c
Range.
d
Median value.
1085
Table 2
Concentration of amphetamine and ecstasy group compounds in wastewater.
Compound
Amphetamine
Country
Italy
Spain
UK
Belgium
Methamphetamine
Croatia
USA
Canada
Italy
Spain
Belgium
USA
MDA
Canada
Australia
Italy
Switzerland
Spain
MDMA
USA
Italy
Switzerland
Spain
Belgium
Croatia
UK
USA
MDEA
Canada
Australia
Italy
Spain
Study site
Milan
Catalonia in NE-Spain
42 different towns in NE-Spain
STPs located at east coast
7 different STPs
STP that gives service only to penal complex
WWTP in Castelln province
STP at Almera
STPs located in NW Spain
Cilfynydd
WWTP Cilfynydd
WWTP Coslech
4 different WWTPs
11 different WWTP
WWTP Brussels
WWTP at city of Zagreb
WWTPs around US
WWTPs serving three Canadian cities
Milan
42 different towns in NE-Spain
STPs located at east coast
7 different STPs
STP that gives service only to penal complex
STP at Almera
11 different WWTP
WWTP Brussels
Nevada
WWTPs around US
Murray WWTP
Omaha, NE
WWTPs serving three Canadian cities
Metropolitan WWTPs in South Australia
Milan
Lugano
42 different towns in NE-Spain
WWTP in Castelln province
STP at Almera
WWTPs around US
Milan
Lugano
STPs at Bern, Basel, Geneva, Lucern, Zurich
Catalonia in NE-Spain
42 different towns in NE-Spain
STPs located at east coast
7 different STPs
STP that gives service only to penal complex
WWTP in Castelln province
STPs located in NW Spain
11 different WWTP
WWTP Brussels
WWTP at city of Zagreb
4 different WWTPs
South Carolina
WWTPs around US
WWTPs serving three Canadian cities
Metropolitan WWTPs in South Australia
Milan
Catalonia in NE-Spain
42 different towns in NE-Spain
Study period
Feb 2006
AprSep 2006
Apr 2006Jan 2007
Jul 2007
Oct 2007Jul 2008
Jun 2008Jan 2009
Jul 2008
MayJun 2010
Feb 2011
Concentration (ng L 1)
Inuent
Efuent
14.7
15
3688c
25.9
148d
97
1400
496
64.1
5236
4310
1196
85.9
206
59
7.3d
206
b 3(LOQ)25c
16.2
3277c
8.2
4.6d
87
614
3.5
3.3
b 2.8(LOQb)
b 1(LOQ)
4210c
1.8
25.7d
1.0d
b 1(LODe)14c
3.5
390c
3.1
1.3d
1.05
800
18
b 7(LOQ)65c
587
4.6
b 8.7(LOQ)
3266c
1690
266
5.0
14.2
13.6
26
49
2598c
135
20.4d
61
15,380
25.6
34.5
10.5
3.4d
6.4
July 2002
Oct 2008Aug 2009
Apr 2009Oct 2009
Feb 2006
AprSep 2006
Apr 2006Jan 2007
210
225
14.2
127
201
2
23.2
935
187
1.5
28
6114c
350
b 2(LOD)95c
1.1
0.9
1200c
680
4.4
5.1
b 11(LOQ)
41
2267c
132
12.7d
10,955
2.0d
6.7
0.5
b 3(LOD)32
b 1.64(LOQ)
b 2.1(LOQ)
12
Reference
no.a
[1]
[2]
[3]
[4]
[5]
[6]
[7]
[19]
[20]
[8]
[9]
[9]
[10]
[11]
[21]
[22]
[12]
[13]
[1]
[2]
[4]
[5]
[6]
[19]
[11]
[21]
[14]
[12]
[15]
[16]
[13]
[17]
[1]
[1]
[2]
[7]
[19]
[12]
[1]
[1]
[18]
[2]
[3]
[4]
[5]
[6]
[7]
[20]
[11]
[21]
[22]
[10]
[14]
[12]
[13]
[17]
[1]
[2]
[3]
a
Reference no.: [1] Castiglioni et al. (2006), [2] Huerta-Fontela et al. (2007), [3] Huerta-Fontela et al. (2008a), [4] Postigo et al. (2008b), [5] Postigo et al. (2010), [6] Postigo et al. (2011),
[7] Bijlsma et al. (2009), [8] Kasprzyk-Hordern et al. (2008), [9] Kasprzyk-Hordern et al. (2009), [10] Kasprzyk-Hordern et al. (2010), [11] van Nuijs et al. (2009a), [12] Chiaia et al. (2008),
[13] Metcalfe et al. (2010), [14] Jones-Lepp et al. (2004), [15] Loganathan et al. (2009), [16] Bartelt-Hunt et al. (2009), [17] Irvine et al. (2011), [18] Berset et al. (2010), [19] Bueno et al.
