NATO-CCMS, 128 juni 2015, Cardiff 2004 Control of landfill leachates contaminated groundwater by a MULTIBARRIER approach L. Diels, J. Dries, L. Bastiaens

NATO-CCMS, 118 april 2023, Cardiff 2004

Control of landfill leachates contaminated groundwater by a MULTIBARRIER approach

L. Diels, J. Dries, L. BastiaensFlemish institute for technological research, Vito

Mol, Belgium

NATO-CCMS Pilot StudyPrevention and Remediation in Selected Industrial Sectors:

Rehabilitation of old landfills Cardiff, May 23 – 26, 2004

No measures


Landfill leakage: Multifunctional treatment zone or Multibarrier for removal of mixed pollutants

Evaluation of several combinations

– Chemical transformation (Fe°),

– Biotransformation (aerobic/anaerobic),

– Bioprecipitation

– Sorption

Two solutions:

-Installation of a new landfill(20 – 40 million EURO)

-Installation of a MULTIBARRIER(2 - 4 million EURO)

Groundwater flow

GW level


EU-project MULTIBARRIER

PARTNERS:

Vito, Mol University of WageningenUniversity of InnsbruckTUniversity of MunchenIBA, HeiligenstadtBIOTECs, BerlinUniversity of PragueDEC, ZwijndrechtUniversity of Latvia, RigaUnivesity of Mining, Sofia, Bulgaria

ENDORSERS:Montgomery Watson Harza, BrusselsIntercommunale Hooge Maey, Antwerp

Microorganisms

bacteria, fungi

Carrier material

Fe 0, Carbon,

Sand

Gro

wth

add

itive

s

Nut

rient

s, O

RC

, com

post

Mixed pollution

heavy metalsVOCls

aromatics


Mixed contamination plumes• Mixed contamination plumes require:

– a combination of different pollutant removal processes (biotic & physico-chemical)

– a combination of barrier types = MULTIBARRIER

• Design and optimisation of multibarriers is more complex than single-barriers– Concept: sequential or mixed multibarrier?

– Effect of the pollutants on the removal process (inhibition, stimulation or no effect)?

– Effect of one pollutant removal process on an other one?


MULTIBARRIER Key-components• Groundwater:

0.5 mM NaHCO3

0.5 mM KHCO3

0.5 mM CaCl2.2H2O

0.5 mM MgCl2.6H2O

+ growth supporting additives (Nutrients, O2, compost,..)

• Carrier materials:Filter sand (1-2 mm)

Zerovalent iron FeA4 (0.3-2 mm)

Activated carbon

GAC F400

GAC Ind. React. (landfills)

(Aquifer material)

Metasorb

Zeolites

Wood chips

•Mixed pollution:VOCls: 2 mg/l PCE

5 mg/l TCE

Metals: 5 mg/l Zn as ZnCl2

0.2 mg/l As(V) as Na2HAsO4

BTEX: 2 mg/l benzene

2 mg/l toluene

2 mg/l m-xylene

Extra: AOX (LFU)

DCM, 11 DCA (UW)

Ni, Cr (Vito)

o-xylene, p-xylene,

Ethylbenzene (Vito)•Micro-organisms:

Aquifer material

Enrichment cultures

Axenic strains


Filtersand

Specific surface [m2/g] (measured)

FiltersandEverzitMetasorbGAC F400Zerovalent Iron

1,9294,1

3,0764,4

1,0Everzit Metasorb GAC F400

magnitude: 500x

Zero Valent IronFiltersand

MULTIBARRIER materials

+ Aquifer as source of micro-organisms


• Different multibarrier concepts:

• Concept = Site specific and depending on the pollutants present• Sorption barrier = polishing step

Design of multibarriers

SorptionBiodegradationReduction - Fe0

Mix

ed p

ollu

tion

g

SorptionBiodegradation Reduction - Fe0

...Mixed multibarrier


MULTIBARRIER concepts: Sequential vs mixed

BIO

Fe0

TEA SEQUENTIAL MIXED

O2

NO3- ?

Fe3+

SO42-

CO2

Bio/Fe0

TEA

SEQUENTIAL MIXED

O2 +

NO3- +

SO42- + +

Fe3+ + +

CO2 + +

As +

VOCls + +


System A (O2) & System B (NO3)

Biocolumns

Ironcolumns

Influent

PCETCE

Mixingvessel

N2

B T m-X

Aerobic/anoxicmedium

A

B

C2 1 3 4


Benzene removal in a denitrifying sequential system

0

20

40

60

80

100

0 100 200 300 400 500

t (d)

% b

en

ze

ne

re

mo

va

l

Fe(0)

Bio

MB

[NO3] (mM): 1 0 1

HRTx 1.3

PCE+TCE

metals

BTX

1,2-cisDCE

BTX

NO3-

(1 mM)

