Oleh Sri Juari Santosa Jurusan Kimia FMIPA UGM ACID MINE Acidity: 1.Oxidation of pyrite 2....
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Transcript of Oleh Sri Juari Santosa Jurusan Kimia FMIPA UGM ACID MINE Acidity: 1.Oxidation of pyrite 2....
![Page 1: Oleh Sri Juari Santosa Jurusan Kimia FMIPA UGM ACID MINE Acidity: 1.Oxidation of pyrite 2. Dissolution of humic and fulvic acids.](https://reader035.fdocuments.net/reader035/viewer/2022062407/56649da55503460f94a90a58/html5/thumbnails/1.jpg)
Oleh
Sri Juari SantosaJurusan Kimia FMIPA UGM
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ACID MINE
Acidity:
1.Oxidation of pyrite
FeS(s) + O2(aq) + 2 H2O(l) Fe2+(aq) + SO4
2-(aq) + 4 H+
(aq) )(24
1gO
Fe3+(aq) + SO4
2-(aq) + 3 H+
(aq) + ½ H2O(l)
2. Dissolution of humic and fulvic acids
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Humic Substances are traditionally fractionated according to their solubilities
Fulvic acids: are those organic materials that are soluble in water at all pH values
Humic acids: are those materials that are insoluble at acidic pH values (pH < 2) but are soluble at higher pH values
Humin: is the fraction that is insoluble in water at all pH values
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Negative Effect of Acid Mine
Attach and erode soil and minerals to result the dissolution of metals, like Fe, Cd, Mn, and Zn
Environmental pollution
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Utilization of Hydrotalcite to remediate acid mine
Study on the ability of Mg/Al hydrotalcite in neutralize the acidity through
exchanging its interlayer hydroxide (OH-), carbonate (CO32-), and
bicarbonate (HCO3-) anions with polluting anions of SO4
2-, humic acid (HA),
and fulvic acid (FA) in aqueous solution
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OH- H O2 CO32- HCO3
-
M , M2+ 3+
M , M2+ 3+
OH
OH
OH
OH
Hydrotalcite (layered double hydroxide anionic clay)
1) General formula: [M2+1-xM3+
x(OH)2]x+(An-)x/n . yH2O
where: M2+ is divalent cation M3+ is trivalent cation An- is interlayer anion (1-x/x) varies from 1 to 5
2) Structure:
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No Name Empirical formula Crystal system Image Origin
1 BarbertoniteNot Radioactive
Mg6Cr2(CO3)(OH)16·4(H2O)
Molecular Weight = 654.01 gm
Hexagonal - Dihexagonal Dipyramidal
Nevada Creek, Tasmania, Australia
2 BechereriteNot Radioactive
Zn4.5Cu1.5Zn2(OH)132(S0.75)2(Si0.25)2(O3)2(OH)
Molecular Weight = 933.60 gmTrigonal -
PyramidalColor: Light
greenTonopah-Belmont mine,
Osborne silver-gold district, Maricopa County, Arizona USA
3 Carbonate-cyanotrichite
Not Radioactive
Cu4Al2(CO3)0.66(SO4)0.34(OH)12·2(H2O)
Molecular Weight = 620.53 gm
Orthorhombic Widowmaker mine, Fry Canyon, San Juan Co., Utah, USA
4 CaresiteNot Radioactive
Fe2+4Al2(CO3)(OH)12·3(H2O)
Molecular Weight = 595.49 gm
Trigonal - Trapezohedral
Poudrette quarry, Mt Saint-Hilaire, Rouville Co., Québec, Canada
5 CarrboyditeNot Radioactive
Ni10Cu4Al9(SO4)4(CO3)2(OH)43·7(H2O)
Molecular Weight = 2,445.61 gm
Hexagonal Carr-Boyd Nickel Mine, Western Australia, Australia
6 ChalcoalumiteNot Radioactive
CuAl4(SO4)(OH)12·3(H2O)
Molecular Weight = 525.67 gm
Monoclinic – Sphenoidal
Lavender Pit, Bisbee, Cohchise County, Arizona, USA
7 Charmarite-2H & Charmarite-3T
Not Radioactive
Mn2+4Al2(CO3)(OH)12·3(H2O)
Molecular Weight = 591.86 gm
Hexagonal – Trapezohedral
Color: Orange brown, Pale brown, Pale blue, Colorless
Mt. St.-Hilaire, QUE, Canada
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8 ChlormagaluminiteNot Radioactive
Mg3.5Fe2+0.5Al2(OH)12Cl(CO3)0.5·2(H2O)
Molecular Weight = 472.53 gm
Hexagonal Color: Colorless, Yellow brown
Kapaev explosion pipe, Angara River, southern Siberian Platform, Russia
9 CyanotrichiteNot Radioactive
Cu4Al2(SO4)(OH)12·2(H2O)
Molecular Weight = 644.33 gm
Orthorhombic Grandview mine, Grand Canyon, Coconino County, Arizona, USA
10 GlaucoceriniteNot Radioactive
Zn3Cu2Al3(SO4)1.5(OH)16·9(H2O)