(2011), [20] Gonzlez-Mario et al. (2012), [21] van Nuijs et al. (2011b), [22] Terzic et al. (2010).
b
Limit of quantication.
c
Range.
d
Median value.
e
Limit of detection.
(Daughton, 2011a; Viana et al., 2010). The illicit drugs and their metabolites present in the atmosphere are primarily associated with particulates due to their physico-chemical properties (low vapour pressures,
high to medium polarity, weak alkalinity, and molecular weight range
between 135 and 360 g mol 1) and have been recognised as potentially useful matrix to investigate the illicit drug consumption pattern
(Postigo et al., 2009; Viana et al., 2010). However, the atmospheric
levels of illicit drugs may be more transient and variable than levels in
1086
Table 3
Concentration of cocainics, opioids, and cannabinoids in surface water.
Compound
Country
Name of river
Study site
Study period
Concentration
(ng L 1)
Reference no.a
Cocaine
Italy
Po
Po
Olona
Lambro
Arno
Thames
2004
2006
2006
2006
2006
Oct 2005
1.2
0.5
44
15
1.7
4.7
[1]
[2]
[2]
[2]
[2]
[2]
Spain
Llobregat
Mezzano, Pavia
Mezzana, Monticelli, Piacenza, Cremona
Downstream of Varese STP
Near its entrance into River Po
Rignano, Limite, Castelfranco, Pisa
New bridge, Shillingford bridge, Chiswick bridge,
House of Parliament, Tilbury of London
Intake of drinking water treatment plant located
in the Llobregat river basin
Intake of a Drinking water treatment plant
Natural park of L'Albufera of Valencia
15 different location along the river basin
23.8
[3]
Sep 2006
Apr 2008
Oct 2007Jul 2008
Jun 2010
JunJul 2007
20072008
20072008
Nov 2006
Mar 2010
2004
2006
2006
2006
2006
Oct 2005
6
0.5
1.4b
30
44
15.3
22.4
11.9
2
2
29
0.4
25
3.7
183
50
21.8
11.2
[4]
[5]
[6]
[16]
[17]
[7]
[8]
[9]
[10]
[11]
[12]
[13]
[1]
[2]
[2]
[2]
[2]
[2]
64
[3]
Sep 2006
Apr 2008
Oct 2007Jul 2008
77
7.4
11.4b
316
142
29.2b
96
84
48.5
3b
85
55
12
1.6
0.3
8.4
3.2
1.6
7.39b
3.6
0.4
0.1
1.3
0.2
0.1
0.3b
38
3.5
3
15.8
[4]
[5]
[6]
[16]
[17]
[18]
[7]
[8]
[9]
[14]
[10]
[11]
[11]
[13]
[2]
[2]
[2]
[2]
[18]
[2]
[2]
[2]
[2]
[2]
[2]
[6]
[2]
[2]
[2]
[2]
10b
5.5
6.0
4.1
9.8b
89
16
1.74b
2.2
0.5
8.6
3.4
[14]
[15]
[5]
[19]
[6]
[16]
[17]
[18]
[13]
[2]
[2]
[2]
Llobregat
Ebro
Sar
Henares
Belgium
UK
Benzoylecgonine
Ireland
Switzerland
Italy
Spain
Taff
Taff
Broadmeadow, Liffey
Po
Po
Olona
Lambro
Arno
Thames
Llobregat
Llobregat
Ebro
Sar
Henares
Tagus
Belgium
Different rivers and brooks
28 different rivers and brooks (N = 43)
Germany
UK
Norbenzoylecgonine
Switzerland
Italy
Norcocaine
Spain
Italy
Cocaethylene
Italy
Morphine
Spain
Italy
Germany
Spain
Methadone
Switzerland
Italy
Jun 2010
Jun 2010
JunJul 2007
20072008