BIO

Fe0


Systems D & E: Strictly anaerobic systems

1 2 3 4

Bio Bio

Bio

Bio+Fe

Fe

Fe

SR: 0.5 mM SO42-

IR: 2.5 mM Fe(III)EDTA


1 2 3 4

Bio Bio

Bio

Bio+Fe

Fe

Fe

System D: PCE & TCE degradation (SR columns)

initial sorption

incomplete PCE degradation

complete TCE degradation

0

25

50

75

100

0 50 100 150 200

t (d)%

PC

E r

em

oval

C1 aq

C2A Fe

C2B aq

C2 MB

C3A aq

C3B Fe

C3 MB

C4 mix

0

25

50

75

100

0 50 100 150 200

t (d)

% T

CE

rem

oval

C1 aq

C2A Fe

C2B aq

C2 MB

C3A aq

C3B Fe

C3 MB

C4 mix


1 2 3 4

Bio Bio

Bio

Bio+Fe

Fe

Fe

System D & E: Benzene removal

SR: no degradation

IR:- all MB- not in C2aq

0

25

50

75

100

0 50 100 150 200

t (d)%

ben

zen

e r

em

oval C1 aq

C2A Fe

C2B aq

C2 MB

C3A aq

C3B Fe

C3 MB

C4 mix

0

25

50

75

100

0 50 100 150 200

t (d)

% b

en

zen

e r

em

oval C1 aq

C2A Fe

C2B aq

C2 MB

C3A aq

C3B Fe

C3 MB

C4 mix

SR

IR


System C: Partially mixed MB system

Columns (L = 50 cm)K1: test columnK2: abiotic control

Layers:L1: FS/Aq/Fe0 = 60/20/20 (W)L2:FS/Aq = 78/22 (W)

Monitoring:chemical analysesmicrobial ecology


Partially mixed MULTIBARRIER: results

0

1

2

3

4

5

6

7

8

9

10

0 100 200 300 400 500 600

Distance in column (mm)

pH

-500

-400

-300

-200

-100

0

100

200

300

ORP (mV)

pH

ORP

0

500

1000

1500

2000

2500

3000

3500

4000

0 200 400 600


PC

E, T

CE

(p

pb

)

0

5

10

15

20

25

30

35

40

45

50

cD

CE

(p

pb

)

PCE

TCE

cDCE

0

500

1000

1500

2000

2500

3000

3500

4000

4500

0 200 400 600


(pp

b) B

T

m-X


100%

50%

10%

0%

System 1-5: Results DCM &11DCA

Noand

50% (2nd)

No

50%

No

>50%

Complete

Complete

No

Fe(0)

redox conditioning

electron donor


Results (% removal)Column

trainsCharacteristics (TEA) Acro-nym PCE TCE Benzene Toluene m-xylene

System A: Zerovalent iron wall followed by a micro-aerobic biobarrier 1

A1 1 – Fe(0)column A1-1 60-80 90-99 4-13 10-53 NA

2 – Bio column (O2) A1-2 80-100 92-100 99-100 99-100 > 90

System B: Zerovalent iron wall followed by a denitrifying biobarrier 1

B1 1 – Fe(0)column B1-1 66-99 97-100 6-18 16-54 NA

2 – Bio column (NO3-) B1-2 80-93 97-100 89-100 99-100 > 90

System C: Partially mixed Fe(0)/biowall followed by anaerobic biowall 2, 1

C1 1 – mixed zone C1-1 95-100 1 95-100 1 20 2 30 2 40 2

2 – bio zone C1-2 95-100 1 95-100 1 20 2 30 2 50 2

System D: sequential and mixed barriers under sulfate reducing conditions 1

D1 1 – Bio column (SO42-) D1-1 0-11 0-15 11-44 97-100 NA

D2 1 – Fe(0)column D2-1 55-71 88-98 4-54 0-36 NA

2 – Bio column (SO42-) D2-2 55-78 89-98 23-67 12-36 < 25

D4 1 – Mixed column (SO42-) D4-1 76-89 99-100 18-62 7-23 > 90

System E: sequential and mixed barriers under iron reducing conditions 1

E1 1 – bio column (Fe3+) E1-1 0-11 9-18 24-29 100 NA

E2 1 – Fe(0)column E2-1 53-67 85-92 50-68 72-91 NA

2 – Bio column (Fe3+) E2-2 54-67 86-92 52-71 77-90 > 90

E4 1 – Mixed column (Fe3+) E4-1 58-73 94-97 55-64 94-98 > 90


Conclusions• Mixed contamination plumes are omnipresent.

• Remediation of mixed contamination plumes using barriers MULTIBARRIERs are required

• Fungi do not play a big role in a Multibarrier

• In lab-scale columns different Multibarrier-concepts have been shown to be effective for the remediation of a mixed plume (PCE, TCE, BTmX, Zn, As).

