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Land Decontamination in South Tangerang and

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Management of Contaminated Soil Waste

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A R T I C L E I N F O A B S T R A C T 12

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AIJ use only:

Received date Revised date Accepted date Keywords:

Contaminated soil

137Cs

Decontamination

Management of contaminated soil Treatments

...

Recently it was found the contamination of 137Cs that was on an empty land in an area at South Tangerang, for that reason the area which was contaminated with

137Cs needs to be cleaned up by doing the decontamination works at that place.

Then continue with the activity of managing contaminated soil. The decontamination works were carried out by peeling the contaminated soil, and then put it into a 100L drum. The drums contained contaminated soil send to the interim storage facility for further treatment. To resolve the case of 137Cs contamination on the soil, it is necessary to study the decontamination and management of contaminated soils. Some techniques and strategies for decontamination and managing 137Cs contaminated in the soil are presented in this paper. Further evaluation needs to be done so that the results of the study could be used appropriately to treat the contaminated soil waste from the land in South Tangerang.

© 2020 Atom Indonesia. All rights reserved

14

INTRODUCTION

15 16

In middle of February 2020, Indonesia was

17

shocked by the founding of 137Cs radioactive

18

contamination on an empty land in the South

19

Tangerang by Bapeten (nuclear energy regulatory

20

body in Indonesia), and then the news in Indonesia

21

(newspaper and online news) was filled with this

22

sensational news [1-5]. Radioactive contamination

23

has been found on an empty land close to the

24

resident home in South Tangerang. The location of

25

the event is shown in Figure 1. The higher activity

26

compared to the surrounding environment causes

27

the regulatory body to pay attention and

28

coordination with National Nuclear Energy Agency

29

(BATAN) to carry out a mitigation plan of the land

30

to perform the decontamination activity. The

31

contamination needs to be handled well, carefully

32

and safely so as not to cause panic in the

33

community, and more importantly that the activity is

34

able to minimize the subsequent impacts such as the

35

possibility of further spreading of radioactive

36

Corresponding author.

E-mail address:

contaminants into around the location. The

37

decontamination activities started under the

38

supervision of BATAN to decontaminate soils.

39

40

Figure 1. Map of location of radioactive contamination 41

has been found 42

43

Before conducting the studies of

44

decontamination and management of contaminated

45

soil by 137Cs, the nature of 137Cs needs to be

46

understood first. Radiocesium-137 has a high

47

solubility properties in solution and has long half-

48

life (about 30 y). When the 137Cs reach the

49

groundwater, it can cause as primary causes of

50 Atom Indonesia

(2)

water contamination to the residents at the

51

surrounding location due to easy associated with

52

plants and species exist in terrestrial and water

53

environment [6]. However the 137Cs is not very

54

mobile in the environment, it tends to accumulate

55

and bind strongly on the most surface of soil hence

56

absorb more localized. Consequently, 137Cs is

57

difficult for uptake by vegetation through roots [7].

58

Since the behavior of Cs+ ion is very similarly to

59

Na+ and K+ ions, thus facilitating its digestion and

60

assimilation in living organisms [8]. If the human

61

body is possessed by 137Cs substance, cells in the

62

body could become damaged due to the radiation

63

that might penetrate the entire body, and then it is

64

deposited in the soft tissues such as muscle and

65

nerve cell, and might also cause cancer [9]. To

66

protect the public health and worker, Bapeten issues

67

the regulations on Radiation Protection and Safety

68

in the Utilization of Nuclear Energy, where the

69

average effective dose limit for radiation workers is

70

set at 20mSv / year, while for the general public is

71

set at 1 mSv / year [10].

72

73

The circumstances in which the problem of

74

radioactive contamination (137Cs) occurred in South

75

Tangerang have a different character from the event

76

of nuclear accidents in Fukushima and Chernobyl.

77

In the events of Fukushima and Chernobyl

78

accidents, the contamination that occurs in the

79

surface soil due to the release of 137Cs from the

80

accident went to the atmosphere which makes it the

81

most abundant radioactive atmospheric pollutant

82

capable of taking health hazards. The 137Cs will then

83

return down to earth as a 137Cs fallout and settle on

84

the soil surface to a large extent as 137Cs

85

contaminants. Most of the contaminants have fallen

86

to the surface of the soil, so soil decontamination

87

activities in Fukushima and Chernobyl were carried

88

out by peeling the surface soil to a depth of about 5-

89

15 cm [12,13]. This activity was intended to clean

90

up the area from contaminants. While the 137Cs

91

contamination in South Tangerang was different.