20072008
Mar and Nov 2005
Mar 2010
2006
2006
2006
2006
Jun 2010
2006
2006
2006
2006
2006
2006
Oct 2007Jul 2008
2006
2006
2006
Oct 2005
Mar and Nov 2005
MarMay 2007
Apr 2008
2007
Oct 2007Jul 2008
Jun 2010
Jun 2010
Mar 2010
2006
2006
2006
1087
Table 3 (continued)
Compound
Country
Methadone
Spain
EDDP
Switzerland
Italy
Spain
Name of river
Study site
Study period
Concentration
(ng L 1)
Reference no.a
Arno
Llobregat
Llobregat
Henares
Tagus
2006
MarMay 2007
2007
Jun 2010
Jun 2010
Mar 2010
2006
2006
2006
2006
MarMay 2007
2007
Jun 2010
Jun 2010
Mar 2010
2006
2006
2006
Oct 2005
4.8
6.4
2.4
7
2.58b
1.7
1
18
9.9
4.3
12.3
6.0
35
7.57b
4.9
0.3
3.7
0.5
1
[2]
[15]
[19]
[17]
[18]
[13]
[2]
[2]
[2]
[2]
[15]
[19]
[17]
[18]
[13]
[2]
[2]
[2]
[2]
MarMay 2007
Oct 2007Jul 2008
24
5.5b
[15]
[6]
Po
Olona
Lambro
Arno
Llobregat
Llobregat
Henares
Tagus
Switzerland
9-tetrahydrocannabinol
Po
Lambro
Arno
Thames
Spain
Llobregat
Ebro
a
Reference no.: [1] Zuccato et al. (2005), [2] Zuccato et al. (2008), [3] Huerta-Fontela et al. (2008b), [4] Huerta-Fontela et al. (2007), [5] Vazquez-Roig et al. (2010), [6] Postigo et al.
(2010), [7] Gheorghe et al. (2008), [8] van Nuijs et al. (2009d), [9] van Nuijs et al. (2009c), [10] Kasprzyk-Hordern et al. (2008), [11] Kasprzyk-Hordern et al. (2009), [12] Bones et al.
(2007), [13] Berset et al. (2010), [14] Hummel et al. (2006), [15] Boleda et al. (2007), [16] Gonzlez-Mario et al. (2010), [17] Bueno et al. (2011), [18] Valcrcel et al. (2012), [19] Boleda
et al. (2009).
b
Median value.
wastewater making it complex to use as a tool to detect drug abuse pattern (Daughton, 2011a).
The determination of illicit drugs and metabolites in the atmosphere
has not received much attention and the data are extremely scarce
worldwide. Reports are available in scientic literatures on the measurement of illicit drugs in ambient air only from the cities of Italy,
Spain, Portugal, Chile, Brazil, Serbia, and Algeria. Initially, Hannigan et
al. (1998) detected the presence of cocaine in outdoor air during a bioassay directed chemical analysis of Los Angeles airborne particulate
matter using a human cell mutagenicity assay. The available reports
on the concentration of illicit drugs and metabolites have been presented in Table 6. The samples collected from Algiers, Algeria and
Panevo, Serbia tested for cocaine were recorded below detection limit
(Cecinato et al., 2009a). The concentrations of benzoylecgonine, heroin,
6-acetylmorphine, 9-tetrahydrocannabinol (THC), amphetamine,
methamphetamine, and MDMA were generally recorded in low
pg m 3 range, but cocaine up to the low ng m 3 level was detected.
