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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Full-scale plant for the elimination of
pharmaceuticals in hospital wastewater –
Comparison of advanced treatment technologies
Dr. Issa Nafo
Sven Lyko
Emschergenossenschaft (Essen, Germany)
1
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Content
• Sources and pathways of pharmaceutical residues
• Current framework regarding pharmaceuticals in waters
• EU-project PILLS: Elimination of pharmaceuticals at local sources
• Results of a full-scale investigation
Pharmaceuticals in hospital wastewater
Treatment efficiency of MBR, Ozone and Powdered activated carbon
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Emschergenossenschaft (EG) and Lippeverband (LV)
• 2 Water Associations working as a joint company since approx. 100 years
• Public corporations
• Management of the natural catchment areas of Emscher and Lippe
• Different services around the water cycle 3
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Emschergenossenschaft and Lippeverband Public corporations - Management of the catchment of the rivers Emscher and Lippe
Emscher-
genossenschaft
Lippe-
verband
Area (km2) 865 3,280
Inhabitants (mil.) 2.4 1.4
Inhabitants / km2 2,775 427
→ Operation of 60 wastewater treatment plants
→ Treatment of 1 billion m³ sewage/year (approx.) 4
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Retention and Management of Rainwater
Groundwater Management
Wastewater Disposal Flood Protection
River Management
River –Restoring and Regeneration
Restructuring of mining facilities
Managing Water- flow Residue Disposal
Emschergenossenschaft and Lippeverband Services around the water cycle
220 km Dikes
49 Flood retention basins
269 Stormwater treatment devices
1.149 km Sewer
289 Pumping stations
752 km Watercourse
806 km² Polder area
3.400 Groundwater monitoring wells
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Human drugs
Sources and pathways
6
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Veterinary drugs
Sources and pathways
7
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Sources and pathways
8
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Current framework (1)
There are no legal requirements for the discharge of wastewater contaminated by
pharmaceuticals residues into waters
Pharmaceuticals in wastewater are not relevant for the design of wastewater treatment
plants
Clarification Primary treatment Filtration
(optional) Denitrification
Activated sludge
Nitrification
Grid
Phosphate
precipitation
(Fe, Al)
9
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
0,0
0,5
1,0
1,5
2,0
2,5
3,0
Ibuprofen Diclofenac Carbamazepine Iopamidol Iohexol Iopromid
Inflow
Outflow
Mean concentration of plant inflow
and outflow in μg/L (n = 4)
(Elimination rate in %)
(99)
(0)
(0)
(30)
(80)
(40)
7,0 4,6
Current framework (2) Conventional wastewater treatment plants are not able to eliminate all pharmaceuticals
residues efficiently
10
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Current framework (3)
There is still a lack of long-term experiences in operating advanced wastewater treatment technologies in "real life"
Membrane
filtration Oxidation processes
Adsorption on
activated
carbon
11
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
⇒ Which pharmaceuticals are relevant?
⇒ What is the contribution of healthcare institutions to the overall emission?
⇒ What are the practical and economical consequences of advanced (local)
wastewater treatment?
⇒ What steps are needed for a sustainable reduction of the overall emissions?
The EU project PILLS Pharmaceuticals Input and Elimination at Local Sources
12
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
PILLS Partnership
Limoges
Zürich
Luxemboug
Essen
Zwolle
Glasgow
2 Water associations
2 Universities
And 2 research institutes
Budget: 8,0 Million Euro
Project Duration: 2008 – 2012
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
LE
AD
PA
RT
NE
R
Pro
ject &
fina
ncia
l ma
na
ge
me
nt
WP 4
Communication
PROJECT STEERING GROUP Representatives of all partners
Responsible
partner: DE
Responsibility & quality control of joint outcomes and products
WP 3
Assessment
WP 2
Technology
WP 1
Analysis
Responsible
partner: LU
Responsible
partner: NL
Responsible
partner: UK
Scientific
Board
PILLS Management Structure
14
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Membrane
filtration Oxidation processes
Adsorption on
activated carbon
Microfiltration Ozonation Powdered activated carbon
Ultrafiltration Advanced oxidation processes
(TiO2/UV, H2O2/O3, UV)
Granulated activated
carbon
Reverse osmosis
Work Package Technology Development & Investigation of wastewater treatment technologies at local sources