92

Here the contamination came from 137Cs source

93

contaminated the surface and also in the sub-surface

94

of soil, so that the decontamination method that

95

must be carried out also has a slight difference in

96

treatment. To do the decontamination activity in

97

South Tangerang, an approach with the MARSSIM

98

manual can help decontamination activities [14].

99

The soil from the result of soil removal were put

100

into 100L drums. From the activity of

101

decontamination in South Tangerang, some

102

hundreds of drums containing 137Cs contaminated

103

soil were produced and sent them to an interim

104

storage (IS) facility to be stored safely before further

105

processing.

106

107

The technique of removal of 137Cs radioactive

108

from soil is a necessity and important, therefore the

109

results of the study are expected to find appropriate

110

technologies for the further use. For this reason, an

111

initiative the study of decontamination of 137Cs

112

contamination into soil and the manage volume of

113

waste generated from decontamination work will be

114

discussed in the paper. Information obtained from

115

the activities of decontamination and management

116

of the wastes, such as procedures, methods,

117

decontamination techniques and management of

118

137Cs contaminated soil (also how to remove and

119

treat the 137Cs from soil) will be explained briefly, as

120

well as some techniques and strategies for

121

approaching the treatment of contaminated soils.

122

Further evaluation needs to be done might the

123

results of the study could be considered

124

appropriately for the stakeholders to manage the

125

contaminated soil waste of the land in South

126

Tangerang.

127 128

METHODOLOGY

129

130

To conduct this study, the existing primary and

131

secondary data and the informations are relevant to

132

the decontamination of 137Cs contaminated soil and

133

its subsequent processing have been used. An

134

approach using the MARSSIM manual can assist in

135

the preparation of the initial survey activity

136

procedures, as well as the results to be obtained

137

from land decontamination activities. Then to learn

138

the techniques of accumulating the 137Cs

139

concentration of contaminated soils used study

140

material of management of contaminated soils

141

which was obtained from a compilation work to

142

similar activities in many places that have been

143

published. From here, the reviewed decontamination

144

techniques are then evaluated to obtain the suitable

145

treatment methods that can be considered for use in

146

the plan for processing of contaminated land waste

147

in further. In the end of the paper, some method to

148

reduce the volume of the contaminated soil wastes

149

are considered to be proposed to the management.

150

151

RESULTS AND DISCUSSION

152 153

In the case of environmental contamination

154

with radioactive material, the mitigation approach

155

can use the guidance of MARSSIM manual, where

156

the survey of area classification in the site

157

investigation process for conducting the radiation

158

survey is shown in Figure 2 [14].

159 160

(3)

The survey process was carried out in a

161

walkover survey method, where the output from this

162

activity was the data about type and level of

163

radiological from the contaminants. The results of

164

the survey can also be used to classify

165

contamination areas, work paths of workers in

166

decontamination activities and to recommend the

167

activities and tools, as well as analytical methods to

168

be used in the decontamination activities.

169 170 171

172

Figure 2. Survey classification process of MARSSIM manual 173

[14].

174 175

From the results of walkover surveys that

176

have been carried out, it has been obtained such as

177

the type and level of radiology of the area of

178

contaminated soil. The type of radionuclide was

179

137Cs which is allegedly come from radioactive

180

sources which spread out over the area. There are

181

some hotspots were found at that location, and the

182

dose exposure in these area is about 149 µSv/hour

183

[15]. The hotspot is then got pay attention to be

184

chosen as the center or target of the decontamination

185

activity plan.

186

187

The results of the analysis of coring activities

188

shown as slightly strange result if the results are

189

intended as radiologic contamination at the surface

190

of the soil. At the location, high activity has been

191

obtained at the ground surface in one point, but at

192

another point there is a high activity in certain

193

depths in the soil was obtained. This showed that

194

contamination occurred at the location with 137Cs

195

radioactive material is an intentional action, and this

196

behavior can be suspected of an attempt to hide

197

radioactive material in the area by an irresponsible

198

person.

199

200

The decontamination activity is carried out,

201

firstly by peeling off the soil layer that has been

202

contaminated by 137Cs. The results obtained from

203

this activity, contaminants can be removed from the

204

incident area and a significant reduction in activity

205

concentration in the contaminated area occurred

206

(from 149 to 0.3-0.75 µSv/hour) [16]. The drums

207

contained contaminated soil and then successfully

208

transported to the interim storage facilities at

209

Serpong Nuclear Center.

