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TREATMENT OF SLUDGE
AND RECLAIMED
WASTEWATER POLLUTED
WITH EMERGING
CONTAMINANTS
Guillem Llorens Blanch
BioremUAB Seminar
April, 24th 2015
Contents
1. Introduction
2. Objectives
3. Methodology
4. Results
I. Degradation of
hydrochlorothiazide in
liquid systems
II. Optimization of
biopile systems
III. Treatment of MBR
sludge
IV. Treatment of WWTP’s
dried sludge
V. Fungi as low-cost
sorbent for Heavy
Metals
VI. Post-treatment of
WWTP’s water
IntroductionI. WWTP Sludge
II. Soil-Aquifer Treatment
i. Groundwater
recharge
ii. Low-cost sorbent
III. Emerging Polllutants
IV. Bioremediation
i. Micoremediation
ii. White rot fungi
iii. Trametes versicolor
I. WWTP Sludge
 A mix of water and solids.
 The main waste produced in WWTPs
 High water content
 High content of OM, N, P, K, Ca, and Mg
 Can contain heavy metals, pathogens, and
organic pollutants
 WWTP sludge activities is becoming an
interesting product in agricultural and forestry
activities.
II. Soil-Aquifer Treatment
 Groundwater is an important natural
resource that can be use to supply water
for municipal, agricultural, and industrial
purposes.
 Artificial recharge methods are faster than
natural systems:
 Direct aquifer injection systems: to put
water directly into the underground water
basins.
 Surface spreading recharge systems: to
replenish aquifers by infiltration
II. Soil-Aquifer Treatment
 With surface spreading, reclaimed
wastewater is intermittently introduced into
spreading basins
 Water will percolate across the ground and
throughout the aquifer
 Water quality improvement thanks to
physical, chemical, and biological natural
processes
 This is the so-called Soil-Aquifer Treatment
(SAT)
II. Soil-Aquifer Treatment
Miotlinski et al. 2010
II. Soil-Aquifer Treatment
 Adsorption is the mass transfer of a
substance from a liquid to a solid’s surface.
 Activated carbon is the universal
adsorbent, but it is expensive.
 Local materials available in large quantities
(natural products or waste) can be utilized
as inexpensive sorbents.
 A material is a low-cost sorbent when
requires little processing, and is abundant.
III. Emerging Pollutants
 Emerging pollutants are a group of man-made
and natural chemicals.
 Not yet regulated; not deeply studied; can be
a danger for the environment, and human and
animal health.
 Detected in salt-water, freshwater and
wastewater
 Concentration: few ng·L-1 to thousands g·L-1
 Formed by: pharmaceuticals products,
personal care products (PCPs), endocrine-
disrupting chemicals (EDCs), perfluorinated
compounds (PFCs), and transformation
products (TPs)
IV. Bioremediation
 The use of microorganisms to remove chemical
compounds; treatments more sustainable and cheap
than traditional physical-chemical treatments.
 Micoremediation: The use of fungi in bioremediation
processes. Fungi are eukaryotic organisms constituted by
especial structures called mycelia.
 White Rot Fungi (WRF): basidiomycets are able to degrade
lignin. These ligninolytic fungi can degrade lignin thanks to
its unspecific extracellular enzyme system.
 Trametes versicolor (T.v.): a WRF widely studied in the
treatment of polluted wastewaters, soils and sludge with:
textile dyes, PPCPs, UV-filters, and PAH
Objectives Study of fungal
degradation of
emerging pollutants
in sludge
 Improvement of a
SAT by removing
emerging pollutants
with low-cost
sorbents
 Environmental and
economic study of
the processes by
LCA and RA
Methodology
I. Sludge
Treatment
II. Reclaimed
Wastewater
Treatment
I. Sludge
Treatment
Sludge...
 Active
 Anaerobic
 WWTP
Thermic
dried
 MBR
Treatment in...
Bioslurry
Biopiles
Spiked
Real
Concentrations
Pollutants
 Lacasse
 ND24
 Glucose
 Degradation
II. Reclaimed
Wastewater Treatment
Wastewater...
