Desalination for landfill leachates containing condensed inorganic salts

Desalination for landfill leachates containing condensed inorganic salts

Desalination, 97 (1994) 415-425 Elsevier Science B.V., Amsterdam - 415 Printed in The Netherlands Desalination for landfill leachates containing con...

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Desalination, 97 (1994) 415-425 Elsevier Science B.V., Amsterdam -

415 Printed in The Netherlands

Desalination for landfill leachates containing condensed inorganic salts Toshio Kawanishi, Shingo Matsumoto, Yasuo Horii and Morio Masuzaki Kubota Corporation, 2-47, Shikitsuhigashi I-chome, Naniwa-ku, Osaka 556 (Japan)

SUMMARY

Recently in Japan, leachates from general waste landfills have increased their inorganic salt concentration and have caused various problems inside and outside treatment facilities. Because there is strong demand for countermeasures to cope with these problems, the authors have undertaken studies on leachate desalination using a continuous type electrodialyzer. The results of the experiments confirmed that stable desalination can be achieved by conducting the conventional leachate treatment as pre-treatment. Furthermore, comparing desalination methods, we have come to the conclusion that electrodialysis is most appropriate for landfill leachate desalination.

INTRODUCTION

In recent years plastic refuse has been incinerated in municipal waste plants in Japan. As a result, fly ash with a high chlorine content is discharged from the exhaust gas hydrogen chloride scrubbing equipment. This ash is eventually disposed of in general waste landfills where leachates have increased their inorganic salt concentration and cause various problems inside and outside the treatment facilities. There is strong demand for countermeasures to cope with these problems. OOll-9X34/94/$07.00 0 1994 Elsevier Science B.V. All rights reserved. SSDIOOll-9164(94)00104-V

416

An outstanding example of ecological damage caused by salt is the appearance in mountain rivers of diatom (Amphiprora alata) which grow in brackish water such as water in a river mouth. Present countermeasures against salt damage, for example damage to paddy rice plants, has been the dilution of leachate with rain water or underground water. The development and practical use of desalination technology for leachate treatment is also expected. Against this background, the authors have undertaken a series of studies on leachate desalination using a continuous type electrodialyzer.

EXPERIMENTALDESIGN

Raw water

Our sample was a leachate from a lysimeter (experimental landfill tub) filled with mixed refuse (Cl- content 2.8% by weight) containing 70% incineration residue, 20% noncombustible shredded refuse, and 10% municipal refuse compost. Equipment

1. Lysimeter - a square steel tub of 6 m width, 10 m length (2x5 m chambers) and 2.5 m height having a hopper base and a total capacity of 112.5 m3 (nominal). The five chambers are of three types: three semiaerobic, one anaerobic, and one leachate circulating semi-aerobic. Table I lists the refuse filling conditions for the lysimeter of which leachate was sampled. TABLE I Filling conditions for lysimeter Status of landfill

Completed

Landfill structure Water content, %

Semi-aerobic

Wet filled weight (t)

20.0

Filled volume (m3)

15.8

19.9

417

14’r”r mnval I .

.

Biol ical Q+tiag trea#ent se#~ti~

sandfiltration, Activated carbon

adsorption OesaliMtiMl AA

r-l-

Fig. 1. Flow diagram of test plant.

2. Leachate treatment test plant - Fig. 1 shows a flow diagram of the test plant based on the addition of sodium carbonate in combination with ferric chloride for Ca removal and a contact aeration process with saddleshaped packing for biological treatment. 3. Desalination equipment - The equipment used was a continuous type electrodialyzer (70 cm W x 120 cm L x 154 cm H) comprising an electrodialysis bath, a demineralized water circulator, a concentrated water circulator, and other elements. Table II gives outline specifications of the electrodialyzer. Fig. 2 is a flow diagram of the electrodialyzer. The multichamber electrodialysis bath employed ion-exchange membranes pretreated for selective passage of monovalent cations and anions based on remarkable differences in ion permeability (Na+ > Ca*+; Cl- b SO:-. TABLE II Outline specifications of electrodialyzer Method of water feed

Continuous type

Electrodialysis

Effective membrane surface area 2dm2 x lopairs

bath

Cation membrane (12 units) Strongly acidic Anion membrane (10 units) Strongly alkaline Rectifier

DC outout = 10 A x 55 V

418

ElectrcdialysSs bath

kctif ier

Fig. 2. Flow diagram of electrodialyzer.

Method

Leachate was temporarily stored in the feed tank and then pumped to the test plant in a fixed volume for pretreatment. After activated carbon adsorption, the pretreated leachate was desalinated under three sets of conditions: Run 1 for a target Cl- level of 200 mg/l, Run 2 for 500 mg/l, and Run 3 for 1000 mg/l.