210

211

The results of peeled soil surface were then

212

put into a 100L drums and the investigation of the

213

distribution of intrusions of 137Cs into sub-soil layer

214

will be identified by coring works in the area of

215

contaminated soil as shown in Figure 3. Some

216

hundred quantity of drum is obtained, after which

217

the drums are brought to the interim storage facility

218

in BATAN for further treatment, Figure 4.

219

220

221

Figure 3. Activities of decontamination and investigation in the 222

land area: (a) soil peeling and (b) coring of soil layer 223

224

a

b

(4)

225

Figure 4. Radiation workers with drums resulting from the 226

surface soil decontamination activities 227

228

The next step after decontamination activity is

229

management plan of the contaminated soil with the

230

treatment works of contaminated soil to reduce the

231

quantity of waste volume that has accumulated in

232

the interim storage facility. If this step is successful,

233

the result can reduce the amount of contaminated

234

soil waste, and also it will reduce the use of drums

235

contained contaminated soil, so that the capacity of

236

interim storage facilities would be increased.

237 238

The strategy to reduce the volume of

239

contaminated soils can be shown in Figure 6.

240

Drums which contain the contaminated soil are

241

separated, the drums which have levels of below the

242

allowable activity concentration and with the drums

243

that have a higher activity concentration.

244

245

Figure 6. Strategy to reduce volume of contaminated soil from 246

decontamination results 247

248

If drums with a low activity concentration is found,

249

then the contaminated soil can be removed from the

250

drum and placed in a location that does not need to

251

be controlled anymore or can be released into the

252

environment after got the approval from Bapeten.

253

Whereas for the drums that are still classified as

254

having a high activity concentration, the soil

255

"needs" to be sorted out again. The soil that have a

256

low activity concentration level can be included in

257

the soil that can be cleared or release them into

258

environment. While parts of the soil which has

259

contain a high concentration activity of 137Cs will be

260

extracted with a chemical agent. The volume

261

reduction method of this works is an ex-situ method,

262

will do at the facility of interim storage.

263

264

Soils which are still high in concentration

265

activity will be further processed. Furthermore,

266

some processing techniques by removing 137Cs from

267

the soil will be studied. Efforts to extract 137Cs from

268

the contaminated soil are carried out by leaching

269

137Cs from the soil sample. Radiocesium would

270

strongly bound to the soil due to the existence of

271

mineral flakes in the contaminated soil structure

272

[17,18]. The presence of minerals in the soil

273

composition could bind the 137Cs firmly [19-22] so

274

an effort to desorption 137Cs from the minerals is

275

needed. Removal of 137Cs from contaminated soils

276

can be done through wet and/or dry processes,

277

where each of the processes has the advantages and

278

disadvantages. But the main thing from this activity

279

is that the principle of radioactive waste treatment

280

must not be ignored, that is the reduction volume of

281

treated waste.

282 283

Since 137Cs is the primary cause of soil

284

contamination in a land at South Tangerang, and

285

recent the contaminated soil is storing at the facility

286

of interim storage, 137Cs radioactive management

287

has now become a priority. As the previous

288

mention that decontamination of 137Cs contaminated

289

soils can be done through wet and/or dry processes.

290

In the next paragraph a brief discussion of some

291

processes that possible to be carried out to manage

292

contaminated soil wastes. In some of the literature,

293

the first stage to manage contaminated soil waste is

294

an attempt to remove 137Cs from the contaminated

295

soil [23-25]. Several methods have been carried out

296

using leaching solutions to remove 137Cs from

297

contaminated soil. And then the solution from the

298

results of the radioactive leaching is processed with

299

a variety of absorbent materials, both derived from

300

natural materials, organic or modified materials, or

301

can also be done by using other methods.

302

303

In fact, the most effective method to reduce

304

the negative effects of radiation in contaminated soil

305

is by removing 137Cs from the contaminated soil.

306

(5)

With regard to the easy operation and volume

307

reduction processes for the radioactively

308

contaminated soil, the extraction process might

309

become an effective strategy for treatment of

310

contaminated soil from the decontamination results.

