IEG 환경지질연구정보센터
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전체 글
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(4) . . . . . . Mobility of Transition Metals by Change of Redox Condition in Dump Tailings from the Dukum Mine, Korea Yong Hee Moon1, Hi-Soo Moon1*, Young Seog Park2, Ji-Won Moon1, Yungoo Song1 and Jong-Chun Lee3 1. Department of Earth System Sciences, Yonsei University, Seoul 120-479, Korea Department of Mineral Resource Engineering, Chosun University, Gwangju 501-759, Korea 3 Youngsan-River Environment Research Laboratory National Institute of Environmental Research, Sooncheon 540-932, Korea 2. Tailings of Dukum mine in the vadose and saturated zone were investigated to reveal the mobility of metal elements and the condition of mineralogical solubility according to redox environments throughout the geochemical analysis, thermodynamic modelling, and mineralogical study for solid-samples and water samples(vadose zone; distilled water: tailings=5:1 reacted, saturated zone; pore-water extracted). In the vadose zone, sulfide oxidation has generated low-pH (2.72~6.91) condition and high concentration levels of SO42−(561~1430 mg/L) and other metals(Zn:0.12~157 mg/L, Pb:0.06~0.83 mg/L, Cd :0.06~1.35 mg/L). Jarosite(KFe3(SO4)2(OH)6) and gypsum(CaSO4 · 2H2O) were identified on XRD patterns and thermodynamics modelling. In the saturated zone, concentration of metal ions decreased because pH values were neutral(7.25~8.10). But Fe and Mn susceptible to redox potential increased by low-pe values(7.40~3.40) as the depth increased. Rhodochrosite(MnCO3) identified by XRD and thermodynamics modelling suggested that Mn4+ or Mn3+ was reduced to Mn2+. Along pH conditions, concentrations of dissolved metal ions has been most abundant in vadose zone throughout borehole samples. It was observed that pH had more effect on metal solubilities than redox potential. However, the release of co-precipitated heavy metals following the dissolution of Fe-Mn oxyhydroxides could be the mechanism by which reduced condition affected heavy metal solubility considering the decrease of pe as depth increased in the saturated zone.. tailings, redox, transition metal, solubility, saturated index.
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(35) . Schematic diagram showing sample for porewater and bulk, with respect to the tailings cross section. For each sampled zone within in the cross-section, porewater samples and bulk samples in select on unsaturation zone(A and B) and saturation zone(C, D and E) analyses for each depth increment.. . . X-ray diffraction patterns for the bulk samples from unsaturation zone (A1 and B1) to saturation zone(C1, D4 and E2). Qz: quartz, Fd: feldspar, Mi: mica, Py: pyrite, Ka: Kaolinite Ja: jarosite, Ga: galena, Sph: sphalerite, Rh: rhodochrosite and Fer: ferrihydrite..
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(54) !. . Table 1. Chemical composition of tailings pore-water from the Dukum mine(All values in mg/L). Sample No.. Depth (cm). pH. pe. Ca. K. A1 0~30 2.72 13.11 167 A2 30~50 6.34 8.36 483 A A3 50~75 6.66 8.11 337 A4 75~100 6.91 6.26 430 A5 100~130 6.88 7.86 282 B1 130~150 7.19 7.60 372 B2 150~183 7.66 7.60 237 B B3 183~200 7.41 8.04 40.0 B4 200~230 7.53 7.54 145 C1 230~260 8.10 6.68 656 C C2 260~280 8.06 6.07 709 C3 280~300 8.00 6.00 729 D1 300~330 7.37 7.40 711 D2 330~365 7.25 7.07 687 D D3 365~400 7.27 6.98 702 D4 400~445 7.35 6.83 676 E1 445~480 7.36 3.40 648 E E2 480~500 7.38 4.59 613 *Detection limit(ppm); Fe:0.08, Mn:0.028,. Na. Mg. Mn. 1.31 0.06 25.2 105.8 6.00 0.06 20.5 119.5 11.3 1.27 10.3 51.8 14.7 1.52 13.3 35.8 7.95 0.72 7.66 15.0 14.2 1.54 11.4 22.9 9.70 0.86 6.34 1.70 9.18 0.56 4.36 1.97 11.8 1.15 3.92 3.53 242 26.0 60.7 2.73 67.1 34.2 53.1 4.19 96.5 44.1 55.9 10.6 138 81.6 59.4 38.2 152 139 47.4 81.5 101 506 46.7 126 117 479 38.3 62.5 97.9 872 36.1 72.6 158 24.9 32.4 83.5 Zn:0.04, Pb:0.04, Cd:0.04. Fe. Zn. Pb. Cd. 7.20 <0.08 0.21 0.10 <0.08 <0.08 <0.08 0.09 0.32 <0.08 <0.08 <0.08 <0.08 <0.08 <0.08 <0.08 0.56 3.38. 