The removing of selected pharmaceuticals on WWTP in the Czech Republic
In this article, the results of three years monitoring of selected pharmaceuticals (diclofenac, ibuprofen, carbamazepine, salicylic acid, clofibric acid) in the wastewaters of the Czech Republic are presented. The monitoring was performed on selected Wastewater Treatment Plants (WWTP) with various t...
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Інститут колоїдної хімії та хімії води ім. А.В. Думанського НАН України
2016
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Digital Library of Periodicals of National Academy of Sciences of Ukraine| id |
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irk-123456789-1607762019-11-20T01:25:49Z The removing of selected pharmaceuticals on WWTP in the Czech Republic Wanner, F. Vana, M. Matousova, L. Fuksa, J.K. Pospichalova, D. Технология водоподготовки и деминерализация вод In this article, the results of three years monitoring of selected pharmaceuticals (diclofenac, ibuprofen, carbamazepine, salicylic acid, clofibric acid) in the wastewaters of the Czech Republic are presented. The monitoring was performed on selected Wastewater Treatment Plants (WWTP) with various treatment technology and designed capacity. The concentrations and treatment efficiency of these substances were observed in various profiles of each WWTP, including influent, mechanical pretreatment, biological treatment, effluent. The main processes of removing selected pharmaceuticals during wastewater treatment are discussed. These results are used for design wastewater treatment technology with improved treatment efficiency of these substances. 2016 Article The removing of selected pharmaceuticals on WWTP in the Czech Republic / F. Wanner, M. Vana, L. Matousova, J.K. Fuksa, D. Pospichalova // Химия и технология воды. — 2016. — Т. 38, № 2. — С. 200-209. — Бібліогр.: 21 назв. — англ. 0204-3556 http://dspace.nbuv.gov.ua/handle/123456789/160776 en Химия и технология воды Інститут колоїдної хімії та хімії води ім. А.В. Думанського НАН України |
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Технология водоподготовки и деминерализация вод Технология водоподготовки и деминерализация вод |
| spellingShingle |
Технология водоподготовки и деминерализация вод Технология водоподготовки и деминерализация вод Wanner, F. Vana, M. Matousova, L. Fuksa, J.K. Pospichalova, D. The removing of selected pharmaceuticals on WWTP in the Czech Republic Химия и технология воды |
| description |
In this article, the results of three years monitoring of selected pharmaceuticals (diclofenac, ibuprofen, carbamazepine, salicylic acid, clofibric acid) in the wastewaters of the Czech Republic are presented. The monitoring was performed on selected Wastewater Treatment Plants (WWTP) with various treatment technology and designed capacity. The concentrations and treatment efficiency of these substances were observed in various profiles of each WWTP, including influent, mechanical pretreatment, biological treatment, effluent. The main processes of removing selected pharmaceuticals during wastewater treatment are discussed. These results are used for design wastewater treatment technology with improved treatment efficiency of these substances. |
| format |
Article |
| author |
Wanner, F. Vana, M. Matousova, L. Fuksa, J.K. Pospichalova, D. |
| author_facet |
Wanner, F. Vana, M. Matousova, L. Fuksa, J.K. Pospichalova, D. |
| author_sort |
Wanner, F. |
| title |
The removing of selected pharmaceuticals on WWTP in the Czech Republic |
| title_short |
The removing of selected pharmaceuticals on WWTP in the Czech Republic |
| title_full |
The removing of selected pharmaceuticals on WWTP in the Czech Republic |
| title_fullStr |
The removing of selected pharmaceuticals on WWTP in the Czech Republic |
| title_full_unstemmed |
The removing of selected pharmaceuticals on WWTP in the Czech Republic |
| title_sort |
removing of selected pharmaceuticals on wwtp in the czech republic |
| publisher |
Інститут колоїдної хімії та хімії води ім. А.В. Думанського НАН України |
| publishDate |
2016 |
| topic_facet |
Технология водоподготовки и деминерализация вод |
| url |
http://dspace.nbuv.gov.ua/handle/123456789/160776 |
| citation_txt |
The removing of selected pharmaceuticals on WWTP in the Czech Republic / F. Wanner, M. Vana, L. Matousova, J.K. Fuksa, D. Pospichalova // Химия и технология воды. — 2016. — Т. 38, № 2. — С. 200-209. — Бібліогр.: 21 назв. — англ. |
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Химия и технология воды |
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| fulltext |
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2200
© F. Wanner, M. Vana, L. Matousova, J.K.Fuksa, D. Pospichalova, 2016