RESULTS AND DISCUSSION

Results of pretreatment

Leachate feed rates were in the 50-60 l/d range. Results of the pretreatment are given in Table III, in which figures for water quality parameters are mean values over the experimental desalination period. BOD, COD and TOC removal

Fig. 3 shows concentration changes by process. BOD was reduced to 8.5 mg/l (99% removal) by contact aeration, marking good performance

7.0 816

7.8

398

135

405

732

0.66

480

2.117

PH M-alkalinity, mg/l

ORP, mV

TOC, mg/l

BOD, mgh

DO, mg/l

COD&, mg/l

COD,,

8.9

221

18,400

1,450

1,363

9,377

TDS, mg/l

T-Ca, mg/l

Ca2+, mg/l

Cl-, mg/l

36

NH,-N, mgl

SS, mg/l

87

Kje-N, mg/l

NO,x-N, mg/l

96

T-N, mg/l

mg/l

23

22

Temperature, “C

9,300

20

24

18,650

28

9.7

29

38

48

1,585

447

637 -

400

134

Calcium removal

Water quality parameter

Test plant treatment results

TABLE III

8,943

27

34

16,550

12

37

0.9

19

55

507

207

2.7

8.5

209

120

788

8.3

23

9,911

30

36

16,250

22

28

1.8

15

41

433

116

-

6.5

148

133

269

7.2

22

9,411

46

56

17,550

21

27

2.4

16

43

347

110

3 -

130

145

262

6.8

22

Contact Coagulating Sand aeration sedimentation filtration

9,505

71

72

17,750

26

28

1.4

4.4

32

243

13

2 -

19

80

211

6.6

22

Activated carbon

191

0.6

0.7

860

0.4

1.1

0.4

0.9

2.0

4.5

4

0.4 -

5

52 -

8.0

22

RUN 1

479

0.7

0.9

1,130

1.8

0.8

0.1

0.8

1.6

8

4

1.3 -

6

65 -

7.4

26

RUN 2

Electrodialysis

939

0.9

1

2,450

2.6

2.3

0.3

0.5

2.8

10

6

1.5 -

8

160 -

7.1

27

RUN 3

P e

420

A=T 0

C

OfB

0 0 x -CODnn 0 =CODcr

Fig. 3. Concentration

changes by process (1).

of the biological treatment. Membrane pollution with organic substances did not occur in the electrodialysis bath, probably because of the low residual BOD of 2 mg/l in the water treated with activated carbon (hereinafter referred to as “pretreated leachate”). Considerable amounts of COD substances remained in the treated water after contact aeration at 207 mg/l for COD,, and 507 mg/l for COD,,, which are attributable to sparingly biodegradable COD substances characteristic of leachate. In the coagulating sedimentation treatment which followed, coagulation was conducted in an acid range (pH 5-6) with a relatively high COD,, removal of 76%. TOC was removed in a pattern similar to that of COD,, removal, with a value of 19 m/l for the pretreated leachate. Nitrogen removal

Fig. 4 shows concentration changes by process. the changes in NH,-N and NO,-N concentrations suggest fair nitrification in the contact aeration chamber. Calcium removal

The mean T-Ca concentration of leachate was 1450 mg/l, 94% of which was accounted for by soluble Ca2+ ions. The Ca removal process reduced the T-Ca content to 24 mg/l (98%) removal) but was followed by a slight increasing tendency after biological treatment.

421

Fig. 4. Concentration changes by process (2).

Results of desalination Table IV gives the operating conditions for the continuous type electrodialyzer. The results of the desalination treatment are given in Table III. Fig. 5 shows desalination characteristics for Run 2. Because reduction in permeate flux, due to density polarization in the ion-exchange membrane of the electrodialysis bath, membrane surface, organic pollution, etc., is critical in the practical application of the system, permeate flux changes were examined in each run. The results are given in Table V. Chlorine ion permeate flux (J Cl), an index of the Cl- permeability of the ion-exchange membrane, was obtained using the Nernst-Planck approximate equation as follows: JCl

= -2 Cl U Cl C Cl

l

d4ldx

(1)

TABLE IV Desalination

conditions

Item

RUN1

RUN2

RUN3

Cl- target level, mg/l Leachate feed rate, l/min Membrane surface flow velocity Stationary DC voltage, V

200 1.2-2.0 2.5-3.9 7- 10

500 1.2-3.2 2.3-6.2 8-10

1000 3.0-3.3 5.8-6.4 9-10

(cm/s)

422

Fig. 5. Desalination

characteristics.

