Tellurium Distribution and Speciation in ... - ACS Publications

Subscriber access provided by UNIVERSITY OF WISCONSIN-MILWAUKEE

Article

Tellurium Distribution and Speciation in Contaminated Soils from Abandoned Mine Tailings: Comparison with Selenium Hai-Bo Qin, Yasuo Takeichi, Hiroaki Nitani, Yasuko Terada, and Yoshio Takahashi Environ. Sci. Technol., Just Accepted Manuscript • Publication Date (Web): 20 Apr 2017 Downloaded from http://pubs.acs.org on April 21, 2017

Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

Environmental Science & Technology is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

Page 1 of 35

Environmental Science & Technology

1

Tellurium Distribution and Speciation in Contaminated Soils from Abandoned

2

Mine Tailings: Comparison with Selenium

3 4

Hai-Bo Qin,*,†,‡ Yasuo Takeichi,§ Hiroaki Nitani,§ Yasuko Terada,∥

5

and Yoshio Takahashi*,‡

6

†

7

Chinese Academy of Sciences, Guiyang 550081, China

8

‡

9

University of Tokyo, Hongo 7-3-1, Bunkyo-ku, Tokyo 113-0033, Japan

State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry,

Department of Earth and Planetary Science, Graduate School of Science, The

10

§

11

Organization (KEK), 1-1 Oho, Tsukuba, Ibaraki 305-0801, Japan

12

∥

13

Sayo-cho, Sayo-gun, Hyogo 679-5148, Japan

Institute of Materials Structure Science, High Energy Accelerator Research

Japan Synchrotron Radiation Research Institute (JASRI), SPring-8, 1-1-1 Kouto,

14 15 16 17 18 19

Corresponding authors:

20

*Phone: +86-85-85895787; fax: +86-851-85891334; e-mail: [email protected]

21

(Hai-Bo Qin)

22

*Phone: +81-3-5841-4517; fax: +81-3-5841-8791; e-mail: [email protected]

23

(Yoshio Takahashi)

24 1

ACS Paragon Plus Environment


25

ABSTRACT

26

The distribution and chemical species of tellurium (Te) in contaminated soil were

27

determined by a combination of micro focused X-ray fluorescence (µ-XRF), X-ray

28

diffraction (µ-XRD), and X-ray absorption fine structure (µ-XAFS) techniques. Results

29

showed that Te was present as a mixture of Te(VI) and Te(IV) species, while selenium

30

(Se) was predominantly present in the form of Se(IV) in the soil contaminated by

31

abandoned mine tailings. In the contaminated soil, Fe(III) hydroxides were the host

32

phases for Se(IV), Te(IV), and Te(VI), but Te(IV) could be also retained by illite. The

33

difference in speciation and solubility of Se and Te in soil can result from different

34

structures of surface complexes for Se and Te onto Fe(III) hydroxides. Furthermore, our

35

results suggest that the retention of Te(IV) in soil could be relatively weaker than that of

36

Te(VI) due to structural incorporation of Te(VI) into Fe(III) hydroxides. These findings

37

are of geochemical and environmental significance for better understanding the

38

solubility, mobility, and bioavailability of Te in the surface environment. To the best of

39

our knowledge, this is the first study reporting the speciation and host phases of Te in

40

field soil by the µ-XRF-XRD-XAFS techniques.

41

2


Page 2 of 35

Page 3 of 35


42

TOC/Abstract Art

43

44 45

3



46

INTRODUCTION

47

Tellurium (Te) has attracted increasing attention due to its wide industrial

48

applications such as improving optoelectronic and thermal properties of steel and glass,

49

developing new materials (e.g., CdTe thin-film solar panels), as well as producing

50

fluorescent probes.1-4 As expected, the expanded use of Te can lead to environmental

51

pollution and induce acute and chronic Te poisoning to human (e.g., the degeneracy of

52

liver and kidney).2,5 The Occupational Safety and Health Administration (OSHA) has set

53

the permissible exposure limit for workers to Te compounds in the workplace as 0.1 mg

54

m-3 over an 8-hour workday.5 In addition, radiotellurium including 127mTe, 129mTe, 131mTe,

55

and 132Te may be released into the environment in the case of the nuclear accidents (e.g.,

56

Fukushima Daiichi Nuclear Power Plant accident in March 2011), which are severely

57

harmful to human health through inhalation and ingestion of contaminated crops.6,7

58

Tellurium is one of the least abundant elements in the earth’s crust, but it is

59

considerably enriched in marine ferromanganese crusts.1,8,9 The environmental fates and

60

biogeochemical behaviors of Te are still poorly known, although its chemical and

61

physical properties are generally considered to be similar to those of selenium (Se) in the

62

same Group 16 of the periodic table. It was recently suggested that the distribution

63

behavior between Te and Se is significantly different in a laboratory soil-water system,10

64

but similar studies in natural systems are lacking due to extremely low Te concentration

65

in geological, environmental, and biological samples.