Molecular Weight = 982.56 gm
Trigonal Mina Serpieri, Laurium, Attiki, Greece
11 HydrombobomkuliteNot Radioactive
Ni0.75Cu0.25Al4(NO3)1.5(SO4)0.5(OH)12·14(H2O)
Molecular Weight = 765.17 gm
Monoclinic Color: Sky blue Mbobo Mkulu cave, Nelspruit district, South Africa
12 HydrowoodwarditeNot Radioactive
Cu0.5Al0.5(OH)2(SO4)0.25·0.75(H2O)
Molecular Weight = 116.81 gm
Trigonal – Hexagonal Scalenohedral
St Christoph Mine, Bärenhecke, Glashütte, Erzgebirge, Saxony, Germany
13 ManasseiteNot Radioactive
Mg6Al2(CO3)(OH)16·4(H2O)
Molecular Weight = 603.98 gm
Hexagonal – Dihexagonal Dipyramidal
Jacupiranga mine, Jacupiranga, Sao Paolo, Brazil
14 MbobomkuliteNot Radioactive
Ni0.75Cu0.25Al4(NO3)1.5(SO4)0.5(OH)12·3(H2O)
Molecular Weight = 567.00 gm
Monoclinic – SphenoidalH
Jomac Uranium mine, White Canyon, San Juan Co., Utah, USA
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15 NickelalumiteNot Radioactive
Ni0.7Cu0.3Al4(SO4)1.5(NO3)(OH)12·3(H2O)
Molecular Weight = 632.31 gm
Monoclinic – Sphenoidal
Color: Sky blue Mbobo Mkulu cave, eastern Transvaal, South Africa
16 Quintinite-2HNot Radioactive
Mg4Al2(OH)12(CO3)·4(H2O)
Molecular Weight = 487.34 gm
Hexagonal – Trapezohedral
Jacupiranga Mine, São Paulo, Southeast Region, Brazil
17 Quintinite-3TNot Radioactive
Mg4Al2(OH)12(CO3)·4(H2O)
Molecular Weight = 487.34 gm
Trigonal – Trapezohedral
Jacupiranga Mine, São Paulo, Southeast Region, Brazil
18 SpangoliteNot Radioactive
Cu6Al(SO4)(OH)12Cl·3(H2O)
Molecular Weight = 797.91 gm
Trigonal – Ditrigonal Pyramidal
Blanchard mine, Bingham, Socorro County, New Mexico, USA
19 WoodwarditeNot Radioactive
Cu4Al2(SO4)(OH)12·3(H2O)
Molecular Weight = 662.34 gm
Hexagonal Green River Formation, Uintah Co., Utah, USA
20 ZaccagnaiteNot Radioactive
Zn3.9Al2.1(OH)12(CO3)·3(H2O)
Molecular Weight = 629.83 gm
Hexagonal – Dihexagonal Dipyramidal
Hilarion Mine, Agios Konstantinos, Lavrion District, Attikí Prefecture, Greece
21 ZincaluminiteNot Radioactive
Zn6Al6(SO4)2(OH)26·5(H2O)
Molecular Weight = 1,278.62 gm
Hexagonal Kamariza Mine, Laurium, Attiki, Greece
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22 ZincowoodwarditeNot Radioactive
Zn0.47Al0.38(OH)2(SO4)0.18(H2O)0.6
Molecular Weight = 103.10 gm
Trigonal - Rhombohedral
Hilarion Mine, Agios Konstantinos, Lavrion District, Attikí Prefecture, Greece
23 Zincowoodwardite-1TNot Radioactive
Zn0.66B0.3Al0.33(OH)2(SO4)0.155·0.96(H2O)
Molecular Weight = 121.50 gm
Trigonal - Rhombohedral
Color: Pale blue, Bluish white
Laurion (Lavrion,Laurium), Greece
24 Zincowoodwardite-3RNot Radioactive
Zn0.5B0.33Al0.33(OH)2(SO4)0.2·0.59(H2O)
Molecular Weight = 109.02 gm
Trigonal - Hexagonal Scalenohedral
Color: Pale bluish white, Bluish white
Laurion (Lavrion,Laurium), Greece
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50 mL mixed solution of Mg2+
and Al 3+
NaOH 0,5 M
Synthesis of Mg/Al hydrotalcite
pH
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pH
oC120
7.00
XRD
IR
Synthesis of Mg/Al hydrotalcite (continued)
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Stability Test
pH
3; 5; 7; 9; 11; 13
50 mL
Aquadest
0.1 g Mg/Al
hydrotalcite
Shaker bath, 2 hours
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Stability Test (countinued)
oC
120
mg
198
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Purified Peat Soil or Humus
Humin(Insoluble fraction)
Fulvic Acid(Soluble)
Purified HumicAcid
Humic Acid(Precipitation)
Humic Substances
(Soluble fraction)
Pure Humic Acid(Solid)
Humic Acid(MIBK phase)
Humic Acid(Aqueous phase)
Humin(MIBK phase)
Humic Acid & Humin
(MIBK phase)Fulvic Acid
(Aqueous phase)
Peat Soil or Humus
Solvent ExtractionAlkaline Extraction
Purification
Shaking in NaOH Solvent extraction with MIBK
Ad. HClBack extractioninto NaOH
Solvent extraction with MIBK
Washing & Evap. MIBKPurification
Isolation of Humic and Fulvic Acids
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Effect of Medium Acidity on the Adsorption
50 mL Humic acid 150 mg/L
pH
3; 5; 7; 9; 11; 13