WWTP with
mixed urban
and industrial
influents
Adsorption…
Biochar
NUA
Real
Concentrations
Pollutants
Soil-Aquifer
Treatment
(SAT)
ResultsI. Degradation of
hydrochlorothiazide
in liquid systems
II. Optimization of
biopile systems
III. Treatment of MBR
sludge
IV. Treatment of WWTP’s
dried sludge
V. Fungi as low-cost
adsorbent for Heavy
Metals
VI. Post-treatment of
WWTP’s water
I. Degradation of hydrochlorothiazide
(HZT) in liquid systems
 HZT degradation experiments in spiked
media cultures at optimal growth
conditions for T.v..
 Analyses of glucose consumption,
laccase activity, and HZT degradation.
I. Degradation of hydrochlorothiazide
(HZT) in liquid systems
I. Degradation of hydrochlorothiazide
(HZT) in liquid systems
 45% of the measured HZT is eliminated from
the media.
 10% of the compound was adsorbed on
the fungal biomass.
 35% degraded.
II. Optimization of biopile systems
 Data from prior experiments
 Soil colonization by Trametes versicolor grown
on lignocellulosic materials: Substrate
selection and naproxen degradation. E.
Borràs, G. Llorens-Blanch, C. E. Rodríguez-
Rodríguez, M. Sarrà, G. Caminal. International
Biodeterioration & Biodegradation 65 (2011)
846-852.
 Practice report Jordi & C. E. Rodríguez-
Rodríguez.
 Experiment with oil pruning and sludge
II. Optimization of biopile systems
Grou
p
Substrate
(g)
Sludge
(g)
Moisture
(%)
1 3.0 6.0 40
2 2.5 6.5 54
3 2.0 7.0 60
4 1.3 7.7 54
5 0.8 8.2 40
6 1.3 7.7 26
7 2.0 7.0 20
8 2.5 6.5 26
9 2.0 6.0 40
III. Treatment of MBR sludge
 Designed to test the ability of T.v. to grow
on liquid MBR sludge, and its degradation
capacity.
 HZT as a target compound.
 3 different culture media: complete media,
glucose media and no-nutrient media.
 Sterile and non-sterile conditions.
III. Treatment of MBR sludge
Sterile Conditions
 Effect of media composition on the
degradation of spiked HZT in sterile bioslurry
system.
III. Treatment of MBR sludge
Complete Media Glucose Media
No-Nutrient Media
Sterile Conditions
III. Treatment of MBR sludge
Complete Media Glucose Media
No-Nutrient Media
Sterile Conditions
III. Treatment of MBR sludge
Non-sterile Conditions
 Non-sterile conditions were tested for the
no-nutrient cultures in order to determine if
T.v. could degrade spiked HZT in
competition with the autochthonous sludge
microorganisms.
III. Treatment of MBR sludge
 Laccase activity was
negligible.
 HZT degradation
higher than in
previous experiments.
 HTZ degradation in
inoculated cultures
faster than in raw
sludge control.
Non-sterile Conditions
III. Treatment of MBR sludge
Pharmaceuticals degradation in non-spiked
bioslurry
 Determine the efficiency of T.v. to eliminate
PPCPs at real concentrations in bioslurry.
 3 groups: sterilized sludge with T.v., non-
sterilized sludge with T.v., and non-sterilized
sludge without T.v.
III. Treatment of MBR sludge
Non-spiked Bioslurry
 Removal:
 Inoculated: 66%
 Non-inoculated: 54%
 In all cases partial or
total drug removal was
observed.
 5 pharmaceuticals
showed negative
elimination rates.
III. Treatment of MBR sludge
Non-spiked Bioslurry
III. Treatment of MBR sludge
 Liquid MBR sludge can be treated with
T.v. at the Erlenmeyer scale.
 T.v. grown under non-sterile conditions
without any extra nutrients.
 The time to eliminate the drug was
reduced with T.v.
Non-spiked Bioslurry
III. Treatment of MBR sludge
Biopiles system
 Determine the efficiency of T.v. to
eliminate HZT in a biopiles system.