66

In the natural environment, Te occurs in several oxidation states (-II, 0, IV, and VI)

67

both in organic and inorganic forms.1,2 Oxyanion tellurate (Te(VI)) is the predominant

68

species of Te in hydrosphere.9,11 Tellurite (Te(IV)) is another soluble form, but its toxicity 4


Page 4 of 35

Page 5 of 35


69

is 10-fold higher than Te(VI).12 Te(IV) is toxic to bacteria even at a low concentration, yet

70

some Te-resistant bacteria that can reduce Te(IV) and Te(VI) to elemental Te(0) have

71

been found in nature.13-15 Elemental Te(0) is insoluble in water, and thus has less mobility

72

and toxicity. These microorganisms could be used to relieve excessive Te in aquatic

73

environment via microbial reduction from Te oxyanions to precipitated Te(0).14,15 Various

74

telluride minerals such as calaverite (AuTe2), rickardite (Cu7Te5), and sylvanite

75

(Ag3AuTe2) often coexist in gold (Au) deposits,1,16 while organic forms of Te (e.g.,

76

dimethyl telluride, telluro-cystine, and telluro-methionine) are mainly related to

77

biological activities.1,2 Thus, Te speciation is crucial for better understanding its

78

distribution, bioavailability, toxicity, and mobility in the environment, because different

79

forms show the unique biogeochemical properties.

80

However, research regarding the distribution and chemical speciation of Te in field

81

soil has been scarcely attempted, owing to challenging analytical methods for Te

82

speciation.17 In the past few decades, X-ray absorption fine structure (XAFS) method that

83

consist of X-ray absorption near edge structure (XANES) and extended X-ray absorption

84

fine structure (EXAFS) spectroscopy has been widely utilized to nondestructively

85

identify metal(loid)s speciation in solid samples.10,18-21 Nevertheless, Te speciation in

86

common soil containing low Te content could not be determined by XAFS technique with

87

reasonably high detection limit. Furthermore, the absorption energies of the K-edge and

88

LIII-edge of Te are 31814 eV and 4341 eV, respectively, but both energies are

89

inaccessible at many traditional XAFS beamlines in the world. The consequence is that

90

synchrotron based XAFS measurement is difficult to be carried out even if Te content in

91

solid sample is high enough to collect the XAFS spectra of Te. 5



92

The Kawazu Mine located at Shimoda City, Shizuoka Prefecture, Japan, is famous

93

for the occurrence of Au-Ag-Te-Mn veins, where a unique Te mineral named Kawazulite

94

(Bi2Te2Se) has been discovered.22-24 However, Te level and speciation in the soil around

95

Kawazu Mine are largely unknown. In this study, we have investigated Te concentration

96

in the soils from abandoned Kawazu Mine tailings. Furthermore, the chemical speciation

97

and host phases of Te in the contaminated soil have been identified using powerful micro

98

focused XAFS (µ-XAFS), X-ray fluorescence (µ-XRF), and X-ray diffraction (µ-XRD)

99

techniques. The aims of this study were (i) to clarify the distribution and speciation of Te

100

in the contaminated soil and (ii) to further provide valuable insights into the migration,

101

bioavailability, and potential risk assessment of Te in the surface environment.