Технология водоподготовки и деминерализация вод
F. Wanner, M. Vana, L. Matousova, J.K. Fuksa, D. Pospichalova
The ReMoVing oF SeLecTeD PhaRMaceuTicaLS
on WWTP in The czech RePubLic
T.G.Masaryk Water Research Institution, Public Research Institute,
Podbabska Prague, Czech Republic
filip_wanner@vuv.cz
In this article, the results of three years monitoring of selected pharmaceuticals
(diclofenac, ibuprofen, carbamazepine, salicylic acid, clofibric acid) in
the wastewaters of the Czech Republic are presented. The monitoring was
performed on selected Wastewater Treatment Plants (WWTP) with various
treatment technology and designed capacity. The concentrations and
treatment efficiency of these substances were observed in various profiles
of each WWTP, including influent, mechanical pretreatment, biological
treatment, effluent. The main processes of removing selected pharmaceuticals
during wastewater treatment are discussed. These results are used for design
wastewater treatment technology with improved treatment efficiency of these
substances.
Keywords: pharmaceuticals, wastewater, wastewater treatment, treatment efficiency.
introduction
The relative importance of common types of pollutions in wastewaters
such as easily biodegradable organic carbon, nitrogen or phosphorus is slightly
decreasing. This situation is caused by reconstruction and intensification of
many Wastewater Treatment Plants (WWTP), which could provide better and
more efficient removing of these substances. Therefore the presence of specific
pollutants in wastewaters is now in attention [1]. These substances can negatively
influence not only water ecosystems, but in case of contaminating drinking
water sources [2], even the human health. Part of these specific pollutants is
substances commonly described as PPCP (pharmaceuticals and personal care
products) [3]. Pharmaceuticals and their metabolites leave the human body
in wastewaters and only some of frequent ones are successfully degraded by
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2 201
microbial communities. The concentrations of many other substances are
practically the same on the effluent as in the effluent to the WWTP. We can
also predicate that consumption of pharmaceuticals will be rising. New, these
days unknown substances will also occur in the future. For that reasons, the
successful removing of these substances from wastewaters seems to be very
important these days. Therefore a research project focused on monitoring of
these substances in wastewaters of the Czech Republic was launched. The main
goals of this project are to describe the concentrations of selected substances in
the wastewaters and the treatment efficiency on classic mechanical biological
WWTP. On the basis of these findings the main issue is to describe and verify
the most suitable technologies on WWTP for removing these substances.
This article summarizes the results of monitoring selected pharmaceuticals
on four WWTP in the Czech Republic. The treatment efficiency of these
substances is described and main treatment processes are discussed. These
observed results are discussed with findings published by other authors. The
possible technologies for improving of treatment efficiency of these substances
are mentioned.
experimental
These days a lot of pharmaceuticals occur in the water environment.
Therefore five main representatives were selected for detailed monitoring.
These substances were chosen on the basis of previous research projects about
pharmaceuticals consumption (diclofenac, ibuprofen, carbamazepine, salicylic
acid, clofibric acid) in the Czech Republic [4]. These substances represent most
frequent drugs used in the Czech Republic.
Four WWTP with various treatment technology and designed capacity were
chosen for monitoring of selected substances. The list of WWTP is described in
the Table 1. These WWTP represents typical wastewater treatment technologies
used in the Czech Republic.
The codes A to D were assigned for better orientation in the results. The
abbreviation PE means population equivalent, which is commonly used as the
indicator of the WWTP size. One PE means 60g BOD per day in the influent.
During the years 2010 – 2012, seventeen series of samples were collected
from selected WWTP. Two series were done on WWTP A and five on WWTP
B, C and D. Each series of samples included profiles as influent, mechanical
pretreatment, biological treatment (denitrification, and nitrification) and
effluent. The samples were collected as a spot sample. The profiles denitrification
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2202
and nitrification were sampled as a wastewater and activated sludge mixture,
where the activated sludge was settled down.