 Waste as substrate: Olive Pruning
III. Treatment of MBR sludge
Biopiles
III. Treatment of MBR sludge
 Removal: 86%
 Is not feasible to treat MBR sludge in
biopiles due to its high water content.
Biopiles
IV. Treatment of WWTP’s dried
sludge
Biopiles in trays
 Determine the efficiency of T.v. to
eliminate PPCPs in larger biopiles (380g).
 Sludge from WWTP El Prat de Llobregat
 Waste as substrate: Pine Bark
IV. Treatment of WWTP’s dried
sludge
Biopiles in trays
IV. Treatment of WWTP’s dried
sludge
Biopiles in trays
IV. Treatment of WWTP’s dried
sludge
SAILAB Results
Compound
Initial
sludge
Biopiles
before
reinoculation
Reinoculated
biopiles at
final time
Non-
einoculated
biopiles at
final time
Sludge +
Substrate at
final time
Sludge at
final time
Bisoprolol 0.5 0 0 0 0 0
Enroflaxicin 1.4 0 0 0 0 0
Progesterone 5.3 0 0 0 0 0
Methadone 5.6 0 0 0 0 0
Diclofenac 1.1 0 0 0 0 0
Gemfibrozil 0.43 0 0 0 0 0.4
Indomethaci
n
0.4 0 0 0 0 0
ICRA Results
 21 compounds
detected
 High disparity
between triplicates
and times
Biopiles in trays
IV. Treatment of WWTP’s dried
sludge
Biopiles in trays
 The low repeatability is due to sampling
technique.
 Difficult to take unitary and representative
samples in large biopiles.
IV. Treatment of WWTP’s dried
sludge
Biopiles in bottles
 Determine the efficiency of T.v. to
eliminate PPCPs in small (20g) but more
representative biopiles.
 Sludge from WWTP El Prat de Llobregat
 Waste as substrate: Pine Bark
IV. Treatment of WWTP’s dried
sludge
Biopiles in bottles
V. Fungi as low-cost sorbent for
Heavy Metals
 Treatment of heavy metals with T.v..
 The first step was to reproduce a
published adsorption experiment with
another fungus.
 Impossible to reproduce the conditions of
the paper.
 Inconsistent results.
 This research line has been abandoned.
VI. Post-treatment of WWTP’s
water
 Improve the quality of reclaimed
wastewater used in SAT.
 Determine the efficiency of 2 low-cost
sorbents to eliminate emerging pollutants.
 NUA: neutralised used acid comes from
heavy mineral processing residue
 BIOCHAR: charcoal produced by the
pyrolysis of biomass (eucalyptus).
 Soil: Alice Springs SAT basin E
VI. Post-treatment of WWTP’s
water
Pilot-scale basinsPilot-scale basins
VI. Post-treatment of WWTP’s
water
Initial Screening
 Determine the capacity of the soil to adsorb
a mixture of 7 compounds without
amendments.
 24h batch sorption.
 3 soil:solution ratio(g:mL): 1:1, 1:5 and 1:50.
 Ibuprofen, carbamazepine, ofloxacin,
trimethorpim, ketoprofen, propranolol, and
sulfamethoxazole
VI. Post-treatment of WWTP’s
water
Initial Screening
VI. Post-treatment of WWTP’s
water
Ratio Experiment
 Effect of the soil:amendment ratio in the
adsorption of 3 compounds.
 2 amendments: Biochar and NUA.
 24h batch sorption.
 1 soil:solution ratio(g:mL): 1:5.
 5 amendment:soil ratio: 0.1, 0.5, 1, 2, and 5%.
 Trimethorpim, propranolol, and
sulfamethoxazole.
VI. Post-treatment of WWTP’s
water
Ratio Experiment
VI. Post-treatment of WWTP’s
water
Incubation Experiment
 Determine the sorption of a mixture of 7
compounds into a soil amended with
biochar and NUA.
 21d batch sorption experiments.
 3 soil:solution ratio(g:mL): 1:1, 1:5 and 1:50.
 1 amendment:soil ratio: 1%.