102 103

MATERIALS AND METHODS

104

Sample Collection and Preparation. The soil samples were collected around

105

Hinokizawa pithead (34.41° N, 138.55° E) of Kawazu Mine (Figure S1), details on its

106

geology and ore deposit are given in the Supporting Information (SI). In the laboratory,

107

soil samples, free of plant roots and detritus, were air-dried and then ground with an agate

108

mortar for chemical and speciation analysis. Furthermore, a thin section of the soil

109

sample that has been firstly sieved to eliminate large particles ( 4.5) were found in the systems of both Te(IV) and Te(VI) adsorption on ferrihydrite and goethite under neutral pH (Figure 5), suggesting that Fe(III) 16


Page 16 of 35

Page 17 of 35


345

hydroxides have high affinities (> 98.4% of Te was adsorbed) for both Te(IV) and Te(IV)

346

under common environmental conditions. In terms of Te species, the logKd levels of

347

Te(IV) were clearly greater than those of Te(VI) adsorption on ferrihydrite and goethite

348

except for strong alkaline environments (e.g., pH=11), implying that Te(IV) seems to be

349

readily adsorbed by Fe oxides. Hein et al.9 suggested that Te(IV) in seawater is

350

preferentially scavenged by FeOOH at the surface of ferromanganese crust, which results

351

in the fact that the thermodynamically more stable Te(IV) is less abundant by factors of 2

352

to 3.5 than Te(VI) in ocean water. In addition, larger logKd values were observed for

353

ferrihydrite relative to goethite in either Te(IV) or Te(VI) system, which is probably

354

ascribed to the higher Brunauer-Emmett-Teller surface area for ferrihydrite (330 m2 g-1)

355

than that for goethite (20 m2 g-1).40,41 These results are consistent with the fact that Fe(III)

356

hydroxides are the host phase of Te in solid samples demonstrated by spectroscopic

357

methods, which is highly reasonable because oxyanions are readily adsorbed by

358

positively-charged Fe(III) hydroxides.

359

In contrast, lesser degree of Te adsorption was found for illite relative to iron oxides

360

regardless of Te species and pH condition. The negatively-charged illite, a 2:1 layer type

361

clay mineral, basically exhibit three types of sorption sites: sites on the basal planar,

362

interlayer sites, and hydroxyl groups on the sheet edges. The first and second sites exhibit

363

negative charge, which are specifically responsible for pH-independent adsorption of

364

cations such as cesium.42,43 However, sorption on the hydroxyl group sites is

365

pH-dependent because of its amphoteric nature, which is speculated to be the most

366

relevant adsorption mechanism for anions. Recently, the complexation models involving

367

mechanism related to surface functional groups have been successfully utilized to 17



368

simulate the adsorption of Se on illite.44,45 Furthermore, much larger amounts of Te(IV)

369

were adsorbed by negatively-charged illite compared with Te(VI) under a relatively lower

370

pH (Figure 5). This is likely to be partially explained since the possible species of Te(IV)

371

such as TeO-OH+ and/or H2TeO3 show some cationic properties, while Te(VI) is mainly

372

present in the forms of anionic H2TeO4 and/or HTeO4- under low pH conditions (Figure

373

S4).31,32 These results confirm the observation that more Te(IV) was found in the hotspots

374

(e.g., Spots 6 and 8) containing more illite in the contaminated soil from abandoned

375

tailings by the µ-XRF-XRD-XAFS technique.

376 377

Comparison between distribution and speciation of Te and Se in soil. For comparison

378

with the distribution and speciation of Te, a similar data set for Se was simultaneously

379

obtained in the soil thin section (e.g., Figures 1D and 1E). The distribution of Se was

380

almost identical to that of iron according to the µ-XRF mapping data (Figure S5), as

381

shown for Te distribution pattern in the same soil grains (Figure 1). Combining with

382

µ-XRD results for these particles (Figure S3) suggests that Fe(III) hydroxides can be the

383

host phases for Se and Te in the soil contaminated by waste tailings. This finding is

384

confirmed by the fact that added Te and Se are mainly associated with Fe(III) hydroxides

385

in incubated soil in the laboratory experiment.10

386

Selenium K-edge µ-XANES spectra for Se hotspots were very similar to that of

387

NaHSeO3 (Figure S5), suggesting that Se(IV) is the predominant form in the

388

contaminated soil from abandoned tailings, which is in line with the observation that

389

Se(IV) is one of major species in soil developed on reclaimed mine lands.46 However, a

390

mixture of Te(VI) and Te(IV) was present in the same soil particles obtained from Te 18


Page 18 of 35

Page 19 of 35


391

K-edge µ-XANES results (e.g., Spots 7, 8, 9, and 10 in Figure 2). This significant

392

difference in speciation of Se and Te in contaminated soil can be well explained by

393

different structures of surface complexes for Se and Te on Fe(III) hydroxides, which has

394

been documented by theoretical prediction and spectroscopic analysis. As shown in

395

Figure 4, the p Κ a values for conjugated anions of Se and Te present an order of Te(VI) >

396

Te(IV) > Se(IV) > H2WO4 >> Se(VI), indicating that Te(VI), Te(IV), and Se(IV) prefer to

397

form stable inner-sphere complexes on the surface of Fe(III) hydroxides, whereas Se(VI)

398

forms less stable outer-sphere complex. These predictions have been well demonstrated

399

by EXAFS results.10,18,47 Thus, Se(VI) has a lower affinity to soil particles and is readily

400

leached from soil into aquatic environment, which can be responsible for the much lesser

401

presence of Se(VI) in the contaminated soil.