311

312

Shibata et.al. [26] conducted a study on 137Cs

313

decontamination by flushing with water to the

314

simulation of 137Cs contaminated soil. The results

315

show that only about 7% of 137Cs are extracted by

316

water and the remaining 90% of 137Cs is still

317

strongly bound in soil samples. Then based on

318

particle size, a sieving equipment was used to sort

319

the contaminated soil. The results showed that most

320

of the 137Cs had accumulated in soil samples with

321

particle size of about 425 μm, which was the

322

particle size of minerals in the soil (vermiculite). It

323

is predicted that 137Cs are absorbed at the frayed

324

edge of vermiculite. The extraction ratio will

325

increase along with a longer processing period.

326

Yanaga and Parajuli [21,24], conducted an

327

extracting 137Cs from solution by contacting

328

artificially contaminated soil with KI solution, and

329

as a comparison they also carried out soil washing

330

with demineralized water. The results show that the

331

process of removing of 137Cs from contaminated soil

332

will increase along with the increase in the

333

concentration of KI was given into the solution.

334

Increasing the processing time does not increase the

335

extracted 137Cs. It is supposed due to the movement

336

of 137Cs in the soil into the mineral site, so that the

337

bond that occurs between 137Cs with minerals

338

becomes stronger. Whereas the extraction with

339

water only gives a little 137Cs which are released

340

into the solution as shown in Figure 7.

341

342

Figure 7. Variation of extraction time versus 137Cs removal 343

from solution [21]

344 345

Hirose [23] extracted 137Cs from

346

contaminated soil using Milli-Q water, Ammonium

347

acetate and acetic acid solutions. The results of

348

overall extracted fractions of 137Cs using the three-

349

step sequential extraction process could only

350

produce less than 30% of 137Cs that were removed

351

from solution. There is an interesting study

352

conducted by Kim et.al [27] to develop a system to

353

washing the contaminated soil. To remove 137Cs

354

from contaminated soil they use many chemical

355

agents, such as H2O, citric acid, citric acid+HNO3,

356

NH4NO3, FeCl3, (COOK)2⋅H2O, (NH4)2SO4,

357

H2C2O4⋅H2O, NaOH, and Na3PO4 solutions. The

358

obtained results showed that the H2C2O4⋅H2O

359

chemical agent has provided the highest efficiency

360

value for removal 137Cs from the solution, where the

361

efficiency was almost to 50%. Oxalic acid will

362

form a stable metal-complex with 137Cs, and

363

dissolves hydroxides. Besides that the H2C2O4⋅H2O

364

also reasonable in price, so H2C2O4⋅H2O is an

365

optimal chemical agent for washing the soil. The

366

contaminated soils that has been extracted 137Cs then

367

can be classified as soil having low radioactive

368

content. But if the soil still has a high radioactive

369

activities, then the soil will be treated with another

370

method, such dry method to avoid increasing a

371

secondary wastes. The previous mention are some

372

methods for removing 137Cs from contaminated soil.

373

The 137Cs extracted solution is then processed in

374

several of ways which can make the activity in the

375

solution reduced.

376 377

To reduce the Cs-137 concentration on the

378

treated water using some methods such as

379

adsorption/ion exchange, electrochemical, and

380

biomaterials processes are being develop intensively

381

through investigating works. Among them some

382

processes are the most attractive for

383

decontaminating 137Cs from solution, were

384

adsorption/ion exchange, and electrochemical

385

processes with considerable removal capabilities.

386

These decontamination strategies research works

387

resulted the large proportion of the publications. For

388

the next topic of discussion mainly address to the

389

attractive investigation works in creating materials

390

for adsorption processes. The adsorption process is

391

usually not a stand-alone process, it is a complex

392

process involving the physical and chemical

393

reactions, although ion exchange is a special kind of

394

chemical adsorption. In the most cases, to improve

395

the capability and selectivity of the adsorption

396

materials, they are always modified or

397

functionalized with an ion-exchanger. As a result,

398

adsorption and ion exchange functions usually

399

occurred simultaneously during a typical adsorptive

400

removal process. Based on the origin of the

401

materials, variations in the composition of the

402

absorbent material will determine the mechanism

403

that dominates when it was used to process 137Cs.

404

Adsorption materials generally could be divided into

405

(6)

three categories, there are carbonaceous, clay, and

406

biomass materials/biosorbents.

407 408

Carbonaceous materials or activated carbon,

409

this material is a pioneer of investigation of the

410

adsorptive materials for the removal of various

411

contaminations (heavy metals or radionuclides)

412

from aqueous solutions. Due to their good active

413

adsorption sites and has special porous structure

414

(extremely large specific area), this material has

415

performed satisfied to its capability in the

416

adsorption of organic and inorganic contaminants.