 Ibuprofen, carbamazepine, ofloxacin,
trimethorpim, ketoprofen, propranolol, and
sulfamethoxazole
VI. Post-treatment of WWTP’s
water
Incubation Experiment
Thanks!

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Treatment of sludge and reclaimed wastewater polluted with emerging contaminants

  • 1. TREATMENT OF SLUDGE AND RECLAIMED WASTEWATER POLLUTED WITH EMERGING CONTAMINANTS Guillem Llorens Blanch BioremUAB Seminar April, 24th 2015
  • 2. Contents 1. Introduction 2. Objectives 3. Methodology 4. Results I. Degradation of hydrochlorothiazide in liquid systems II. Optimization of biopile systems III. Treatment of MBR sludge IV. Treatment of WWTP’s dried sludge V. Fungi as low-cost sorbent for Heavy Metals VI. Post-treatment of WWTP’s water
  • 3. IntroductionI. WWTP Sludge II. Soil-Aquifer Treatment i. Groundwater recharge ii. Low-cost sorbent III. Emerging Polllutants IV. Bioremediation i. Micoremediation ii. White rot fungi iii. Trametes versicolor
  • 4. I. WWTP Sludge  A mix of water and solids.  The main waste produced in WWTPs  High water content  High content of OM, N, P, K, Ca, and Mg  Can contain heavy metals, pathogens, and organic pollutants  WWTP sludge activities is becoming an interesting product in agricultural and forestry activities.
  • 5. II. Soil-Aquifer Treatment  Groundwater is an important natural resource that can be use to supply water for municipal, agricultural, and industrial purposes.  Artificial recharge methods are faster than natural systems:  Direct aquifer injection systems: to put water directly into the underground water basins.  Surface spreading recharge systems: to replenish aquifers by infiltration
  • 6. II. Soil-Aquifer Treatment  With surface spreading, reclaimed wastewater is intermittently introduced into spreading basins  Water will percolate across the ground and throughout the aquifer  Water quality improvement thanks to physical, chemical, and biological natural processes  This is the so-called Soil-Aquifer Treatment (SAT)
  • 8. II. Soil-Aquifer Treatment  Adsorption is the mass transfer of a substance from a liquid to a solid’s surface.  Activated carbon is the universal adsorbent, but it is expensive.  Local materials available in large quantities (natural products or waste) can be utilized as inexpensive sorbents.  A material is a low-cost sorbent when requires little processing, and is abundant.
  • 9. III. Emerging Pollutants  Emerging pollutants are a group of man-made and natural chemicals.  Not yet regulated; not deeply studied; can be a danger for the environment, and human and animal health.  Detected in salt-water, freshwater and wastewater  Concentration: few ng·L-1 to thousands g·L-1  Formed by: pharmaceuticals products, personal care products (PCPs), endocrine- disrupting chemicals (EDCs), perfluorinated compounds (PFCs), and transformation products (TPs)
  • 10. IV. Bioremediation  The use of microorganisms to remove chemical compounds; treatments more sustainable and cheap than traditional physical-chemical treatments.  Micoremediation: The use of fungi in bioremediation processes. Fungi are eukaryotic organisms constituted by especial structures called mycelia.  White Rot Fungi (WRF): basidiomycets are able to degrade lignin. These ligninolytic fungi can degrade lignin thanks to its unspecific extracellular enzyme system.  Trametes versicolor (T.v.): a WRF widely studied in the treatment of polluted wastewaters, soils and sludge with: textile dyes, PPCPs, UV-filters, and PAH
  • 11. Objectives Study of fungal degradation of emerging pollutants in sludge  Improvement of a SAT by removing emerging pollutants with low-cost sorbents  Environmental and economic study of the processes by LCA and RA
  • 13. I. Sludge Treatment Sludge...  Active  Anaerobic  WWTP Thermic dried  MBR Treatment in... Bioslurry Biopiles Spiked Real Concentrations Pollutants  Lacasse  ND24  Glucose  Degradation
  • 14. II. Reclaimed Wastewater Treatment Wastewater... WWTP with mixed urban and industrial influents Adsorption… Biochar NUA Real Concentrations Pollutants Soil-Aquifer Treatment (SAT)
  • 15. ResultsI. Degradation of hydrochlorothiazide in liquid systems II. Optimization of biopile systems III. Treatment of MBR sludge IV. Treatment of WWTP’s dried sludge V. Fungi as low-cost adsorbent for Heavy Metals VI. Post-treatment of WWTP’s water
  • 16. I. Degradation of hydrochlorothiazide (HZT) in liquid systems  HZT degradation experiments in spiked media cultures at optimal growth conditions for T.v..  Analyses of glucose consumption, laccase activity, and HZT degradation.