The results indicated the maximum occurrence of cocaine in the ambient
air followed by THC. The concentrations of synthetic illicit drugs in ambient air are relatively low.
The objective of air monitoring is mainly to detect illicit drug
usage pattern rather than concern regarding public health impacts
because the cumulative lifetime doses (e.g., cocaine 0.3 mg), even
in contaminated areas, are much less than one drug dose (Cecinato
et al., 2010; Daughton, 2011a). However, possible health hazard derived from chronic exposure to such low ambient concentrations
and potential effects of short or medium term exposures on specic
risk groups (children, elderly, and asthmatics) needs attention
(Viana et al., 2011; Cecinato et al., 2011).
4. Ecotoxicity of illicit drugs
Illicit drugs are being continuously discharged into aquatic environment due to their high production and consumption and thus continuous monitoring of sewage efuents would minimize their undesirable
effects on environment (Valcrcel et al., 2012). Many reports are available on the occurrence level of illicit drugs in water worldwide, however,
the ecotoxicity of illicit drugs has received less attention compared to licit
pharmaceuticals especially with regard to low level mixed stressor
1088
Table 4
Concentration of amphetamine and ecstasy group compounds in surface water.
Compound
Country
Name of river
Study site
Study period
Concentration
(ng L 1)
Reference no.a
Amphetamine
Spain
Llobregat
20
[1]
Apr 2008
Oct 2007Jul 2008
Jun 2010
2006
2006
3.38
6.8b
309
4
5
1
1.7
2.1
[2]
[3]
[9]
[4]
[5]
[5]
[6]
[6]
1.3
[1]
0.4b
3.22b
16.6
[3]
[10]
[7]
2006
Oct 2005
1.2
3
[6]
[6]
9.2
[1]
2006
2006
2006
2006
Oct 2005
0.2
1.7
1.1
1.0
3.6
[6]
[6]
[6]
[6]
[6]
14.1
[1]
Sep 2006
Apr 2008
Oct 2007Jul 2008
Jun 2010
3
0.9
1.0b
2.07b
[8]
[2]
[3]
[10]
UK
Methamphetamine
Italy
Spain
Ebro
Henares
Taff
Taff
Ely
Olona
Lambro
Llobregat
Ebro
Tagus
USA
MDA
MDMA
Italy
Arno
Thames
Spain
Llobregat
Italy
Po
Olona
Lambro
Arno
Thames
Spain
Llobregat
Llobregat
Ebro
Tagus
a
Reference no.: [1] Huerta-Fontela et al. (2008b), [2] Vazquez-Roig et al. (2010), [3] Postigo et al. (2010), [4] Kasprzyk-Hordern et al. (2008), [5] Kasprzyk-Hordern et al. (2009),
[6] Zuccato et al. (2008), [7] Bartelt-Hunt et al. (2009), [8] Huerta-Fontela et al. (2007), [9] Bueno et al. (2011), [10] Valcrcel et al. (2012).
b
Median value.
1089
Table 5
Concentration of illicit drugs and their metabolites in groundwater and tap water.
