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22

483

Figure legends

484

Figure 1 Sampling points in each lake (Lake Nakaumi, 35.43°N 144.27°E; Lake Suigetsu,

485

35.58°N 135.88°E; Lake Suga, 35.58°N 135.90°E; Lake Biwa, 35.00°N 135.57°E; Lake

486

Kawaguchi, 35.51°N 138.73°E).

487

Figure 2 Schematic experimental process to evaluate PSi stability. The 0.4-µm nuc

488

leopore filter was used to separate the silicates adsorbed on Fe(OH)3 precipitate f

489

rom the initial solution (the mixture of MSi and DFe). Moreover, the 0.2-µm nu

490

cleopore filter was used to remove FeS precipitate, including the colloidal FeS c

491

ompletely.

492

Figure 3 Vertical profiles of TSi (□), MSi (〇), and PSi (▲) in the pore water of Lake

493

Nakaumi (August 21, 2017). No significant difference was observed between TSi and

494

MSi concentrations.

495

Figure 4 Vertical profiles of TSi (□), MSi (〇), and PSi (▲) in the pore waters of Lakes

496

Suigetsu (left) and Suga (right) on May 20, 2017.

497

Figure 5 Vertical profiles of DO in Lake Biwa (●, September 21, 2017) and Lake

498

Kawaguchi (〇, September 30, 2017).

499

Figure 6 Vertical profiles of DFe and H2S + HS− in the pore waters of Lake Biwa (●,

500

September 21, 2017) and Lake Kawaguchi (〇, September 30, 2017).

501

Figure 7 Vertical profiles of TSi (□), MSi (〇), and PSi (▲) in the pore waters of Lake

502

Biwa (left; September 21, 2017) and Lake Kawaguchi (right; September 30, 2017).

23

503

504

Figure 8 Annual change in DO concentration in the hypolimnion layer (water depth: 12

m) of Lake Biwa.

505

Figure 9 Vertical profiles of DFe (■), H2S +HS− (△), TSi (□), MSi (〇), and PSi (▲)

506

in the pore water of Lake Biwa from March 14 to December 15, 2017.

507

Figure 10 Formation of polymeric silicate in the adsorption reaction of silicate onto

508

ferric hydroxide, over 120 days. Only the concentrations of TSi (□), MSi (〇), and PSi

509

(▲) in the precipitate are presented.

510

Figure 11 Stability of PSi under each set of conditions, namely HNO3 + Aeration (〇),

511

HNO3 + Anaeration (□), Na2S + Aeration (●), and Na2S + Anaeration (▲), over 14

512

days.

513

Figure 12 Changes in the concentration of H2S + HS− and DO under each set of

514

conditions, over two weeks. □: DO in HNO3 + Aeration, ●: DO in Na2S + Aeration,

515

△: H2S + HS− in Na2S + Aeration, and ▲: H2S + HS− in Na2S + Anaeration. Note that

516

concentrations of DO in HNO3 + Anaeration, DO in Na2S + Anaeration, and H2S + HS−

517

in HNO3 + Aeration/Anaeration have been omitted because these values were 0 mg-O2

518

L-1 (DO) or 0 mmol L-1 (H2S + HS−) throughout the experimental period.

519

520

24

521

Figures

522

523

Figure 1 Sampling points in each lake (Lake Nakaumi, 35.43°N 144.27°E; Lake Suigets

524

u, 35.58°N 135.88°E; Lake Suga, 35.58°N 135.90°E; Lake Biwa, 35.00°N 135.57°E; La

525

ke Kawaguchi, 35.51°N 138.73°E).