402

Furthermore, approximately 0.1% of Se and less than 0.001% of Te in the same soil

403

sample were leached by water, respectively, implying that Se is much more soluble (>100

404

times) than Te in soil (Table S4). Similarly, the laboratory study10 also showed that the

405

distribution of Se to water is much higher than that of Te in the synthetic soil-water

406

system. It has been further documented that the larger affinity of Te for soil in originates

407

from the formation of the inner-sphere complexes of Te(IV) and Te(VI) on Fe(III)

408

hydroxides, while higher distribution of Se to water was ascribed to highly soluble Se(VI)

409

and its weak outer-sphere complex as shown for dominant Se(VI) in water phase.10

410

Therefore, the difference in the speciation and solubility of Se and Te in contaminated

411

soils from abandoned mine tailings can be strongly confirmed by the distribution

412

behaviors of Se and Te observed in the laboratory study.

413 19



414

Environmental Implications. It has been suggested that numerous ions (e.g., Zn2+, Cr3+,

415

Ge4+, As5+, and Sb5+) can be structurally incorporated into Fe(III) site of iron

416

oxides.18,41,48,49 Compared with surface adsorption, structural incorporation cannot be

417

greatly affected by environmental factors such as pH, ionic strength, and competitive

418

ions, resulting in the relatively low solubility and mobility in the environment. Similarly,

419

Te(VI) in soil can be expected to be relatively stable and difficult to mobilize if Te(VI) is

420

structurally incorporated into Fe(III) oxides in soil as demonstrated for ferromanganese

421

crust, although chemical processes for Te enrichment in contaminated soil could be more

422

complicated due to various affecting factors. However, Te(IV) was also an important

423

chemical species in addition to Te(VI) in the contaminated soil. Unlike Te(VI), Te(IV)

424

can be adsorbed by illite and Fe(III) hydroxides in soil via the formation of surface

425

complexes. Thus, the retention of Te(IV) in soil could be less stable than with that for

426

Te(VI), possibly resulting in easier release and migration for Te(IV) in soil under suboxic

427

conditions.

428

In the study area, the total Te concentrations in fern and moss species were 0.13 and

429

1.26 mg kg-1, respectively. In comparison with a recent investigation,7 these values are

430

greatly higher than Te levels in Japanese crops ranging from 0.0001 to 0.12 mg kg-1 with

431

a geometric mean of 0.0018 mg kg-1, but the soil-to-crop transfer factors (TFs) of Te in

432

our study are within the range of TFs in various crops (1.3×10-3-2.3×10-1). These facts

433

suggest that plant uptake of Te is likely to depend on its bioavailable fraction in soil, as

434

documented for other trace elements like Se.50,51 It has been assumed that Te in paddy

435

soil could be reduced to highly mobile HTeO3- under flooded condition, resulting in

436

higher Te concentration in brown rice than that in upland crop.7 However, further study is 20


Page 20 of 35

Page 21 of 35


437

necessary to clarify the bioavailability of every Te speciation in soil to different plant

438

species.

439

Our study clarifies the chemical speciation and host phases of Te in the

440

contaminated soil by the µ-XRF-XRD-XAFS techniques. These findings are of

441

significant importance for better understanding the solubility, mobility, and

442

bioavailability of Te in contaminated soil environment, which also can be extended to

443

similar surface environments. As Te concentration in common sample is much lower than

444

the level required for XAFS analysis, it is needed to develop the modeling of solid-water

445

distribution of Te to extend the speciation results of Te to much lower Te level in

446

environment.

447 448 449

Supporting Information

450

Complementary materials including figures (S1-S5), tables (S1-S4), as well as

451

several supplemental texts for the materials and methods section. Figures showing the

452

location of study area, total Te concentration in soil, µ-XRD patterns of Te hotspots,

453

Eh-pH diagram for Te, and the distribution and speciation of Se in contaminated soil.

