This document summarizes research analyzing concentrations of pharmaceuticals, consumer chemicals, illicit drugs, pesticides, and perfluoroalkyl substances (PFCs) in sewage sludge samples collected from 15 wastewater treatment plants in 4 regions in Spain. The study found various drugs, pesticides, and PFCs present in the sludge samples, with cannabinoids and opioids being most common. Concentrations of studied contaminants were compared between regions and years. Some contaminants like PFOS and pharmaceuticals were found to accumulate in sewage sludge. The document also discusses similar analyses of sewage sludge in the US and China, finding pharmaceuticals and PFCs widely present.

1. Pharmaceuticals and organic consumer chemicals in
Sewage Sludge: Concentrations in Biosolids from
Spain vs. the USA and China.
Damià Barceló, Bozo Zonja, Alicia Navarro
and Rolf Halden

2. Analysis of illicit and abused drugs, pesticides and PFCs in sewage sludge
SEWAGE SLUDGE SAMPLES
15 WWTPs in 4 Mediterranean watersheds in Spain
Autumn 2010
Pooled grab samples at the end of the sewage sludge treatment– 1 Kg
Basin
STP
name
Sewage
type
Population
equivalent
Flow
(m3
day-1
)
Water
Treatment
Sludge
Treatment
LLOBREGAT
LL1 D, I 196167 53500 Pre + BIO + DeN ANA+BFP
LL2 D 285666 20000 Pre + BIO ANA+CF
LL3 D 80000 23000 Pre + BIO + DeN ANA+CF
EBRO
E1 D 776190 86141 Pre + BIO + DeN ANA+CF
E2 D 466560 51387 Pre + BIO + DeN ANA+CF
E3 D 46237 18573 Pre + BIO ANA+CF
E4 D 1200000 259200 Pre + BIO + DeN GRAV+CF
E5 D 186000 59706 Pre + BIO + DeN ANA+CF
E6 D 46847 6670 Pre + BIO ANA+CF
JUCAR
J1 D 80000 15000 Pre + BIO ANA+CF
J2 D 232656 33584 T ANA+CF
GUADALQUIVIR
G1 D 522000 108000 Pre + BIO ANA+CF
G2 D 30480 - Pre + BIO ANA+CF
G3 D 30000 90000 Pre + BIO ANA+CF
G4 D 1487500 135000 Pre + BIO + DeN ANA+CF
G5 D 555000 90000 T ANA+CF
GUADALQUIVIR
JUCAR
EBRO
D= domestic wastewater
I= industrial wastewater
Pre – Pretreatment: screening, sand and fat-free
BIO – Biological treatment: aeration, flocculation
and settling
DeN – denitrification;
T=Tertiary treatment: microfiltration, osmosis,
disinfection;
ANA – Anaerobic digestion
CF – centrifuge thickening and dewatering
BFP – belt filter press thickening and dewatering
GRAV – gravity thickening and dewatering

3. Analysis of illicit and abused drugs in sewage sludge
Mastroianni et al. J. Chromatogr. A (2013) 1322: 29-37.
• Total amounts of target abused and illicit drugs and metabolites= 138-1560 ng/g d.w.
CONCENTRATIONS FOUND IN SEWAGE SLUDGE SAMPLES
LL1 LL2 LL3 E1 E2 E3 E4 E5 E6 G1 G2 G3 G4 J1 J2
0
200
400
600
800
1200
1600
2000
ng/gd.w.
Cannabinoids Benzodiazepines Opioids
Amphetamine-like compounds Cocainics

4. Analysis of illicit and abused drugs in sewage sludge
HER, 6ACM, LSD and OH-LSD were
not detected
The most ubiquitous compounds
were METH, EDDP and THC (Log
Kow>3) (100%), followed by COC,
EPH and CBD (≥ 80%)
The most abundant compounds
were the cannabinoids (median
concentrations ranged from 78.4
ng/g d.w. (OH-THC) to 168 ng/g d.w.
(CBD)), followed by EDDP (45.6
ng/g d.w.) and METH (15.9 ng/g
d.w).
The remaining compounds
presented median concentrations
lower than 6.6 ng/g d.w.
Mastroianni et al. J. Chromatogr. A (2013) 1322: 29-37.
C
O
C
BE
C
E
EPH
AM
M
AM
D
M
A
M
O
RM
ETHED
D
P
ALP
D
IA
TH
C
C
BD
C
BNO
H
-TH
C
0
20
40
60
80
100
%
C
O
C
BE
C
E
EPH
AM
M
AM
D
M
A
M
O
RM
ETHED
D
P
ALP
D
IA
TH
C
C
BD
C
BNO
H
-TH
C
0.1
1
10
100
1000
ng/gd.w.
Median and concentration range
of target analytes in sludge samples (n=15)
Frequency of detection
of target analytes in sludge samples (n=15)
Occurrence of target analytes in sludge samples