Table 1. The list of the observed WWTP
WWTP Range of PE Technological scheme
A over 80 000
Mechanical-biological WWTP with biological
nitrogen and phosphorus removal, anaerobic sludge
stabilization.
B 10 000 – 50 000
Mechanical-biological WWTP with bio-filters,
chemical precipitation aerobic sludge stabilization.
C 50 000 – 80 000
Mechanical-biological WWTP with biological
nitrogen and phosphorus removal, anaerobic sludge
stabilization
D 10 000 – 50 000
Mechanical-biological WWTP (carrousel type)
with biological nitrogen removal, aerobic sludge
stabilization.
Samples for determination of pharmaceuticals were filtered through
cellulose membrane filters (porosity 0,45 μm) and after addition of mixture of
internal standards 5 ml was preconcentrated by on-line SPE on Hypersil Gold
20x2,1 columns. For the entire determination method of LC/MS was used on
liquid chromatograph Agilent 1200 RR equipped by binary and isocratic pumps,
degasser, termostated autosampler, termostat of columns and by mass detector
Applied Biosystems 4000 Q Trap with the triplicated quadrupole. Zorbax XDB
50, 50x4,6 mm, 4 μm column was used, with the mobile phase methanol/water
acidified 0,2% of acetic acid in the gradient elution. The mass detection was done
by an electrospray in the negative (ESI) and positive (ESI+) modes. For the input
to SPE (5 ml volume) the Aspec GX-271 instrument (Gilson) was used.
Results and discussion
The results were summarized into Tables 2 – 4. The total treatment
efficiencies of selected substances on the observed WWTPs are described in the
Table 2. The best removing efficiency of observed substances was reached for
Ibuprofen. For this substance, average removal efficiency 98% was observed.
The removal ratio was also very stable; results of WWTP A, C and D are also
very stable with no variation. The only exception is WWTP B, where treatment
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2 203
efficiency even about 50% occurred. Similar results were detected for
salicylic acid. The removal efficiency was in the interval of 90 – 98%
with one exception, when during sample No. 4 at W WTP B only 55%
removal efficiency was founded. It can be assumed, that these relatively
low treatment efficiencies of ibuprofen and salicylic acid were caused by
unstable biological processes which occurred during taking sample No. 4.
In that case even low treatment efficiency of COD and especially ammonia
nitrogen were observed.
Table 2. The total treatment efficiency of observed substances
WWTP
No.
of Sample
Clofibric
Acid
Diclofenac Ibuprofen
Salicylic
Acid
Carbama-
zepine-
[%]
A
1 x 20 98 95 -26
2 x -118 99 96 0
B
1 ≥ 59 -31 94 98 -51
2 ≥ 57 -8 98 98 -18
3 ≥ 52 -46 95 92 -16
4 x -58 50 55 -367
5 x -28 64 95 -14
C
1 x -88 99 93 -44
2 2 1 96 98 -24
3 ≥ 54 -15 99 98 -10
4 x -19 99 95 9
5 x -40 98 90 -36
D
1 ≥ 66 33 99 97 27
2 ≥ 35 3 99 98 14
3 x -25 98 99 -2
4 x -19 98 95 3
5 x -78 98 96 9
According to data obtained from monitoring, diclofenac and
carbamazepine are substances which are resistant to biological treatment.
In a few cases maximal treatment efficiency 33% for diclofenac and
27% for carbamazepine was reached. More often the increase of the
concentrations for these substances during wastewater treatment
was observed. As mentioned in the introduction, these substances
leave human body in various forms (original substance, metabolites).
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2204
The diclofenac and carbamazepine are commonly known for slow deconjugation
of metabolites to the original substance. While average hydraulic retention time
on common WWTP is approximately several hours, this is the sufficient time
for that deconjugation. Because we are not able to measure the metabolites of
these substances in the influent the concentrations are "rising" at the effluent.
The concentrations of the clofibric acid in the wastewaters were very
variable. Concentrations under the detection limit in the influent and also
effluent was observed on WWTP A. On the other three WWTP various
concentrations of clofibric acid were observed. The removal ratio for this
substance was approximately 55%.