526

25

1.0 mmol L-1 MSi and 0.1 mmol L-1 DFe (Fe3+) at pH 7.0 (1000 mL)

Storage for 6 months

First Fraction

(HNO3 + Aeration)

Second Fraction

(HNO3 + Anaeration)

Third Fraction

(Na2S + Aeration)

Fourth Fraction

(Na2S + Anaeration)

100 mL

100 mL

100 mL

100 mL

Filtration (0.40-µm Nucleopore Filter)

Filtrate

Precipitate

Filtrate

Precipitate

Filtrate

Precipitate

Filtrate

Precipitate

Chemical

Analysis

0.02 mol L-1

HNO3

100 mL

Chemical

Analysis

0.02 mol L-1

HNO3

100 mL

Chemical

Analysis

0.3 mmol L-1

Na2S

100 mL

Chemical

Analysis

0.3 mmol L-1

Na2S

100 mL

Filtration (0.20-µm Nucleopore Filter)

Aeration

Anaeration

Aeration

Anaeration

Leave for 0 - 14 days under each condition

527

Chemical Analysis for MSi, TSi, PSi, DO and total dissolved hydrogen sulfide (H2S + HS-)

528

Figure 2 Schematic experimental process to evaluate PSi stability. The 0.4-µm

529

nucleopore filter was used to separate the silicates adsorbed on Fe(OH)3 precipitate

530

from the initial solution (the mixture of MSi and DFe). Moreover, the 0.2-µm

531

nucleopore filter was used to remove FeS precipitate, including the colloidal FeS

532

completely.

533

26

534

535

Figure 3 Vertical profiles of TSi (□), MSi (〇), and PSi (▲) in the pore water of Lake

536

Nakaumi (August 21, 2017). No significant difference was observed between TSi and

537

MSi concentrations.

538

539

540

27

541

542

Figure 4 Vertical profiles of TSi (□), MSi (〇), and PSi (▲) in the pore waters of Lakes

543

Suigetsu (left) and Suga (right) on May 20, 2017.

544

545

28

546

547

Figure 5 Vertical profiles of DO in Lake Biwa (●, September 21, 2017) and Lake

548

Kawaguchi (〇, September 30, 2017).

549

29

550

551

Figure 6 Vertical profiles of DFe and H2S + HS− in the pore waters of Lake Biwa (●,

552

September 21, 2017) and Lake Kawaguchi (〇, September 30, 2017).

553

30

554

555

Figure 7 Vertical profiles of TSi (□), MSi (〇), and PSi (▲) in the pore waters of Lake

556

Biwa (left; September 21, 2017) and Lake Kawaguchi (right; September 30, 2017).

557

558

559

31

560

561

562

Figure 8 Annual change in DO concentration in the hypolimnion layer (water depth: 12

m) of Lake Biwa.

563

564

32

565

566

Figure 9 Vertical profiles of DFe (■), H2S +HS− (△), TSi (□), MSi (〇), and PSi (▲)

567

in the pore water of Lake Biwa from March 14 to December 15, 2017.

568

33

569

570

Figure 10 Formation of polymeric silicate in the adsorption reaction of silicate onto

571

ferric hydroxide, over 120 days. Only the concentrations of TSi (□), MSi (〇), and PSi

572

(▲) in the precipitate are presented.

573

574

575

34

576

577

Figure 11 Stability of PSi under each set of conditions, namely HNO3 + Aeration (〇),

578

HNO3 + Anaeration (□), Na2S + Aeration (●), and Na2S + Anaeration (▲), over 14

579

days.

580

35

581

582

Figure 12 Changes in the concentration of H2S + HS− and DO under each set of

583

conditions, over two weeks. □: DO in HNO3 + Aeration, ●: DO in Na2S + Aeration,

584

△: H2S + HS− in Na2S + Aeration, and ▲: H2S + HS− in Na2S + Anaeration. Note that

585

concentrations of DO in HNO3 + Anaeration, DO in Na2S + Anaeration, and H2S + HS−

586

in HNO3 + Aeration/Anaeration have been omitted because these values were 0 mg-O2

587

L-1 (DO) or 0 mmol L-1 (H2S + HS−) throughout the experimental period.

588

36

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