• Behaviour of AOX in a Multibarrier is under study

• No toxicity detected in effluent (toxicity reduction) • The design and optimisation of multibarriers is more complex in

comparison with ‘single barriers’Many influencing parameters have to be taken into accountMixed Multibarrier under iron or sulfate reducing conditions


• Sequential Multibarrier: ZVI + Micro-aerofilic biobarrier– PCE, TCE dehalogenation in ZVI– Zn, As removal in ZVI– BTX degradation in biobarrier– No degradation of cDCE

• Sequential Multibarrier: ZVI + Anaerobic biobarrier (denitrifying)– PCE, TCE dehalogenation in ZVI– Zn, As removal in ZVI– T, X degradation in biobarrier– B partially degraded in biobarrier– No degradation of cDCE

• Mixed Multibarrier: filtersand, aquifer materiaal, ZVI + Anaerobic biobarrier in aquifer – PCE, TCE dehalogenation– Zn, As removal in ZVI– BTX degradation in mixed zone– No formation of cDCE or VC

Conclusions


Upscaling promising multibarrier concept

Aquifer AquiferReactive materials

Groundwater

Closed system

Pollutant-mixing& monitoring unit Posttreatment

A: coarse zone (25 cm)

B: Aquifer material

C: mixed Bio/Fe0 barrier : FeA4/Aq/HM = 30/60/10

D: Biobarrier Aq/ HM (90/10)

E: Biobarrier Aq

E: coarse zone (25 cm)

F: Sorption barrier

0.5 m 1 m 3 m

BIOFe0/BIO

PCE, TCE, Zn, As, BTEX Polishing

BTEX?A B C D E F G


Set-up of MB on pilot scale



MULTIBARRIER Monitoring System (MMS)

• On-line measuring and logging system pH, T, ORP, conductivity, O2 and pressure :

– Tested in the pilot system

– Focus on EC-measurement

• in-well mixing system has been tested:– Works very well


Pilot MULTIBARRIER system: First experiment

• Monitoring strategy:

10-20 cm bgs170-180 cm bgs

90-100 cm bgs 90-100 cm bgs

10-20 cm bgs170-180 cm bgs

EC-measurementsStirred electrode set

Non-stirred electrode set


Monitoring of PRBs

A

B

B

B

C

C

C

D

E

E

E

F

G

G

Plume

Gravel

Reactive material

Monitoring well

100 m

- UK guidelines - US EPA guidelines - Flanders (OVAM) guidelines - Germany (in preparation?)


In situ mesocosm-systems

Monitoring of microbiology (molecular biology)


WP3: HM + Mesocosms container

Pearson correlation (Opt:0.90%) [0.0%-100.0%]MB

100

90807060504030

MB

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

MESO A1 T0 A

MESO A2 T0 A

MESO A2 T0 B

MESO A1 T0 B

MESO A5 T0 A

MESO A5 T0 B

MESO A7 T0 A

MESO A7 T0 B

mengsel HM/AqDEC (bulk) B

mengsel HM/AqDEC (bulk) A

AqDEC (bulk) B

AqDEC (bulk) A

mengsel HM/AqDEC/FeA4 (bulk) B

mengsel HM/AqDEC/FeA4 (bulk) A

MB Aquifer

HM (bulk) B

HM (bulk) A

JD 112

JD 112

JD 107

JD 106

JD 104

JD 105

HM

HM

Aëroob 2 onder

Aëroob 2 (REF) boven

Aëroob 1 (MB) boven

Aëroob 1 onder

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

16/07/03C

10/04/03G

16/07/03C

16/07/03C

18/07/03D

03/04/03D

03/04/03D

03/04/03D

03/04/03D

03/04/03D


MULTIBARRIER Modelling System: salt injection


Modelled salt-peaks • Permeability: 24.17 m/dag• Dispersivity: 0.3 m• Monitoring wells: filter 100 cm bgs,• Result: migration of pollutant initally faster, afterwards slower in comparsion with

measured values

0

10

20

30

40

50

60

70

80

90

0 5 10 15 20 25 30 35 40

d = 5 m

d = 3,5 m

d = 1,5 m

Time (days)

Conc %


Pilot scale Multibarrier:Curilo deposit


Installation at Curilo deposit

3 m

2 m0.1 m0.6 m

1.5 m

2.0 m

1.5 m

1.0 m

5.0 m

0.8 m

1.0 m

12

34

5

0,5 m

3

4

17.5 m

15.0 m

1.6 m


Curilo deposit: constructed wetland + Multibarrier


Thanks to all the partnersand the European Commission

QLK3-CT-2000-00163+

QLRT-2001-02916

www.multibarrier.vito.be

Documents

NATO-CCMS, 128 juni 2015, Cardiff 2004 Control of landfill leachates contaminated groundwater by a MULTIBARRIER approach L. Diels, J. Dries, L. Bastiaens