417

To enhance their abilities to be more selective for

418

certain metal ion or radionuclide, some chemical

419

additives often to be added to the carbonaceous

420

materials [28]. Carbonaceous materials has the low

421

stability and selectivity properties towards the target

422

metal ions, so they require the modification/

423

immobilization with a selective inorganic ion

424

exchanger on their large surface of activated carbon.

425

This process can not only enhance the adsorption

426

capacity but also improve their stability and

427

selectivity properties. Some researchers have

428

conducted research on modification of activated

429

carbon materials, but these two studies will be very

430

interesting to be noted. They modified the natural

431

materials came from nature such as of rice hull and

432

areca nut where the surface of the material was

433

immobilized with nickel hexaxyanoferrate (NiHCF)

434

[29], or potassium nickel hexaxyanoferrate

435

(KNiHCF-GAC) to absorb Cs ions in solution [30].

436

The results show that these material has become

437

better in their performance for absorbing Cs ions in

438

solution, and the maximum adsorption capacity

439

reaches 163.9 mg/g for KNiHCF-GAC. Many

440

results of research have been reported from the use

441

of carbonaceous material to absorb metal ions or

442

radionuclides, but the disadvantage of this material

443

is the stability of the properties of the final product

444

is still rough. The process of making these materials

445

to achieve as a standardized product still needs to be

446

considered. And many more absorbent materials

447

made from activated carbon, such as those made as

448

carbon nanotubes, but this discussion is not

449

mentioned.

450 451

Other natural materials that got pay attention

452

for radionuclide decontamination such as 137Cs are

453

clay material as electrochemical process. This

454

natural material is very attractive because of its

455

good ion exchange capability, where ions such as

456

Na, K, Ca, Mg exist at their exchange site. Metal

457

ions such as 137Cs in solution will replace their

458

position in the clay material and then the sorption of

459

radionuclides can occur into the material. Many clay

460

materials have been intensively studied, such as

461

zeolite, bentonite, kaolinite minerals as absorbent

462

materials to absorb 137Cs, both for treatment

463

processing purposes and as buffer material in the

464

near surface disposal facilities [31,32]. But for

465

decontamination activities, these materials need to

466

be modified previously to increase or improve their

467

absorption capacity (cation exchange capacity /

468

CEC). Modification of clay material by using

469

nickel [33], or by pillarization of clay

470

(montmorillonite and geothite materials) before

471

used as absorbent [34]. Since clay materials have

472

alumina octahedral sheet in their structure

473

(especially for bentonite and zeolite), the lattice has

474

unbalance charge due to the Al-octahedral sheet

475

give the excess of negative charge. If any cation

476

present in solution (such as 137Cs), it could be

477

counterbalance to this negative charge in order to

478

neutralization the compound [35]. Figure 8 is the

479

illustration of bentonite structure.

480

481

Figure 8. The structure of bentonite mineral [35]

482 483

Naturally clay materials are widely used to

484

providing the alternative materials choice for

485

decontamination of 137Cs in the soil. Another

486

advantage by using the natural material is, this

487

natural material is easily available and attractive in

488

prices and easily bound to the immobilization

489

material of radioactive waste package.

490

491

Biomass material (as biosorbents) used to

492

absorb metal ions has also attracted the attention to

493

the researchers. Cross linking between persimmon

494

waste and sulfuric acid was used by Pangeni et al

495

[36] to eliminate 137Cs from the solution. The

496

adsorption capacity towards 137Cs has become

497

greatly increased after the used of this process.

498

There is also the creation of walnut shell and pine

499

cone for absorbing 137Cs by functionalizing with

500

NiCHF and Fe (III) HCF which are useful for

501

increasing the absorption capacity of materials to

502

metal ions. The advantage of this material is, as

503

materials derived from carbonaceous materials, the

504

management of spent material is easy. The

505

(7)

combustion process with an incinerator unit can

506

complete the volume reduction process, this

507

material will be reduced to almost 91.9% in volume

508

(at 500o C for 2 h).

509

510

Because the materials as previously

511

mentioned have the property of low capacity,

512

stability and small in size. The using of other

513

materials with more sophisticated technology

514

(advanced materials) can also be considered to be

515

created to eliminate 137Cs from the environment,

516

such as the use of graphene-like layers that are

517

chemically durable and resist to radiation emission.