158 9.52 42.5 23.5 14.4 2.79 <0.04 0.81 0.12 <0.04 <0.04 <0.04 <0.04 0.07 0.13 0.18 0.04 <0.04. 0.05 0.38 0.38 0.06 0.83 0.04 0.04 <0.04 <0.04 <0.04 <0.04 <0.04 <0.04 <0.04 0.05 0.05 <0.04 <0.04. 1.35 0.50 0.18 0.08 <0.04 0.17 <0.04 0.06 0.04 0.04 <0.04 <0.04 <0.04 <0.04 <0.04 <0.04 0.04 <0.04. F. Cl. SO4. 4.62 2.04 0.00 1.74 1.67 2.30 2.95 2.30 2.44 3.74 3.98 4.31 3.68 3.44 10.3 7.54 3.20 0.00. 3.31 0.00 3.36 1.15 1.18 1.60 2.99 2.65 2.88 192 67.4 79.2 168 256 391 386 516 460. 1090 1430 780 914 561 691 424 95.2 286 1360 1400 1500 1590 1610 1840 1590 1640 1470. Table 2. Equilibrium reactions of Iron and Manganese species at 25oC used in pH-pe diagram calculations. log Ko. Equilibrium reaction 3+. −. Fe +e. Fe. 2+. Fe(OH)3(ferrihydrite)+3H++e−. Fe2++3H2O +. K++3Fe3++2SO42−+6H2O. KFe3(SO4)2(OH)6(jarosite)+6H FeS2(pyrite)+2H++2e−. Fe2++2HS+. +. KFe3(SO4)2(OH)6(jarosite)+6H. K +3Fe +2SO4 +6H2O K++3Fe2++2SO42−+6H2O. Lindsay(1979). 41.89. Lindsay(1979). 35.38. Lindsay(1979). Mn2++2H2O. 25.27. Lindsay(1979). 0.32. MnOOH(manganite) Mn3O4(hausmanite)+2H2O. Mn3O4(hausmanite)+8H++3CO32−+2e− +. −. MnOOH(manganite)+HCO3+2H +e Mn(OH)2(pyrochroite)+2H++CO32−. Mn3O4(hausmanite)+2H++2e−+2H2O. 3MnCO3(rhodochrosite)+4H2O MnCO3(rhodochrosite)+2H2O MnCO3(rhodochrosite)+2H2O 3Mn(OH)2(pyrochroite). L 0( # +Q *BC f< X /E M;; /· = 0f45 " N '@ -/ ÷@ ï 0L + )# E,T ÷Þ ´'E / $7 . . . -12.51. 2+. MnCO3(rhodochrosite)+H+ Mn2++HCO3-. β-MnO2(pyrolusite)+H +e. Parkhurst(1999). Mn2++2H2O Mn +1.8H2O. 3MnOOH(manganite)+H++e−. -18.48. Lindsay(1979). −. −. Lindsay(1979) Lindsay(1979). Lindsay(1979). δ-MnO1.8(birnessite)+3.6H +e. +. 3.54 -12.51. -16.05. 3Fe(OH)3(ferrihydrite)+K++2SO42−+3H+. β-MnO2(pyrolusite)+4H++2e− MnOOH(manganite)+3H++e−. Lindsay(1979). 0.53. KFe3(SO4)2(OH)6(jarosite)+H2O +. 2−. 3+. KFe3(SO4)2(OH)6(jarosite)+6H++3e−.
(55) . Reference. 13.04. . Fetter(1999). 16.62. Lindsay(1979). -12.78. Lindsay(1979). 38.79. Lindsay(1979). 6.4. Lindsay(1979). 25.96. Fetter(1999). 17.46. Lindsay(1979). T ï = î E /R ð ï = $7 + w4L ´'E G ÉÊ ; < #k$E FG: ÷n; R% A E !¦¿= & 4L . ' '. .
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(57) . . Saturation indices of some mineral phases for the tailings porewater calculated waing PHREEQC2. Samples are the same as those in Fig. 3a.
(58) . Mineral phase Gypsum Ferrihydrite Jarosite Siderite Pyrolusite Birnessite Manganite Hasmannite Rhodochrosite . A1. Composition. B1. CaSO4 · 2H2O Fe(OH)3 KFe3(SO4)2(OH)6 FeCO3 β-MnO2 δ-MnO2 MnOOH Mn3O4 MnCO3. . E2 -0.07 3.24. . -0.45 -2.61 0.89 2.65 1.02. . . 2. . 2. . . . . . 0. D. 6( C. 7 C. . L6= =L'(. C. E / 23+ E< Ð *í @ /] S: ~ 0L «lQ µ n % +Q F©# ~ + < .E< x @L ML'. D. -. #. . . . F * ' . . .
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(79) . . 6. pH-pe diagram for the system Mn-CO2-H2O at 25oC and 1bar pressure, assuming Mn(aq)=10−2.82 mol/kg at solid/ solution boundariesand CO2=10−3.0 mol/kg on E(480-500 cm). First, dashed line(----) is solid/solution boun-dary for Mn(aq)=10−3.28 mol/kg on B(130-150 cm). Second, dashed line(- · - · -) is solid/solution boundary for Mn(aq)=10−4.32 mol/kg on C(480-500 cm). A circle symbols are chemical parameters(pe-pH) in the vadose zone. A square symbols are chemical parameters in the saturated zone. Figure is modified after Hem(1985).. """. ?0. . :. 2. pH-pe diagram for the system Fe-SO4-H2O at 25oC and 1bar pressure, assuming Fe(aq)=10−3.9 mol/kg at solid/solution boundaries, S(aq)=10−2 mol/kg and K=10−4.5 mol/kg on A(>30 cm). Short dashed line is solid/solution boundary for Fe(aq)=10−6.1 mol/kg, S(aq)=10−2.14 mol/kg, K=10−3.44 mol/kg on B(130-150 cm). Long dashed line is solid/solution boundary for Fe(aq)=10-4 mol/kg, S(aq)=10−2 mol/kg, K=10-2.4 mol/kg on E(480-500 cm). A circle symbols are chemical parameters(pH-pe) in the vadose zone. A square symbols are chemical parameters in the saturated zone. Figure is modified after Hem(1985)..
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