15
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Investigated pilot plants in the PILLS project S
ma
ll-s
ca
le p
lan
ts
Fu
ll-s
ca
le p
lan
ts
1.2
m³/
day
1-
3 m
³/d
ay
200
m³/
day
10
m³/
ho
ur
16
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Building of the Pilot plant at Marienhospital Gelsenkirchen (Germany)
17
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Membran-Bioreactor
(MBR)
Powdered activated
carbon reactor (PAC)
Exhaust air
treatment
Ozone reactor
Treatment technologies in the pilot plant
18
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Pilot plant design allows different operation modes of the treatment technologies
19
Fine Screen Biological Treatment Membrane
Filtration
Ozone reactor
(3 m³)
Powdered activated
carbon (PAC, 9 m³)
to Sludge
Treatment
(external)
Sand Filtration
(moving bed)
200 m³/d
250 m³
Operation modes:
1. MBR → 100% O3 → 100% PAC → river
2. MBR → 100% PAC → 100% O3 → river
3. MBR → 50% O3 and 50% PAC → river
4. MBR → 100% O3 (partly recirculated) → river
5. MBR → 50% O3 and 50% PAC (recycled to MBR)
6. MBR → 100% O3 → river
7. MBR → 100% PAC → river
8. MBR → river
9. MBR → 100% O3 → SF→ river
10.PAC addition in MBR → river
Applied Doses:
• 5 mg O3/L (0.5 g O3/g DOC)
• 20 mg PAC/L
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Scre
en
ing
Tre
atm
en
t e
ffic
ien
cy
Preliminary sampling
campaign before pilot
plant implementation:
Characterisation of the
hospital wastewater
• Sampling of hospital effluent
• 24 h flow-proportional composite samples
• 1 Week intensive screening (31. Jan - 6. Feb 2011)
• 121 substances
• 17 groups of substances (pharmaceuticals and metabolites ,
dsinfection agents, chemicals, …)
Main sampling campaign
after pilot plant
implementation:
Process analysis
• 24 h flow-proportional composite samples
• Relevant substances in13 groups of pharmaceuticals and
metabolites
• Classical wastewater parameters (TSS, COD, BOD, N, P)
• Sampling of influent and effluent of treatment processes
Conducted sampling campaigns
MBR Ozone reactor
Sand filter
OFI
AC
PAC reactor
Sand filter
OS
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Pharmaceutical loads in raw hospital wastewater Intensive sampling campaign Jan 31 – Feb 06, 2011(24h composite samples), n = 7
21
X-ray contrast media98,677%
Analgesics / Anti-Inflammatories
0,392%
Antibiotics0,322%
Enzyme inhibitor0,180%
Diuretics0,166%
Betablockers / Anti-hypertensives
0,119%Metabolites of
pharamaceuticals0,069%
Lipid Regulators0,031%
Antiepileptics0,025%
Psycho-active Drugs
0,009%
Hormones0,004%
Cytostatics0,003%
Andere1,323%
Pharmaceuticals in hospital raw wastewaterIntensive sampling campaign Jan 31 – Feb 06, 2011(24h composite samples), n = 7
total loads 3,59 kg/d
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Load distribution of analgesics and NSAIDs in the raw hospital wastewater Intensive sampling campaign Jan 31 – Feb 06, 2011(24h composite samples), n = 7
22
The load of 4 substances (ibuprofen, diclofenac, indometacin and naproxen) represents
60% of the total amount of the detected 14 NSDAIDs in the raw hospital wastewater
Carprofen 0,6%
Diclofenac 9,1%
Fenoprofen 0,0%
Flurbiprofen 0,2%
Ibuprofen 41,3%
Indometazin 8,3%
Indoprofen 1,2%
Ketoprofen 0,0%
Naproxen 1,8%
Paracetamol 30,7%
Phenanzone 1,5%
Propyphenanzone 0,1%
Tolfenamic acid 0,1%
Tramadol 5,0%
total load: 14.06 g/day
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Mean concentration of analgesics and NSAIDs in raw hospital wastewater Intensive sampling campaign Jan 31 – Feb 06, 2011(24h composite samples), n = 7
23
0
5
10
15
20
25
30
35
40
co
nce
ntr
ation
in
µg
/l
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Concentration variation of analgesics and NSAIDs in raw hospital wastewater Intensive sampling campaign Jan 31 – Feb 06, 2011(24h composite samples), n = 7
SunSatFriThuWedTueMon SunSatFriThuWedTueMon
24
0
1
2
3
4
5
6
7
8
9conc.µg/l Diclofenac
0
5
10
15
20
25
30
35
40conc.µg/l Ibuprofen
0
2
4
6
8
10
12conc.µg/l Indometacin
0
1
1
2
2
3
3
4conc.µg/l Naproxen
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Evaluation of pilot plant treatment efficiency
Focus in this presentation:
• analgesics and non-steroidal anti-inflammatory drugs (NSAIDs)
• Operation mode MBR → 50% O3 and 50% PAC → river
MBR Ozone reactor
Sand filter
OFI
AC
PAC reactor
50% of MBR permeate
treated by ozonation
50% of MBR permeate
treated by PAC addition
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Process performance of the MBR Stable operation since start-up in April 2011
26
From April to September 2011 a total of 16,000 m³ hospital wastewater were treated. The
average flow rate of 100 m³/d is below the maximum design value of 200 m³/d.