518

The use of Prussian blue nano particles (PBNP)-

519

incorporated with polyvinyl alcohol (PVA) to form

520

a composite of nano particles [37], or to create a

521

unique structural properties of the titanate nanotubes

522

also promised their use to absorb 137Cs from solution

523

[38]. And there are many more materials in the form

524

of composite nano particles prepared by researchers

525

to absorb 137Cs from solution, however we do not

526

discussed it yet. Meanwhile, an important role in

527

the adsorption process of clay materials plays both

528

ion exchange and electrostatic interactions. The

529

modification and combination of these materials are

530

of considerable concern and necessity to improve

531

their adsorption capacity increased. Removal of

532

137Cs from the solution by using an adsorption and

533

ion exchange methods is summarized in Table 2

534

[26]. The leaching solution from contaminated soil

535

containing 137Cs is then processed with materials as

536

discussed above or processed it with an evaporation

537

unit, before finally the remaining solution from

538

processing results can be released into the

539

environment.

540 541

542 543

After the management of contaminated soil

544

waste is carried out by the wet method, we now

545

discuss the contaminated soil waste is treated in a

546

dry methods. The electrokinetic method will be

547

discussed in this part. Yu has conducted his

548

research on decontamination of 137Cs using the

549

electrokinetic method [39]. He conducted this

550

research to test the feasibility of electrochemical

551

methods removing 137Cs from soil inspired by the

552

Chernobyl accident. Electrokinetic decontamination

553

has a few unique advantages. It works by electro-

554

osmotic effects, the removal of contaminants by soil

555

flushing in where pressure-driven flow is so low

556

such in low-permeability soils as clays materials.

557

The location of the electrodes will determine the

558

electric field lines, and it causing the ions to move

559

along the electric field lines to reach a high level of

560

flow direction control. Electromigration of charged

561

species independent to soil pore size and thus it

562

applies equally to coarse and fine-grained soils.

563

This method has been widely used to remove

564

heavy metals from the soil. The experiment has used

565

a compartment model with a one-dimensional

566

electrokinetic process on the soil. To decontaminate

567

contaminants from the soil, electrokinetic soil

568

technology applies a low-level direct current to the

569

contaminated soil by placed the electrodes in the

570

soil samples. And according to their charge,

571

contaminants travel toward the cathode or anode.

572

The contaminants are then deposited at the

573

electrodes. The mass transfer rate can be divided

574

into four components. One is caused by pressure-

575

driven advection, by dispersion/diffusion, by ionic

576

migration and by electro-osmosis. The components

577

are obtained from the difference between mass

578

fluxes into the compartment and the fluxes out of

579

the compartment. The electrical potential appearing

580

in the mass flux expressions for electromigration,

581

and electro-osmosis might be related to the electric

582

current by charge flux of both diffusion and ionic

583

migration of all charged species. Large forces may

584

restore the charge balance on a time-scale much

585

faster than any other in the system. By assuming

586

that the solution outside the electric double layer is

587

electrically neutral, which means that there is no net

588

charge accumulation in each compartment, the

589

electric current will be constant along the one-

590

dimensional medium. Figure 9 is a schematic

591

diagram of the electrokinetic process used to extract

592

metal ions/radionuclides from the soil.

593

594

Figure 9. Schematic diagram of the electrokinetics soil 595

decontamination process [39]

596 597

The soil is flushed at a low velocity with

598

water constantly. The flushing is used to remove the

599

radionuclide that accumulates at the cathode. The

600

(8)

soil then was given a 100 V DC voltage using 2

601

inert electrodes. The application of the DC voltage

602

to soil causes the evolution of oxygen at the anode

603

and the evolution of hydrogen at the cathode

604

occurred. The effect of electrokinetic processes on

605

the soil also depends on the sorption and diffusion

606

parameters of radionuclides in the soil.

607

608

High sorption and slow diffusion properties

609

of the soil, makes radionuclides cleaning up process

610

take a long time, a few months. Increasing DC

611

current on the soil sample can reduce the treatment

612

time. In materials that have good absorption ability

613

such as bentonite, the treatment time will be longer.

614

Figure 10 shows the typical of remaining fraction of

615

137Cs after treatment by using electrokinetic method

616

[39]. A high of Kd value will cause the treatment

617

time of 137Cs much longer.