Figure shows typical progress of concentrations during wastewater
treatment. Ibuprofen and salicylic acid are removed during biological
treatment, while diclofenac and carbamazepine are not biologically degradable
and the concentrations in the eff luent are almost the same as in the influent.
0
2000
6000
10000
14000
ng l�1
ng l�1 ng l�1
ng l�1
C1C1
C1
C1
C2
C2
C2C2
C3
C3
C3
C3
C4C4
C4
C4
C5
C5
C5C5
0
5000
15000
25000
35000
0
100
300
500
700
900
0
200
600
1000
a b
c d
The progress of concentrations of observed substances during biological treatment
on WWTP C: ibuprofen (a), salicylic acid (b), diclofenac (c), carbamazepine (d).
The Table 3 summarizes the removal efficiency for mechanical pre-
treatment (profiles influent, sand catcher, primary clarifiers) and biological
treatment (profiles denitrification, nitrification and effluent). These results
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2 205
show that observed substances are eliminated almost in the biological stage
and mechanical pre-treatment does not plays any significant role.
Table 3. The treatment efficiency on mechanical and biological stage of observed
substances
WWTP
No. of
sample
Profile
Clofibric
Acid
Diclo-
fenac
Ibu-
profen
Salicyl
Acid
Carba-
mazepine
[%]
A1
Mech. Pre-reatment x 36 28 32 5
Biological treatment x -24 98 92 -33
A2
Mech. Pre-reatment x -21 6 13 11
Biological treatment x -79 99 96 -11
B1
Chem. precipitation 31 -21 46 80 -34
Biofilters ≥ 41 -8 90 89 -12
B2
Chem. precipitation 5 -35 7 28 -5
Biofilters ≥ 55 20 98 97 -13
B3
Chem. precipitation 17 -11 6 95 6
Biofilters ≥ 42 -32 94 91 -24
B4
Chem. precipitation x -18 -10 38 -41
Biofilters x -34 55 28 -232
B5
Chem. precipitation x -32 28 47 -11
Biofilters x 3 51 91 -3
C1
Mech. pre-treatment x 16 0 5 2
Biological treatment x -122 99 92 -46
C2
Mech. pre-treatment -16 0 -10 -28 -63
Biological treatment 15 2 97 99 24
C3
Mech. pre-treatment 7 -10 -1 3 -12
Biological treatment ≥ 51 -5 99 98 2
C4
Mech. pre-treatment x -15 -14 1 -2
Biological treatment x -4 99 95 11
C5
Mech. pre-treatment x 43 28 49 6
Biological treatment x -146 98 80 -45
The difference of removal efficiency of observed substances during
denitrification and nitrification processes is summarized in the Table 4. The
results of WWTP A, B and C indicate that for successful removing ibuprofen
and salicylic acid stable nitrification processes is the main factor. The WWTP
D is carrousel type technology and denitrification and nitrification is not
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2206
consequent but simultaneous. Therefore, these results are not fully comparable
with WWTP A to C.
Table 4. The treatment efficiency of denitrification and nitrification of observed
substances
WWTP
No. of
sample
Profile
Clofibric
Acid
Diclo-
fenac
Ibuprofen
Salicyl
Acid
Carba-
mazepine
[%]
A1
Denitrification x 32 49 76 -1
Nitrification x -78 96 96 -1
A2
Denitrification x -55 53 69 -8
Nitrification x 12 96 87 -5
B1
Anoxic biofilter x -3 16 84 -9
Oxic biofilter x -5 87 29 -3
B2
Anoxic biofilter 32 31 47 53 4
Oxic biofilter ≥ 34 -16 97 94 -17
B3
Anoxic biofilter x 5 49 62 -13
Oxic biofilter x -39 89 77 -10
B4
Anoxic biofilter x -5 52 71 -17
Oxic biofilter x -27 5 -148 -184
B5
Anoxic biofilter x 8 33 72 1
Oxic biofilter x -6 26 67 -4
C1
Denitrification x -122 55 92 -30
Nitrification x 9 98 -16 -6
C2
Denitrification 27 -2 63 79 10
Nitrification 7 97 99 97 99
C3
Denitrification ≥ 51 -11 65 99 -1
Nitrification x 15 99 -14 4
C4
Denitrification x 43 75 94 11
Nitrification x -87 98 23 -3
C5
Denitrification x -42 70 79 -27
Nitrification x -83 95 11 -6
D1
Denitrification x 44 99 98 25
Nitrification x 47 99 95 26
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2 207
D2
Denitrification x 16 97 92 15
Nitrification x -4 99 98 15
D3
Denitrification x 10 96 98 -2
Nitrification x -10 99 99 -4
D4
Denitrification x -13 94 96 8
Nitrification x -6 99 96 12
D5
Denitrification x -35 96 95 9
Nitrification x -27 99 95 6
The main factors of removing PPCP on WWTP. Hydraulic retention time
(HRT) and sludge retention time (SRT) are the key parameters of activation
treatment plants. Generally, activation process effect on drug elimination
increases with increasing retention time (HRT) and especially with increasing
sludge retention time (SRT) – it is explained, besides longer reaction time, by
higher diversity and adaptation of sludge microbial communities.