Process Parameter Unit Median ± Standard
deviation
Flow rate hospital wastewater m³/d 90.0 ± 21.4
MLSS concentration kg/m³ 9.5 ± 0.9
T in bioreactor °C 26.8 ± 1.0
pH in bioreactor - 6.8 ± 0.2
O2 in bioreactor mg/L 0.8 ± 0.5
Sludge production kg/m³ 0.095
Organic sludge load gCOD/gTSS/d 0.0396
Permeability L/m²/h/bar 171 ± 46
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Effluent quality of the pilot plant MBR had a good biological removal efficiency regarding classical parameters
27
Biological transformation in the MBR is the major treatment process to achieve the current
required effluent quality for the rejection of plant effluent into surface water body
Parameter Unit Required
effluent quality Influent Effluent Elimination
COD mg/L 110 709 ± 280 31.0 ± 6.0 96 %
Total N mg/L - 64 ± 11 3.3 ± 5.8 95 %
Total P mg/L - 8.3 ± 1.3 2.0 ± 5.6 76 %
TSS mg/L - 97 ± 33 < 10 > 90 %
BOD mg/L - 325 ± 112 < 3 > 99 %
n = 7
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Elimination of the selected NSDAIs MBR reduced the load of the selected NSAIDs considerably
28
0,00
1,00
2,00
3,00
4,00
5,00
6,00
MBR influent MBR effluent MBR + 5mg O3/L MBR + 20 mgPAC/L + SF
load (g/day)
Naproxen
Indometacin
Diclofenac
Ibuprofen
96% removed
n = 7
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Elimination of the selected NSDAIs Pilot plant reduced the concentration of the selected NSAIDs considerably
NSAID Elimination MBR Elimination
Ozonation Elimination PAC-SF
Ibuprofen 99.9% 62.% 52%
Diclofenac 25.9% 95.% 59%
Indometacin 87.5%* -* -*
Naproxen 91.9% 53.8%* 53.8%*
29
n = 7
* Concentration below detection limit (calculation with detection limit)
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
NSAIDs in effluent of the advanced treatment
30
0,05 0,02 0,02
2,00
0,10
0,82
<LOQ <LOQ <LOQ
0,026 <LOQ <LOQ
0,00
0,50
1,00
1,50
2,00
2,50
MBR effluent MBR + 5mg O3/L MBR + 20 mgPAC/L + SF
conc. (ug/L)
Ibuprofen
Diclofenac
Indometacin
Naproxen
n = 7
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Some options to reduce pharmaceuticals in waters
31
Politics and
Authorities Labeling of existing "water relevant" drugs
Changes in the legal framework (human and veterinary drugs)
Development and optimization of recycling schemes
Industry Development of degradable "water-friendly" drugs
Adjustment of the dosage amounts to the needs of the human body
Medical
System
Change in prescribing practice
Appropriate counseling in pharmacies
Information for a changed use of medicines
The minimization of the emissions is a common task!
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Communication Encourage stakeholders for actions
32
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Key messages
• Local sources may be hot spots for pharmaceuticals emission in the
sewer system
• MBR, Ozonation and PAC addition can reduce pharmaceutical loads
at local sources considerably
• Advanced wastewater treatment at local sources can be one measure
among others for the reduction of pharmaceuticals emissions to
waters
• Integrated actions are required in all steps of the life cycle of
pharmaceuticals to reduce the emissions to waters
• Policy framework is needed which ensure a sustainable approach:
Produce environment-friendly substances
Use environment-friendly substances or use less substances
Reduce losses & emissions
33
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16th International EWA Symposium, IFAT 2012, Munich, 8th-9th May
Thank you for your attention!
34
Acknowledgment: • Investments of the full-scale plants and investigations co-financed in the
framework of the EU INTERREG IV B project PILLS
• Staff of the Marienhospital Gelsenkirchen
• Operation staff of the pilot plant Emschergenossenschaft
• Joint laboratory of Ruhrverband/Emschergenossenschaft/Lippeverband
(chemical analyses)
• IUTA (chemical analyses)
• Tuttahs & Meyer (engineering consultancies)
www.pills-project.eu