618

619

Figure 10. Remaining fraction of activity during the treatment, 620

with variation of Kd values (m3kg-1), modification from 621

ref.[39].

622 623

Likewise the presence of organic matter in the

624

soil can reduce the decontamination ability of

625

electrokinetic devices. Radionuclides will be

626

associated with organic matter in the soil so that the

627

effect of soil pH is also important. Increasing pH in

628

the soil causes the functional groups in organic

629

matter to do the protonization processes, and

630

radionuclides absorbed in organic matter hardly. In

631

the electrokinetic decontamination process at least

632

there will be affected by several parameters such as

633

the activity of metal ion concentration in the soil,

634

electric current density, electrode distance, flow of

635

washing solution (chemical agent), type of soil

636

sample, treatment time, soil pH etc. Manipulation of

637

all parameter values will obtaine the optimal

638

conditions of the electrokinetic process to be able to

639

decontaminate metal ions or radionuclides such as

640

137Cs from the contaminated soils.

641 642

In the course of time, this method has been

643

studied more advance by Cameselle [40], Shahrani

644

[41] and Mao [42]. Then to improve the

645

decontamination results of 137Cs, electrokinetic

646

method is combined with other methods such as

647

water flushing [43], acid enhanced [44] and

648

electodialytic [45].

649

650

From the study, there is an interesting information,

651

where soil from the clean-up resulted is processed

652

by classifying it based on their particle size. This

653

method is very interesting to use as an initial stage

654

of decontamination proses of contaminated soils

655

before other methods are used to extract 137Cs from

656

contaminated soils. It is known that 137Cs will be

657

absorbed in soil particles, and it was believed that

658

137Cs will bind stronger in the smaller particle sizes

659

of soil. Where the smaller the particle, the stronger

660

137Cs are bound due to in the smaller particle sizes

661

contain many mineral fragment. The 137Cs

662

deposited on soils with tightly bound at the

663

exchangeable site of the soil. Kim et.al. used a

664

sieving method based on the differences in particle

665

size of the soil, contaminated soil was managed

666

where 3 sieve sizes were <0.063, 0.063 <x <0.1,>

667

0.1 mm was used [27]. Particle size distribution

668

used for the research is highly dependent on the

669

characteristics of the soil at the contaminated

670

location. Kim took the soil samples with particle

671

size > 0.063 mm for treatment, because the soil with

672

particle size <0.063 mm contained high

673

concentration of 137Cs and then was immediately

674

immobilized.

675

676

For the experiment, Kim et.al. taken 50 drums

677

were selected based on the surface effective doses

678

rate of waste drums. There are about 7% of drums

679

having a surface effective dose rate exceed from

680

0.05 mR/h, 33% of drums below 0.02 mR/h, while

681

the majority of drums (60%) are in the range

682

between 0.02 - 0.05 mR/h. About 10 kg of

683

contaminated soil is taken from each drum, and then

684

dried before the sieving process based on their

685

particle size. The radioactive Cs target as a part of

686

soil that used are have the concentration level of >

687

400 Bq/kg. Radiometric measurement of soil

688

samples used an MCA units. The soil sample is first

689

dried for more than a week before being used for the

690

experiments. Soil that has dried and then classified

691

with a sieving unit into 3 particle sizes for 30

692

minutes. The results of the particle size

693

classification analysis of contaminated soil are

694

shown in Table 3.

695

(9)

696 697

The radioactive concentrations of 137Cs in the parts

698

of contaminated soil were higher than the target

699

concentration level, especially in the drums with

700

has surface effective dose > 0.05 mR/h. The soil

701

with particle size with range between 0.063 to 1.0

702

mm provides the largest portion in soil particle size.

703

It is easier to decontaminate a soil having a particle

704

size larger than 1.0 mm, the soil particles having

705

sizes that range from 0.063 to 1.0 mm is selected to

706

be washed with water to take the 137Cs

707

contaminant. The smaller size of the soil particle

708

resulted the higher radioactive concentration emitted

709

from soil particles. Soil that has the particle size

710

smaller than 0.063 mm and then to be processed

711

with compaction method to reduce their volume

712

before to immobilized it. By using water washing

713

method, the fine particles (<0.063 mm) gave

714

extremely low in removal efficiency of 137Cs.

715

Contaminated soil is then washed by using the

716

chemical agents such as citric acid, citric acid +

717

HNO3, NH4NO3, FeCl3, (COOK)2⋅H2O,

718

(NH4)2SO4, H2C2O4⋅H2O, NaOH, and KI solutions

719

[22,39]. All the chemical agents were compared

720

their ability to remove 137Cs from contaminated soil.