0.1 g Mg/Al hydrotalcite
Shaker bath, 2 hours
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Effect of Medium Acidity on the Adsorption (continued)
filtrateseparation
UV-Vis 400 nm
Aads Vs pH
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Rate of Adsorption
50 mL Humic acid
150 mg/L
9.00
0.1 g Mg/Al hydrotalcite
Shaker bath
minute
10, 20, 40, 60, 180, 300
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Rate of Adsorption (continued)
filtrate UV-Vis 400 nm Aads Vs t
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Adsorption Capacity
50 mL Humic acid
ppm
120, 150, 180, 210, 240
0.1 g Mg/Al hydrotalcite Shaker bath
minute
t optimum
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Adsorption Capacity (continued)
filtrate UV-Vis 400 nm Aads Vs A0
Ceq/m Vs Ceq
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25 mL NaOH 0.5
M
0.01 g humic acid + Mg/Al
hydrotalcite
Desorption
minute
5, 15, 30, 60, 120
Shaker bath separation
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Desorption (continued)
filtrate UV-Vis 400 nm
% Elution Vs t
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Characterization of Functional Group of Humic Acid
Table Distribution of oxygen containing functional groups (meq/100 g) in humic acids isolated from widely different climatic zones
Climatic zone
Tropical
Indonesia
Kalimantan Acidity Artic@ Subtropical@
South1) Central2) East3)
North Sumatera4)
Central Java5)
Others@
COOH 320 420 - 520 341 424 353 322 343 380 - 450
Phenolic OH 240 210 - 250 332 288 330 298 300 210 - 570
Alcoholic OH 490 290 6 29 6 10 n.d. 20 - 490
Total 560 630 - 770 673 712 683 619 643 560 - 890
@ Stevenson, 1982 1) Gambut district 2) Barembeng village 3) Sambutan village 4) Labuhan Batu village 5) Rawa Pening n.d.: not determined
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0 3 6 9 12 14
pH
Sta
bili
ty o
f M
g/A
l hyd
ota
lcit
e (%
)
20
80
60
40
100
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0
0.25
0.5
0.75
1
0 5 10 15
pH
Fra
cti
on
of
ad
orb
ed
an
ion
SO42-
HA
FA
Effect of Medium Acidity on the Adsorption of Anions on Mg/Al Hydrotalcite
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The Change of Medium Acidity after the Adsorption of Anions
pH pH pH Anion
Awal Akhir Anion
Awal Akhir Anion
Awal Akhir
3.0 5.1 3.0 4.2 2.9 4.6
5.0 5.7 5.0 5.1 5.0 5.3
7.0 6.2 7.0 5.6 7.3 5.9
9.0 8.1 9.0 8.4 9.3 8.4
11.0 8.9 11.0 9.2
Fulvat-
11.3 9.0
SO42-
13.0 9.3
Humat-
13.0 9.7
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Interpretation of the Adsorption Process
OH- H O2 CO32- HCO3
-
OH-
H O2
CO32-
HCO3-
M , M2+ 3+
M , M2+ 3+
OH
OH
OH
OH
+ +
Hydrotalcite Anionic sorbate (A )n- Hydrotalcite containing sorbate
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Effect of Interaction Time on the Adsorption of Anions
0
20
40
60
80
100
0 30 60 90 120 150 180
t (min)
An
ion
re
ma
ine
d (
%)
HA
SO42-
FA
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Adsorption Capacity of Mg/Al Hydrotalcite for Humic Acid
0
40
80
120
Ad
sorp
tio
n c
apac
ity
(mg
/g)
Kaolin
cla
y
Fisher
PAC D
arco
G-6
0
ALDRICH G
raphite
pow
der
Cabot V
ulcan x
c72
Cabot M
onarch
140
0
Cabot P
earls
200
0
Carbon
Chitin
Chitosan
Mg/A
l Hyd
rota
lcite
Zn/Al H
ydro
talc
ite
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0
25
50
75
100
0 60 120 180
Adsorption time (min)
%
HA
FA
0 60 120 180
Desorption time (min)
HA
FA
Regeneration of Mg/Al Hydrotalcite from Humic Acid
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Mg/Al hydrotalcite is a very potential adsorbent for the remediation of acid mine since:
1. Easy to be synthesized2. Highly stable at wide range of medium acidity3. Highly adsorb anions occurring in acid mine4. Increasing the pH of medium to close to neutral5. Easy to be regenerated
Implication:1. Dissolution of metals from soil and minerals in acid mine may be minimized2. The desorption product may be used to ameliorant
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