5. 0
10
20
30
40
50
60
70
80
90
100
Averageconcentrations(ng/gd.w.)
2010 2011334
0
5
10
15
20
25
30
Averageconcentration(ng/gd.w.)
2010 2011GUADALQUIVIR
0
10
20
30
40
50
60
70
80
90
100
Averageconcentration(ng/gd.w.)
2010 2011
0
50
100
150
200
250
300
Averageconcentration(ng/gd.w.)
2010 2011
425 1235
EBRO
LLOBREGATJÚCAR
Analysis of pesticides in sewage sludge
CONCENTRATIONS FOUND IN SEWAGE SLUDGE SAMPLES

6. 0
5
10
15
20
25
30
i,p-PFNA
L-PFBS
L-PFDS
L-PFHpS
L-PFHxS
L-PFOS
PFODA
PFOSA
i,p-PFNS
PFBA
PFDA
PFDoA
PFHpA
PFHxA
PFHxDA
PFNA
PFOA
PFPeA
PFTeDA
PFTrDA
PFUdA
57 442
0
5
10
15
20
25
30
Guadalquivir
0
5
10
15
20
25
30
Júcar
175 81 94
0
5
10
15
20
25
30
Ebro
Llobregat
1491790
Analysis of PFCs in sewage sludge
CONCENTRATIONS FOUND IN SEWAGE SLUDGE SAMPLES

7. 0-25%
50-75%
25-50%
i,p-PFNA, i,p-PFNS, L-PFDS, PFDoA, PFHxA,
PFHxDA, PFODA, PFOSA, PFTeDA, PFTrDA
L-PFBS, L-PFHpS,
L-PFHxS, PFDA,
PFUdA
L-PFOS, PFHpA, PFNA, PFOA,
PFPeA
PFBA
Introduction•Experimental•Resultsanddiscussion•Conclusions
5%
24%
24%
48%
Analysis of PFCs in sewage sludge
OCURRENCE FREQUNCY IN THE 15 STPs

8. • >200 WWTPs
• Representative of 16,000+
plants
• Unbiased national
estimates
• >10% of U.S. population
• >32M people
• Largest, most studied archive in
the U.S.
• Anonymity through size
• E.g.: ~200,000 kg/yr of
antimicrobials to US soils
Venkatesan & Halden, 2014. Environ. Sci. Pollut. Res. 22 (3), 1577-1586.
Halden, 2014. Environ. Sci. Technol. 2014, 48, 3603−3611
National Sewage Sludge Repository at ASU (NSSR)

9. • 38 out of 72 detected
• 0.002 to 48 mg/kg dw
• TCC & TCS most abundant
• 36 ± 8 & 12.6 ± 3.8 mg/kg dw
McClellan & Halden, 2010. Water Res, 44(2), 658-668.
• ∑PPCPs load in biosolids
• 210 – 250 metric t
• 2001 vs 2006/7
• =>Limited fluctuation over years
Pharmaceuticals in NSSS collected in 2001

10. 10
• A globally shared resource at
ASU
• Environmental samples
• Wastewater, sediments,
sludge, surface water,
plants, dust etc.
• Human samples
• Urine, blood, serum etc.
Venkatesan & Halden, 2014. Environ. Sci. Pollut. Res. 22 (3), 1577-1586.
ASU Human Health Observatory (HHO)

11. • 123 chemicals
• 55 potentially
bioaccumulative
chemicals
• 93 % halogenated
• 8 priority chemicals
• 3 BFRs
• 3 Surfactants
• 2 Antimicrobials
11
(12) (100) (11)
Venkatesan & Halden, 2014. Sci. Rep. 4, 3731.
Using Sewage Sludge Analysis as a Diagnostic Tool Informing Chemical
Regulation

12. 14.1 y
14.5
y

13. 13Ag > Cu > Au > P > Fe > Pd > Mn > Zn > Ir > Al > Cd > Ti...
City of 1M people:
metals & P in sludge
=> $13M/y
ES&T 2015, 49:9479-9488
Where is the Value in Sludge?

14. US EPA
NIEHS
CDC
Dr. Arjun Venkatesan
Dr. Kristin McClellan
Erin Driver
AND MANY OTHERS
NIEHS R01ES015445; R01ES020889
ESTCP 200914; 201122
Virginia G. Piper Charitable Trust: LTR 05/01/12
Johns Hopkins Center for a Livable Future
14
Thanks to:
IDAEA-CSIC team