454

Tables showing the geochemical characteristics of studied samples, the best fitting results

455

for Te k-edge µ-XANES spectra of Te hotspots, structural parameters of EXAFS spectra

456

for the Te hotspot in soil and adsorbed samples, and leached results for the contaminated

457

soil using water.

458 459

21



460

Acknowledgments

461

This work was supported by Grants-in-Aid for Scientific Research from the Japan

462

Society for the Promotion of Science (Nos. 16K13911, 16K12627, 16H04073, 15H02149,

463

and 24110008), the National Natural Science Foundation of China (41303099), Chinese

464

Academy of Sciences “Light of West China” Program, and State Key Laboratory of

465

Environmental Geochemistry (SKLEG2015201). This study was performed with the

466

approval of JASRI/SPring-8 (2015B0118, 2015B0127, 2016A0118, and 2016A0127) and

467

Photon Factory (2016G632 and 2015G664).

468

22


Page 22 of 35

Page 23 of 35


469

References

470

(1) Belzile, N.; Chen, Y. W. Tellurium in the environment: A critical review focused on

471

natural waters, soils, sediments and airborne particles. Appl. Geochem. 2015, 63, 83-92.

472

(2) Ba, L.A.; Doring, M.; Jamier, V.; Jacob, C. Tellurium: an element with great

473

biological potency and potential. Org. Biomol. Chem. 2010, 8, 4203-4216.

474

(3) Tang, Z. Y.; Zhang, Z. L.; Wang, Y.; Glotzre, S. C.; Kotov, N. A. Self-assembly of

475

cdte nanocrystals into free-floating sheets. Science 2006, 314, 274-278.

476

(4) Deng, Z. T.; Zhang, Y.; Yue, J. C.; Tang, F. Q.; Wei, Q. Green and orange CdTe

477

quantum dots as effective pH-sensitive fluorescent probes for dual simultaneous and

478

independent detection of viruses. J. Phys. Chem. B. 2007, 111, 12024-12031.

479

(5) Issa, Y. M.; Abdel-Fattah, H. M.; Shehab, O. R.; Abdel-Moniem, N. B. Determination

480

and speciation of tellurium hazardous species in real and environmental samples. Int. J.

481

Electrochem. Sci. 2016, 11, 7475-7498.

482

(6) Tagami, K.; Uchida, S.; Ishii, N.; Zheng, J. Estimation of Te-132 distribution in

483

Fukushima Prefecture at the early stage of the Fukushima Daiichi Nuclear Power Plant

484

reactor failures. Environ. Sci. Technol. 2013, 47, 5007-5012.

485

(7) Yang, G.; Zheng, J.; Tagami, K.; Uchida, S. Soil-to-crop transfer factors of tellurium.

486

Chemosphere 2014, 111, 554-559.

487

(8) Cohen, B. L. Anomalous behavior of tellurium abundances. Geochim. Cosmochim.

488

Acta 1984, 48, 203-205.

489

(9) Hein, J. R.; Koschinsky, A.; Halliday, A. N. Global occurrence of tellurium-rich

490

ferromanganese crusts and a model for the enrichment of tellurium. Geochim.

491

Cosmochim. Acta 2003, 67, 1117-1127. 23



492

(10) Harada, T.; Takahashi, Y. Origin of the difference in the distribution behavior of

493

tellurium and selenium in a soil–water system. Geochim. Cosmochim. Acta 2008, 72,

494

1281-1294.

495

(11) Lee, D. S.; Edmond, J. M. Tellurium species in seawater. Nature 1985, 313,

496

782-785.

497

(12) Karlson, U.; Frankenberger, W.T. Metal ions in biological systems; Marcel Dekker:

498

New York, 1993.

499

(13) Chasteen, T. G.; Fuentes, D. E.; Tantalean, J. C.; Vasquez, C. C. Tellurite: history,

500

oxidative stress, and molecular mechanisms of resistance. FEMS Microbiol. Rev. 2009,

501

33, 820-832.

502

(14) Ramos-Ruiz, A.; Field, J. A.; Wilkening, J. V.; Sierra-Alvarez, R. Recovery of

503

elemental tellurium nanoparticles by the reduction of tellurium oxyanions in a

504

methanogenic microbial consortium. Environ. Sci. Technol. 2016, 50, 1492-1500.