721

The use of oxalic acid and KI chemical agents has

722

given a high removal efficiency value to

723

decontaminate 137Cs from the soil. Around 50% of

724

137Cs can be taken out from the soil contaminated by

725

both chemical agents. What is more, the price of

726

both chemical agents is reasonable. Solution from

727

extraction resulted which is containing the 137Cs

728

concentration is then treated by using one of the

729

absorbent material as previous mentioned, while the

730

absorbent can be advance processed in various

731

ways, such as compaction, incineration (combustion

732

then ash are immobilized), immobilization and

733

polymerization (when using organic resins as

734

absorbents).

735

736

The final result of this study is a proposal of

737

the strategy to treat appropriately the contaminated

738

soil waste from the land in South Tangerang. Here,

739

we suggest 3 proposals to be considered, one of

740

which is hopely the most suitable method to be

741

applied to manage the waste of contaminated soil

742

from South Tangerang,

743 744

In the first proposal, 137Cs contaminated soil

745

waste is treated by separation method according to

746

their particle size. Three sizing particle sizes are

747

object of this process. Only soil with particle size

748

greater than 0.063 mm will be further processed.

749

Advanced treatment by using wet method

750

(chemically), where contaminated soil (with particle

751

size greater than 0.063 mm) is contacted with

752

chemical agents such as KI or H2C2O4 to remove

753

137Cs from the soil into solution. The solids part

754

which are obtained are expected to be low in 137Cs

755

concentration, so they can be released into the

756

environment. The obtained liquid is then processed

757

again by absorption method use the material that has

758

selectively absorption property to 137Cs. The liquid

759

which “clean” from 137Cs or a low concentration of

760

137Cs can then be released into the environment, or

761

used as a mixing fluid in the immobilization

762

process. The solids which are rich with 137Cs are

763

then immobilized by compaction and cementation

764

methods becomes as waste packages. The waste

765

package is then sent to a long-term storage facility

766

(LTSF). The flow chart of proposal 1 is shown in

767

Figure 11. We do not use HNO3 or H2SO4 to extract

768

137Cs from soil due to avoid of strong acid in the

769

next processes.

770

771

In the second proposal, we propose the

772

contaminated soil is treated with a dry method. In

773

the beginning of the treatment process is similarly as

774

did in the first proposal, where the contaminated soil

775

is separated based on particle size. But in the next

776

process, the accumulation process of 137Cs in the

777

soil is done by dry method (electrokinetic method),

778

where the soil which has a particle size > 0.063 mm

779

is put into a column. The column and then is given a

780

DC electric voltage and a flush water to maintain

781

soil pH.

782

(10)

783

Figure 11. The first proposal (wet processes) 784

785

Based on the different in electrical voltage,

786

the metal ion as a positive charge (such as 137Cs)

787

will move and be deposited at the cathode, and vice

788

versa to anode. To make the catode saturated with

789

137Cs, the long treatment time required. And then the

790

cathode immobilized by compacting or cementing.

791

Soil that was contaminated then becomes less

792

contaminated, and can be released into the

793

environment or applied as the cover of waste

794

package on the LTSF. The flow chart of the

795

processes is shown in Figure 12.

796

797

Figure 12. The second proposal (dry process) 798

799

As a comparison of the two kinds of

800

treatment processes, the treatment method in the

801

first proposal is relatively more familiar and has

802

more proven technology compared to the process

803

which is carried out in the second ones. In the first

804

treatment method, the treatment time also looks

805

relatively faster and the material used is more

806

reliable and feasible than the materials in the second

807

proposal. Processing with electrokinetic method will

808

require more lot of energy, longer treatment time,

809

more complicated process, and the technology has

810

not been proven (relatively expensive). The use of

811

the treatment method proposed in the first proposal

812

is more promising to be applied in the near future.

813

Affected parameters must be obtained completely so

814

the engineers can design the required processing

815

units. However good mastery of electrokinetic

816

methods can do the cleanup activities in situ.

817

818

And the last proposal -perhaps this is the

819

easiest method to do- is the compaction method

820

applied to all drums containing the remediated soil.

821

The 100L drum is compacted in the inside of the

822

200L drum, then the 200L drum contained the

823

results of the compaction will be sent to the long-

824

term storage facility

825 826

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