Removal efficiency over 90% is stated for most pharmaceutics at quite
standard SRT about 15 – 20 days, except carbamazepine, clofibric acid and
diclofenac [5 – 7] - some standard WWTP show surprisingly low elimination
of e.g. degradable ibuprofen [8]. Experimental data on the influence of SRT
do not always match with the real processes in wastewater treatment plants –
under regular operation conditions activation process efficiency could vary with
fluctuating sludge retention time during storm events [9]. Zhang et. al. [10]
summarized the data dealing with influence of SRT in activation treatment
plants on particulary problematic drugs carbamazepine and diclofenac.
Carbamazepine was resistant in extent of total SRT (100 days), diclofenac
showed maximum (50% elimination) in the segment from 20 to 50 days.
carbamazepine unlike clofibric acid and diclofenac, which concentrations after
passing WWTP decrease at least in some cases, is not degraded and increase
in its concentrations is found along WWTP [7, 11, 12]. Slower deconjugation
into determinable parent substance is the partial explanation, but already input
evaluations of carbamazepine do not match with the assumptions based on
average consumption and number of people connected to WWTP [13].
Membrane reactors are specific for their technical capabilities maintain high
SRT. That corresponds to a statistically significant increase in elimination of drugs
as compared with standard activation processes [14 – 17]. Also activation processes
with enhanced nutrient removal are more efficient in drug elimination [14, 18, 19].
Table 4. (Contd.)
ISSN 0204–3556. Химия и технология воды, 2016, т.38, №2208
Effect of mechanical pretreatment ondrug elimination is generally considered to
be insignificant, except for the gradual transformation of estrone to estradiol.
Special processes aimed at elimination of drugs in the secondary treatment of
wastewater are still working as experimental operation rather than real operation.
Salgado et al. [20] conducted experiments with disinfection of wastewater effluent
from a wastewater treatment plant by UV radiation. The system was effective
on clofibric acid and diclofenac (wastewater after passing through WWTP), it
was not effective on ibuprofen elimination. Serrano et al. [21] noted a positive
influence of dosing of powdered activated carbon for removal of carbamazepine.
On the contrary, using FeCl
3
as the coagulant for the removal of drugs has
proved ineffective. Okuda et al. [19] found positive effect of ozonation on drug
elimination, technologies such as coagulation, sedimentation and sand filtration,
chlorination and UV disinfection had any effect.
conclusions
These results gained during three years of monitoring of selected substances
comply with results published by other authors. It was confirmed that mechanical
pre-treatment do not plays any significant role in removing for all observed
substances. Ibuprofen and salicylic acid are highly biodegradable in WWTP, but
even 99% treatment efficiency significant concentrations of these substances can
be found in the WWTP effluents. The main factors of high removal efficiency are
hydraulic retention time and sludge age. The diclofenac and carbamazepine are
not removable on common mechanical biological WWTP. Therefore for sufficient
removing of these substances, new technologies as ozonation or UV radiation
must be involved as a part of tertiary treatment. Low concentrations of clofibric
acid in the influents were detected. This is not corresponding with estimated
consumption in the Czech Republic. However explanation of this situation could
be the fact that the drugs based on this substance were substituted.
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Received 07.02.2014
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