  • 17. I. Degradation of hydrochlorothiazide (HZT) in liquid systems
  • 18. I. Degradation of hydrochlorothiazide (HZT) in liquid systems  45% of the measured HZT is eliminated from the media.  10% of the compound was adsorbed on the fungal biomass.  35% degraded.
  • 19. II. Optimization of biopile systems  Data from prior experiments  Soil colonization by Trametes versicolor grown on lignocellulosic materials: Substrate selection and naproxen degradation. E. Borràs, G. Llorens-Blanch, C. E. Rodríguez- Rodríguez, M. Sarrà, G. Caminal. International Biodeterioration & Biodegradation 65 (2011) 846-852.  Practice report Jordi & C. E. Rodríguez- Rodríguez.  Experiment with oil pruning and sludge
  • 20. II. Optimization of biopile systems Grou p Substrate (g) Sludge (g) Moisture (%) 1 3.0 6.0 40 2 2.5 6.5 54 3 2.0 7.0 60 4 1.3 7.7 54 5 0.8 8.2 40 6 1.3 7.7 26 7 2.0 7.0 20 8 2.5 6.5 26 9 2.0 6.0 40
  • 21. III. Treatment of MBR sludge  Designed to test the ability of T.v. to grow on liquid MBR sludge, and its degradation capacity.  HZT as a target compound.  3 different culture media: complete media, glucose media and no-nutrient media.  Sterile and non-sterile conditions.
  • 22. III. Treatment of MBR sludge Sterile Conditions  Effect of media composition on the degradation of spiked HZT in sterile bioslurry system.
  • 23. III. Treatment of MBR sludge Complete Media Glucose Media No-Nutrient Media Sterile Conditions
  • 24. III. Treatment of MBR sludge Complete Media Glucose Media No-Nutrient Media Sterile Conditions
  • 25. III. Treatment of MBR sludge Non-sterile Conditions  Non-sterile conditions were tested for the no-nutrient cultures in order to determine if T.v. could degrade spiked HZT in competition with the autochthonous sludge microorganisms.
  • 26. III. Treatment of MBR sludge  Laccase activity was negligible.  HZT degradation higher than in previous experiments.  HTZ degradation in inoculated cultures faster than in raw sludge control. Non-sterile Conditions
  • 27. III. Treatment of MBR sludge Pharmaceuticals degradation in non-spiked bioslurry  Determine the efficiency of T.v. to eliminate PPCPs at real concentrations in bioslurry.  3 groups: sterilized sludge with T.v., non- sterilized sludge with T.v., and non-sterilized sludge without T.v.
  • 28. III. Treatment of MBR sludge Non-spiked Bioslurry  Removal:  Inoculated: 66%  Non-inoculated: 54%  In all cases partial or total drug removal was observed.  5 pharmaceuticals showed negative elimination rates.