505

(15) Kim, D. H.; Kim, M. G.; Jiang, S.; Lee, J. H.; Hur, H. G. Promoted reduction of

506

tellurite and formation of extracellular tellurium nanorods by concerted reaction between

507

iron and Shewanella oneidensis MR-1. Environ. Sci. Technol. 2013, 47, 8709-8715.

508

(16) Grundler, P. V.; Brugger, J.; Etschmann, B. E.; Helm, L.; Liu, W.; Spry, P. G.; Tian,

509

Y.; Testemale, D.; Pring, A. Speciation of aqueous tellurium(IV) in hydrothermal

510

solutions and vapors, and the role of oxidized tellurium species in Te transport and gold

511

deposition. Geochim. Cosmochim. Acta 2013, 120, 298-325.

512

(17) Chen, Y. W.; Alzahrani, A.; Deng, T. L.; Belzile, N. Valence properties of tellurium

513

in different chemical systems and its determination in refractory environmental samples

24


Page 24 of 35

Page 25 of 35


514

using hydride generation-Atomic fluorescence spectroscopy. Anal. Chim. Acta. 2016,

515

905, 42-50.

516

(18) Kashiwabara, T.; Oishi, Y.; Sakaguchi, A.; Sugiyama, T.; Usui, A.; Takahashi, Y.

517

Chemical processes for the extreme enrichment of tellurium into marine ferromanganese

518

oxides. Geochim. Cosmochim. Acta 2014, 131, 150-163.

519

(19) MacLean, L. C.; Beauchemin, S.; Rasmussen, P. E. Lead speciation in house dust

520

from Canadian urban homes using EXAFS, micro-XRF, and micro-XRD. Environ. Sci.

521

Technol. 2011, 45, 5491-5497.

522

(20) Mitsunobu, S.; Takahashi, Y.; Terada, Y. µ-XANES evidence for the reduction of

523

Sb(V) to Sb(III) in soil from sb mine tailing. Environ. Sci. Technol. 2010, 44, 1281-1287.

524

(21) Grafe, M.; Donner, E.; Collins, R. N.; Lombi, E. Speciation of metal(loid)s in

525

environmental samples by X-ray absorption spectroscopy: A critical review. Anal. Chim.

526

Acta 2014, 822, 1-22.

527

(22) Hori, H.; Koyama, E.; Nagashima, K. Kinichilite, a new minera from the Kawazu

528

mine, Shimoda city, Japan. Miner. Journ. 1981, 10, 333-337.

529

(23) Shimizu, M.; Kato, A.; Matsubara, S. Hemusite and paraguanajuatite from the

530

Kawazu mine, Shizuoka Prefecture, Japan. Miner. Journ. 1988, 14, 92-100.

531

(24) Nakata, M.; Komuro, K. Chemistry and Occurrences of Native Tellurium from

532

Epithermal Gold Deposits in Japan. Resour. Geol. 2011, 61, 211-223.

533

(25) Igarashi, N.; Nitani, H.; Takeichi, Y.; Niwa, Y.; Abe, H.; Kimura, M.; Mori, T.;

534

Nagatani, Y.; Kosuge, T.; Kamijo, A.; Koyama, A.; Ohta, H.; Shimizu, N. Newly

535

designed double surface bimorph mirror for BL-15A of the photon factory. AIP

536

Conference Proceedings 2016, 1741, 040021. 25



537

(26) Zabinsky, S. I.; Rehr, J. J.; Ankudinov, A.; Albers, R. C.; Eller, M. J.

538

Multiple-scattering calculations of X-ray-absorption spectra. Phys. Rev. B. 1995, 52,

539

2995-3009.

540

(27) Jumas, J. C.; Wintenberger, M.; Philippot, E. Etude magnetique des phases du

541

systeme Fe2O3TeO2 structure magnetique de Fe2TeO5 a 4.2 K. Mater. Resear. Bullet.

542

1977, 12, 1063-1070.

543

(28) Krishnan, K.; Singh Mudher, K. D.; Rama Rao, G. A.; Venugopal, V. Structural and

544

thermochemical studies on Cr2TeO6 and Fe2TeO6. J. Alloy. Compd. 2001, 316, 264-268.

545

(29) Salminen, R.; Plant, J. A.; Reeder, S. Geochemical atlas of Europe. Part 1,

546

background information, methodology and maps. Espoo: Geological Survey of Finland,

547

2005.