TABLEV Chlorine ion permeate flux by run Flux (mol/cm2

where 2 Cl represents an ionic valency, C Cl the Cl concentration in the membrane, U Cl the Cl- mobility through the membrane, $J the potential, and x a variable (cm) at a right angle with respect to the membrane surface. Permeate flux Chlorine ion permeate flux values (Table V) demonstrated no significant reduction due to membrane pollution in any of the runs. The results show that the greater the target level (200 mg/l, 500 mg/l, 1000 mg/l), the greater the chlorine ion permeate flux. Desalination level We were able to desalinate a pretreated leachate containing about 10,000 mg/l chlorine ions below the target Cl- concentrations of 200,500,

423

and 1000 mg/l for Runs 1, 2 and 3, respectively. The TDS/Cl- ratio increased from about 1.9-2.0 for the leachate to 2.6-4.5 for the desalinated water, suggesting selective permeation of Cl- ions. Other water quality parameters

BOD decreased from 2 mg/l for the pretreated leachate to 0.4-1.5 mg/l, and TOC from 19 mg/l to 5-8 mg/l, indicating a slight removal of organic substances. As for nitrogen, high N removal efficiencies were obtained, irrespective of the form of N - with treated water T-N concentrations of 1.6-2.8 mg/l, or 91-95% T-N removal. Use of this system shows the potential to achieve effluent T-N levels of under 3 mg/l.

PRACTICAL

LEACHATE

DESALINATION

We also conducted an experiment with a sampling of treated leachate from an actual facility. It confirmed that the leachate can be desalinated using our experimental electrodialyzer. Table VI gives an example of the practical leachate desalination results. TABLE VI

Practical leachate desalination results Chlorine ion concentration

RUN A

RUNB

Leachate Cl-, mg/l Treated water Cl-, mg/l

5192 268

5203 573

COMPARISON

OF LEACHATE

DEiSALINATION METHODS

Currently available methods of chlorine ion removal include ion exchange, distillation, reverse osmosis, and electrodialysis. Of these the ion-exchange method is used at the lower extreme of Cl- concentrations of 500 mg/l or lower, while the distillation method is used at the higher extreme, or Cl- concentrations of a few tends of thousands of milligrams per liter or higher. Since the adaptability of these methods for landfill

424

TABLE VII Comparison of desalination methods Item

Electrodialysis

Reverse osmosis

Membrane-passing substance (s)

Cations and anions

Water

Membrane type

Ion-exchange membrane

Semi-permeable membrane

Recovery ratio

90-95 I

50-70 %I

Features

aHigher valencies facilitate separation *Inappropriate membrane surface flow rates result in concentration polarization tending to reduce the desalination efficiency

When the silica (Si02) content increases above 20 mg/l, membrane clogging is likely

TABLE VIII Si and SiO, concentration changes by process Process

Si (mg/l)

SiO, (mg/l)

Feed tank Calcium removal Contact aeration Coagulating sedimentation Sand filtration Activated carbon Electrodialysis

147 119 95 56 46 43 20

316 254 203 121 98 92 43

leachate treatment is poor, the reverse osmosis and electrodialysis methods are under investigation as practical methods. Table VII lists the characteristics of these latter two methods for comparison. Table VIII gives Si and SiO, concentration changes by process. The leachate contained a high concentration - 316 mg/l - of SK&. The SiO, concentration decreased to

425

92 mg/l after activated carbon treatment but remained above the value of 20 mg/l. Membrane clogging is therefore likely in the reverse osmosis method.

RECAPITULATION

Results of the present basic experiments on leachate desalination using a continuous type electrodialyzer are summarized as follows: 1. Even when chlorine ion concentration is as high as 10,000 mg/l, continuous desalination of the leachate to a chlorine ion concentration of 200 mg/l or lower is possible solely by using the electrodialysis method. 2. Appropriate pretreatment prevents reduction in the chlorine ion permeate flux in continuous electrodialysis treatment and increases the permeate flux with a rise in the target value for chlorine ion treatment. 3. Because leachate sometimes contains a high concentration of silica (SiO,), as in the present study, and the treatment water recovery ratio of the electrodialysis method is higher than that of reverse osmosis, then electrodialysis is the most appropriate method for leachate desalination. 4. Continuous electrodialysis proved capable of stably removing nitrogen, showing the potential for reduction of the treated water nitrogen concentration to below 3 mg/l.

CONCLUSIONS

The present study was conducted within the framework of a cooperative project by the Association for the Study of High Salt Leachate Treatment Systems. The Association will continue to study leachate desalination based on continuous electrodialysis, together with the investigation of membrane service life and the development of concentrated water recycling technology. REFERENCES 1

2

M. Hanajima,, T. Shimaoka, S. Higuchi, R. Yamaguchi, Y. Horii and H. Nagaoka, Proc., First Annual Conference of the Japan Society of Waste Management Experts, pp. 337-340. M. Hawjima, T. Shimaoka, S. Higuchi, Y. Horii and N. Nagaoka, Proc., Second Annual Conference of the Japan Society of Waste Management Experts, pp. 293-296.