Control of landfill leachates contaminated groundwater by a ...Ni, Cr (Vito) o-xylene, p-xylene,...

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

NATO-CCMS, 11 juli 2004, Cardiff 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


Microorganismsbacteria, fungi

Carrier material

Fe 0, Carbon,

Sand

Growth

addi

tives

Nutrien

ts, O

RC, com

post

Mixed pollution

heavy metalsVOCls

aromatics

PARTNERS:

Vito, MolUniversity 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

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 CaCl2.2H2O0.5 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 F400GAC Ind. React. (landfills)

(Aquifer material)MetasorbZeolitesWood chips

•Mixed pollution:VOCls: 2 mg/l PCE

5 mg/l TCEMetals: 5 mg/l Zn as ZnCl2

0.2 mg/l As(V) as Na2HAsO4

BTEX: 2 mg/l benzene2 mg/l toluene2 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 culturesAxenic strains


MULTIBARRIER materials

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

+ Aquifer as source of micro-organisms


Design of multibarriers


• Different multibarrier concepts:

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

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


TEA

SEQUENTIAL MIXED

O2 +

NO3- +

SO42- + +

Fe3+ + +

CO2 + +

As +

VOCls + +

Bio/Fe0

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


PCE+TCE

metals

BTX

1,2-cisDCE

BTX

NO3-

(1 mM)

BIO

Fe0 0

20

40

60

80

100

0 100 200 300 400 500

t (d)

% b

enze

ne r

emov

a

Fe(0)BioMB

[NO3] (mM): 1 0 1

HRTx 1.3

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


System D: PCE & TCE degradation (SR columns)1 2 3 4

Bio Bio

Bio

Bio+Fe

Fe

Fe


initial sorption

incomplete PCE degradation

complete TCE degradation

0

25

50

75

100

0 50 100 150 200

t (d)%

PC

E re

mov

al

C1 aqC2A FeC2B aqC2 MBC3A aqC3B FeC3 MBC4 mix

0

25

50

75

100

0 50 100 150 200

t (d)

% T

CE

rem

oval


System D & E: Benzene removal

1 2 3 4

Bio Bio

Bio

Bio+Fe

Fe

Fe


SR: no degradation

IR:- all MB- not in C2aq

0

25

50

75

100

0 50 100 150 200

t (d)%

ben

zene

rem

oval


0

25

50

75

100

0 50 100 150 200

t (d)

% b

enze

ne re

mov

al


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

0123456789

10

0 100 200 300 400 500 600

Distance in column (mm)

pH

-500

-400

-300

-200

-100

0

100

200

300

ORP (mV)

pHORP

0

500

1000

1500

2000

2500

3000

3500

4000

0 200 400 600


PCE,

TC

E (p

pb)

0

5

10

15

20

25

30

35

40

45

50

cDC

E (p

pb)

PCETCEcDCE

0500

10001500200025003000350040004500

0 200 400 600


(ppb

) BTm-X



System 1-5: Results DCM &11DCA

100%

50%

10%

0% Noand

50% (2nd)

No

50%

No

>50%

Complete

Complete

No

Fe(0)

redox conditioningelectron donor

Results (% removal)


Column trains

Characteristics (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 barriersMULTIBARRIERs 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

Conclusions


• 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


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-systemsMonitoring of microbiology (molecular biology)


WP3: HM + Mesocosms containerPearson correlation (Opt:0.90%) [0.0%-100.0%]MB

100

90807060504030

MB

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

.

MESO A1 T0 AMESO A2 T0 A

MESO A2 T0 BMESO A1 T0 B

MESO A5 T0 A

MESO A5 T0 BMESO A7 T0 A

MESO A7 T0 Bmengsel HM/AqDEC (bulk) B

mengsel HM/AqDEC (bulk) A

AqDEC (bulk) BAqDEC (bulk) A

mengsel HM/AqDEC/FeA4 (bulk) Bmengsel HM/AqDEC/FeA4 (bulk) A

MB Aquifer

HM (bulk) BHM (bulk) A

JD 112JD 112

JD 107JD 106

JD 104

JD 105

HMHM

Aëroob 2 onderAëroob 2 (REF) boven

Aëroob 1 (MB) boven

Aëroob 1 onder


MULTIBARRIER Modelling System: salt injection

new gage3

new gage2

new gage1

X

Y

Z

new gage3

new gage2

new gage1

X

Y

Z


new gage3

new gage2

new gage1

X

Y

Z

new gage3

new gage2

new gage1

X

Y

Z

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 md = 3,5 md = 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

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Control of landfill leachates contaminated groundwater by a ...Ni, Cr (Vito) o-xylene, p-xylene,...

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