548

(30) Perkins, W. T. Extreme selenium and tellurium contamination in soils-an eighty

549

year-old industrial legacy surrounding a Ni refinery in the Swansea Valley. Sci. Total.

550

Environ. 2011, 412-413, 162-169.

551

(31) Brookins, D. G. Eh-pH diagram for geochemistry; Springer-Verlag: Berlin, 1988.

552

(32) McPhail, D. C. Thermodynamic properties of aqueous tellurium species between 25

553

and 350℃. Geochim. Cosmochim. Acta 1995, 59, 851-866.

554

(33) Dzombak, D. A.; Morel, F. M. M. Surface complexation modeling, hydrous ferric

555

oxide; John Wiley & Sons: New York, 1990.

556

(34) Dean, J. A. Lange’s Handbook of Chemistry; 15th, ed.; McGraw Hill: New York,

557

1999.

558

(35) Li, Y. H. Ultimate removal mechanisms of elements from ocean. Geochim.

559

Cosmochim. Acta 1981, 45, 1659-1664. 26


Page 26 of 35

Page 27 of 35


560

(36) Kashiwabara, T.; Takahashi, Y.; Tanimizu, M.; Usui, A. Molecular-scale

561

mechanisms of distribution and isotopic fractionation of molybdenum between seawater

562

and ferromanganese oxides. Geochim. Cosmochim. Acta 2011, 75, 5762-5784.

563

(37) Kashiwabara, T.; Takahashi, Y.; Marcus, M. A.; Uruga, T.; Tanida, H.; Terada, Y.;

564

Usui, A. Tungsten species in natural ferromanganese oxides related to its different

565

behavior from molybdenum in oxic ocean. Geochim. Cosmochim. Acta 2013, 106,

566

364-378.

567

(38) Manceau, A.; Drits, V. A. Local structure of ferrihydrite and feroxyhite by EXAFS

568

spectroscopy. Clay. Miner. 1993, 28, 165-184.

569

(39) Waychunas, G. A.; Rea, B. A.; Fuller, C. C.; Davis, J. A. Surface-chemistry of

570

ferrihydrite: part 1. EXAFS studies of the geometry of coprecipitated and adsorbed

571

arsenate. Geochim. Cosmochim. Acta 1993, 57, 2251-2269.

572

(40) Langmuir, D. Aqueous environmental geochemistry; Prentice Hall: Upple Saddle

573

River, 1997.

574

(41) Mitsunobu, S.; Takahashi, Y.; Terada, Y.; Sakata, M. Antimony(V) incorporation

575

into synthetic ferrihydrite, goethite, and natural iron oxyhydroxides. Environ. Sci.

576

Technol. 2010, 44, 3712-3718.

577

(42) Qin, H. B.; Yokoyama, Y.; Fan, Q. H.; Iwatani, H.; Tanaka, K.; Sakaguchi, A.;

578

Kanai, Y.; Zhu, J.; Onda, Y.; Takahashi, Y. Investigation of cesium adsorption on soil

579

and sediment samples from Fukushima Prefecture by sequential extraction and EXAFS

580

technique. Geochem. J. 2012, 46, 355-360.

581

(43) Fan, Q. H.; Tanaka, M.; Tanaka, K.; Sakaguchi, A.; Takahashi, Y. An EXAFS study

582

on the effects of natural organic matter and the expandability of clay minerals on cesium 27



583

adsorption and mobility. Geochim. Cosmochim. Acta 2014, 135, 49-65.

584

(44) Goldberg, S. Modeling selenite adsorption envelopes on oxides, clay minerals, and

585

soils using the triple layer model. Soil. Sci. Soc. Am. J. 2013, 77, 64-71.

586

(45) Missana, T.; Alonso, U.; García-Gutiérrez, M. Experimental study and modelling of

587

selenite sorption onto illite and smectite clays. J. Colloid. Interf. Sci. 2009, 334, 132-138.

588

(46) Ryser, A. L.; Strawn, D. G.; Marcus, M. A.; Fakra, S.; Johnson-Maynard, J. L.;

589

Möller, G. Microscopically focused synchrotron X-ray investigation of selenium

590

speciation in soils developing on reclaimed mine lands. Environ. Sci. Technol. 2006, 40,

591

462-467.

592

(47) Hayes, K. F.; Roe, A. L.; Brown, G. E.; Hodgson, K. O.; Leckie, J. O.; Parks, G. A.

593

In situ x-ray absorption study of surface complexes: selenium oxyanions on a-FeOOH.