  • 29. III. Treatment of MBR sludge Non-spiked Bioslurry
  • 30. III. Treatment of MBR sludge  Liquid MBR sludge can be treated with T.v. at the Erlenmeyer scale.  T.v. grown under non-sterile conditions without any extra nutrients.  The time to eliminate the drug was reduced with T.v. Non-spiked Bioslurry
  • 31. III. Treatment of MBR sludge Biopiles system  Determine the efficiency of T.v. to eliminate HZT in a biopiles system.  Waste as substrate: Olive Pruning
  • 32. III. Treatment of MBR sludge Biopiles
  • 33. III. Treatment of MBR sludge  Removal: 86%  Is not feasible to treat MBR sludge in biopiles due to its high water content. Biopiles
  • 34. IV. Treatment of WWTP’s dried sludge Biopiles in trays  Determine the efficiency of T.v. to eliminate PPCPs in larger biopiles (380g).  Sludge from WWTP El Prat de Llobregat  Waste as substrate: Pine Bark
  • 35. IV. Treatment of WWTP’s dried sludge Biopiles in trays
  • 36. IV. Treatment of WWTP’s dried sludge Biopiles in trays
  • 37. IV. Treatment of WWTP’s dried sludge SAILAB Results Compound Initial sludge Biopiles before reinoculation Reinoculated biopiles at final time Non- einoculated biopiles at final time Sludge + Substrate at final time Sludge at final time Bisoprolol 0.5 0 0 0 0 0 Enroflaxicin 1.4 0 0 0 0 0 Progesterone 5.3 0 0 0 0 0 Methadone 5.6 0 0 0 0 0 Diclofenac 1.1 0 0 0 0 0 Gemfibrozil 0.43 0 0 0 0 0.4 Indomethaci n 0.4 0 0 0 0 0 ICRA Results  21 compounds detected  High disparity between triplicates and times Biopiles in trays
  • 38. IV. Treatment of WWTP’s dried sludge Biopiles in trays  The low repeatability is due to sampling technique.  Difficult to take unitary and representative samples in large biopiles.
  • 39. IV. Treatment of WWTP’s dried sludge Biopiles in bottles  Determine the efficiency of T.v. to eliminate PPCPs in small (20g) but more representative biopiles.  Sludge from WWTP El Prat de Llobregat  Waste as substrate: Pine Bark
  • 40. IV. Treatment of WWTP’s dried sludge Biopiles in bottles
  • 41. V. Fungi as low-cost sorbent for Heavy Metals  Treatment of heavy metals with T.v..  The first step was to reproduce a published adsorption experiment with another fungus.  Impossible to reproduce the conditions of the paper.  Inconsistent results.  This research line has been abandoned.
  • 42. VI. Post-treatment of WWTP’s water  Improve the quality of reclaimed wastewater used in SAT.  Determine the efficiency of 2 low-cost sorbents to eliminate emerging pollutants.  NUA: neutralised used acid comes from heavy mineral processing residue  BIOCHAR: charcoal produced by the pyrolysis of biomass (eucalyptus).  Soil: Alice Springs SAT basin E
  • 43. VI. Post-treatment of WWTP’s water Pilot-scale basinsPilot-scale basins
  • 44. VI. Post-treatment of WWTP’s water Initial Screening  Determine the capacity of the soil to adsorb a mixture of 7 compounds without amendments.  24h batch sorption.  3 soil:solution ratio(g:mL): 1:1, 1:5 and 1:50.  Ibuprofen, carbamazepine, ofloxacin, trimethorpim, ketoprofen, propranolol, and sulfamethoxazole
  • 45. VI. Post-treatment of WWTP’s water Initial Screening
  • 46. VI. Post-treatment of WWTP’s water Ratio Experiment  Effect of the soil:amendment ratio in the adsorption of 3 compounds.  2 amendments: Biochar and NUA.  24h batch sorption.  1 soil:solution ratio(g:mL): 1:5.  5 amendment:soil ratio: 0.1, 0.5, 1, 2, and 5%.  Trimethorpim, propranolol, and sulfamethoxazole.
  • 47. VI. Post-treatment of WWTP’s water Ratio Experiment
  • 48. VI. Post-treatment of WWTP’s water Incubation Experiment  Determine the sorption of a mixture of 7 compounds into a soil amended with biochar and NUA.  21d batch sorption experiments.  3 soil:solution ratio(g:mL): 1:1, 1:5 and 1:50.  1 amendment:soil ratio: 1%.  Ibuprofen, carbamazepine, ofloxacin, trimethorpim, ketoprofen, propranolol, and sulfamethoxazole
  • 49. VI. Post-treatment of WWTP’s water Incubation Experiment