Compound
Country
Study site
Study period
Concentration
(ng L 1)
Reference no.a
(a) Groundwater
Cocaine
Benzoylecgonine
Cocaethylene
Morphine
Methadone
EDDP
MDMA
Spain
Spain
Spain
Spain
Spain
Spain
Spain
Barcelona
Barcelona
Barcelona
Barcelona
Barcelona
Barcelona
Barcelona
MayDec
MayDec
MayDec
MayDec
MayDec
MayDec
MayDec
3.8
1.5
0.1
1.4
7.4
0.7
3.9
[1]
Spain
Different 43 cities
Cazalegas reservoir
20082009
Jun 2010
Different 43 cities
Cazalegas reservoir
20082009
Jun 2010
Different 43 cities
Different 43 cities
Cazalegas reservoir
DWTP from Toledo City
20082009
20082009
Jun 2010
Jun 2010
Different 43 cities
Cazalegas reservoir
20082009
Jun 2010
0.4
2.11
0.1
0.6
0.4
2.47
0.2
4.5
0.2
0.2
0.47
0.99
0.1
0.2
0.4
0.34
0.4
0.1
0.4
[2]
[3]
[2]
[2]
[2]
[3]
[2]
[2]
[2]
[2]
[3]
[3]
[2]
[2]
[2]
[3]
[2]
[2]
[2]
2010
2010
2010
2010
2010
2010
2010
Benzoylecgonine
Europe
Latin Americac
Spain
Cocaethylene
Methadone
Europeb
Latin Americac
Spain
Spain
EDDP
Europeb
Latin Americac
Spain
b
Europe
Japan
Latin Americac
a
b
c
Reference no.: [1] Jurado et al. (2012), [2] Boleda et al. (2011), [3] Valcrcel et al. (2012).
Includes large cities in Austria, France, Germany, Iceland, Slovakia, Switzerland, and United Kingdom.
Cities in Argentina, Brazil, Chile, Colombia, Panama, Peru, and Uruguay.
Table 6
Concentration of illicit drugs and their metabolites in ambient air.
Compound
Country
Study site
Study period
Concentration
(pg m 3)
Reference no.a
Cocaine
Italy
20032006
2008
Sep 2007
2009
20062007
Jun 2007
20022003
Nov 2007Jan 2008
Sep 2007Jan 2008
Nov 2007Jan 2008
Sep 2007Jan 2008
20082009
Nov 2007Jan 2008
Sep 2007Jan 2008
Nov 2007Jan 2008
Sep 2007Jan 2008
20082009
SepOct 2008
SepOct 2008
Mar 2007
Nov 2007Jan 2008
Sep 2007Jan 2008
Nov 2007Jan 2008
Sep 2007Jan 2008
20082009
Nov 2007Jan 2008
Sep 2007Jan 2008
20082009
Nov 2007Jan 2008
Sep 2007Jan 2008
20082009
1098b
13267b
687b
9116b
148
2800
47590b
305.61
204480b
23.5
1429
b DL(2.49)29b
83.7
b DL84.0b
22.8
b DL22.8b
b DL(7.36)32b
44104b
3058b
39
33.2
2744b
2.02
1.42.3b
b DL(1.05)15b
3.49
0.93.5b
b DL(2.73)10b
2.90
b DL2.9b
b DL(1.26)5b
[1]
[4]
[5]
[6]
[4]
[4]
[4]
[2]
[7]
[2]
[7]
[8]
[2]
[7]
[2]
[7]
[8]
[3]
[3]
[3]
[2]
[7]
[2]
[7]
[8]
[2]
[7]
[8]
[2]
[7]
[8]
Portugal
Chile
Brazil
Spain
Benzoylecgonine
Spain
Heroin
Spain
6-Acetylmorphine
Spain
9-tetrahydrocannabinol
Italy
Spain
Amphetamine
Spain
Methamphetamine
Spain
MDMA
Spain
DL = Detection limit.
a
Reference no.: [1] Cecinato and Balducci (2007), [2] Postigo et al. (2009), [3] Balducci et al. (2009), [4] Cecinato et al. (2009a), [5] Cecinato et al. (2009b), [6] Cecinato et al.
(2010), [7] Viana et al. (2010), [8] Viana et al. (2011).
b
Range of mean concentrations of data either from different cities or seasons.
1090
Table 7
A list on the patterns of main problem drugs in different parts of the world.
Compound
Opiates
Cannabis
Cocaine type
Amphetamines type
stimulants
Others
S. America
Europe
Africa
Asia
Oceania
9.8
35.3
31.2
12.4
2.6
30.8
54
2.2
60.1
18.9
9.1
11.9
15.7
63.6
9.6
5.2
63.3
11.5
0.4
19.1
32.6
47.3
0.4
18.2
11.3
10.4
5.9
5.7
1.5
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