594

Science 1987, 238, 783-786.

595

(48) Manceau, A.; Schlegel, M. L.; Musso, M.; Sole, V. A.; Gauthier, C.; Petit, P. E.;

596

Trolard, F. Crystal chemistry of trace elements in natural and synthetic goethite. Geochim.

597

Cosmochim. Acta 2000, 64, 3643-3661.

598

(49) Martinez, C. E.; McBride, M. B. Cd, Cu, Pb, and Zn coprecipitates in Fe oxides

599

formed at different pH: aging effects on metal solubility and extractability by citrate.

600

Environ. Chem. 2001, 20, 122-126.

601

(50) Qin, H. B.; Zhu, J. M.; Su, H. Selenium fractions in organic matter from Se-rich

602

soils and weathered stone coal in selenosis areas of China. Chemosphere 2012, 86,

603

626-633.

604

(51) Qin, H. B.; Zhu, J. M.; Liang, L.; Wang, M. S.; Su, H. The bioavailability of

605

selenium and risk assessment for human selenium poisoning in high-Se areas, China. 28


Page 28 of 35

Page 29 of 35

606


Environ. Int. 2013, 52, 66-74.

607

29



608

Captions

609

Figure 1. µ-XRF maps of selected areas in contaminated soil. The upper figures are

610

optical image of five interested areas (A-E), while the middle and lower figures show the

611

maps of Te and Fe, respectively. The open circles in Te maps indicate interested hotspots

612

for further µ-XAFS measurement.

613

Figure 2. Te K-edge µ-XANES spectra (solid lines) of interested hotspots in soil grains

614

marked by open circles in Figure 1. Red dotted lines on each spectrum are simulation

615

spectra obtained from the best LCF results by combining Na2TeO3 and Na2H4TeO6 in the

616

range of 31800-31835 eV.

617

Figure 3. Te K-edge EXAFS spectra of hotspots in soil grains and adsorbed samples: (A)

618

k3-weighted x(k) spectra, and (B) their RSFs (phase shift not corrected). Solid lines are

619

spectra obtained by experiments, and red dash lines are calculated spectra by curve-fitting

620

analysis.

621

Figure 4. Relationship between pKa values and attachment modes on ferrihydrite for

622

various oxyanions. The pKa1 and pKa2 values are obtained from the reference.33

623

Figure 5. Adsorption envelopes for Te(IV) and Te(VI) on ferrihydrite (Fh), goethite (Goe)

624

and illite as a function of pH. Diamond, triangle and circle represent ferrihydrite, goethite

625

and illite, respectively. Solid and dotted lines indicate Te(IV) and Te(VI) species,

626

respectively.

627

30


Page 30 of 35

Page 31 of 35


628

629 630 631 632 633 634 635

Figure 1. µ-XRF maps of selected areas in contaminated soil. The upper figures are optical image of five interested areas (A-E), while the middle and lower figures show the maps of Te and Fe, respectively. The open circles in Te maps indicate interested hotspots for further µ-XAFS measurement.

31



636

637 638 639 640 641 642

Figure 2. Te K-edge µ-XANES spectra (solid lines) of interested hotspots in soil grains marked by open circles in Figure 1. Red dotted lines on each spectrum are simulation spectra obtained from the best LCF results by combining Na2TeO3 and Na2H4TeO6 in the range of 31800-31835 eV.

32


Page 32 of 35

Page 33 of 35


643

644 645 646 647 648 649

Figure 3. Te K-edge EXAFS spectra of hotspots in soil grains and adsorbed samples: (A) k3-weighted x(k) spectra, and (B) their RSFs (phase shift not corrected). Solid lines are spectra obtained by experiments, and red dash lines are calculated spectra by curve-fitting analysis.

33



650

651 652 653 654

Figure 4. Relationship between pKa values and attachment modes on ferrihydrite for various oxyanions. The pKa1 and pKa2 values are obtained from the reference.33

34


Page 34 of 35

Page 35 of 35


655

656 657 658 659 660 661 662

Figure 5. Adsorption envelopes for Te(IV) and Te(VI) on ferrihydrite (Fh), goethite (Goe) and illite as a function of pH. Diamond, triangle and circle represent ferrihydrite, goethite and illite, respectively. Solid and dotted lines indicate Te(IV) and Te(VI) species, respectively.

35


Tellurium Distribution and Speciation in ... - ACS Publications

Recommend Documents