ELSEVIER

Journal of Geochemical Exploration 64 (1998) 215222

Geochemistry of heavy metals derived from gold-bearing sulphide

minerals in the Marmato District (Colombia)
Gloria Prieto
INGEOMINAS Diagonal 53 # 34-53, Santafe de Bogota, Colombia
Accepted 31 May 1998

Abstract
Heavy metals (Cu, Pb, Zn, Cd, Ag, As, Hg, Sb, and Bi) released from the mining and processing of gold-bearing
sulphide minerals from the Marmato District in western Colombia, were studied to determine their geochemical behaviour
and distribution in regional streams. Waters from Marmato carry appreciable dissolved metals (Zn, Cd, Cu, and As). The
concentrations of these metals and of cyanide (0.133.8 mg l 1 ) make these waters unsuitable for drinking, agriculture, or
industrial use. The concentrations of these metals in sediments and particulate matter are: 129619 g g 1 for Cu; 330
g g 1 2.28% for Pb; 1365 g g 1 1.8% for Zn; 7.6200 g g 1 for Ag; 2181850 g g 1 for As; 6.856 g g 1
for Sb; 28240 g g 1 for Cd; 95370 ng g 1 for Hg; and 4306 g g 1 for Bi. The highest values were found for the
Marmato River, while the larger Cauca River shows the lowest values, and the concentration of the metals in its sediments
reflects the contents of its tributaries. Chemical speciation shows that Cd, Zn, Pb and Bi have the highest bioavailability
potential (exchangeable fraction) while Sb and Hg do not have mobile fractions. 1998 Elsevier Science B.V. All rights
reserved.
Keywords: gold mining; heavy metals; speciation; Colombia; mine drainage; sequential extraction

1. Introduction
Colombia is one of the largest gold producers in
Latin America (INGEOMINAS, 1995). Antiquated
technological processes are used in the mining and
mineral processing of gold and result in a negative
impact on the environment (Priester et al., 1992;
Gonzalez and Prieto, 1993). Cu, Pb, Zn, Cd, Ag,
As, Hg, Sb, and Bi were selected to study their geochemical behaviour and distribution; these elements
are predominantly released by the mining activities
in the Marmato area (Marmato Gold District vein
type). The main sources of these elements are acid
Fax:

C57-1-2220824; E-mail: gprieto@trilobite.ingeomin.gov.co

mine drainage, tailings, and erosion of waste rock

deposits (Salomons, 1995). These elements enter
the streams either in dissolved form or as particulates. In the streams numerous processes take place
that change the distribution between the particulate
and dissolved phase. In particular, the dominant adsorption processes cause a transfer of the dissolved
metals to the suspended matter and deposited sediments.

2. Physiographic and geographic aspects

The Marmato District, covering approximately
76 km2 , is located in western Colombia northwest

c 1998 Elsevier Science B.V. All rights reserved.

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G. Prieto / Journal of Geochemical Exploration 64 (1998) 215222

of the Caldas Department on the east side of the

Western Cordillera. The topography of the area is
greatly dissected with irregular, steep slopes (between 45 and 60) and altitudes ranging from 680 to
2000 m.
Marmato belongs to the Tropical Dry Wood Zone
climate region (dw-T) (Espinal, 1964) with two dry
periods (summer) and two wet periods (winter).
Mean annual rainfall ranges from 1000 to 2300 mm
and the mean annual temperature is 24C (HIMAT,
1994). Most native vegetation has been destroyed
by mining activities. Because of this, agricultural
activities are currently restricted. The Marmato Hydrographic Basin comprises the Cauca and Arqua
river systems as well as some smaller streams (Marmato and Chirapoto) which are tributaries of the
Cauca River

3. Geological setting
Igneous, metamorphic, and sedimentary rocks
outcrop in the study area. Ages of these rocks range
from Palaeozoic to Tertiary. Quaternary sediments
overlay much of the area. The main geologic unites
are: the Arquia Group (Palaeozoic), a metamorphic
unit composed of schists, amphibolites and serpentinites; the Quebradagrande Formation (Mesozoic),
composed of basic igneous and sedimentary units
including ultramafic rocks, gabbros, spillites and
basalts belonging to the Cauca Ophiolitic Complex; the Amaga Formation (Tertiary), a sequence
of sedimentary rocks including arenites, argillites,
and coal beds; and the Combia Formation (Tertiary),
composed of a sequence of volcanic and pyroclastic
rocks intruded by porphyritic andesite bodies (Tertiary). Gold mineralization is concentrated in the
daciteandesite porphyry rocks (belonging to the
Marmato stock) which are the dominant unit outcropping in the area (Gonzalez, 1980).
The Marmato stock has been classified as a gold
silver epithermalmesothermal vein type deposit.
Exploitation has occurred along veins where gold
is free or associated with sulphides (mainly pyrite)
iron-rich sphalerite, galena, arsenopyrite, chalcopyrite and pyrrhotite. Free silver and pyrargyrite are
also found. Covellite is present as an alteration product (Botero and Zuluaga, 1980; Lozano and Pulido,

1986; Catano, 1990; MINERALCO, 1994; INGEOMINAS, 1995).

Four alteration zones, showing different mineral
paragenesis, are recognized at this time: a propylitic
zone (chlorite, epidote, calcite, sericite, associated
with sphalerite, pyrite, galena, Au, Ag); a phyllic
zone (sericite, quartz, with pyrite, bornite, chalcopyrite, sphalerite, galena, Au, Ag); a potassic zone
(quartz, potash feldspar, secondary biotite, sericite,
and pyrite, chalcopyrite); a supergene alteration zone
(quartz, clay minerals, iron oxides, gypsum, calcite)
and secondary malachite, azurite, and zincite (Mora
and Cuellar, 1982).

4. Methodology
A sampling program was carried out in both the
summer and winter seasons. Surface waters, sediments and suspended sediments (particulate matter) were collected in streams (Aguas Claras, QAc;
Cascabel, QCa; Pantanos, QPa; Marmato, QM; Arqua, QAr; Chirapoto, QChi), mine drainages (DM1
and DM2), and processing effluents from Marmato
(E1 and E2), and in the Cauca River (6 sampling
stations located upstream and downstream of Marmato). Aguas Claras was used as a reference stream,
since it is still in a pristine state. Temperature, pH,
conductivity, turbidity, sulphides and flow were determined in situ. Cyanide (total and free), chemical oxygen demand (COD), total organic carbon
(TOC), total solids (TS), dissolved solids (DS), ammonium (NH3 ), chloride, cations (NaC , KC , Ca2C ,
Mg2C ), and dissolved metals (Cu, Pb, Zn, Cd, Ag,
As, Hg, Sb and Cd) were determined. Heavy metals (total strong acid digestion) and the bioavailable fraction (leaching with 0.1 N HCl) were analyzed in sediments and suspended particulate matter. The distribution of the metals over the various
phases was studied with selective extraction methods
using Tessiers speciation methodology (Tessier et
al., 1979). The fractions obtained with this scheme
are: F1-exchangeable (exchangeable ions), F2-carbonatic (carbonates), F3-reducible (Fe, Mn-oxides),
F4-sulphidic=organic (sulphides and organic matter),
and F5-residual (lithogenic crystallites). In this way
it was possible to distinguish between geochemically
reactive and non-reactive (inert) fractions.

G. Prieto / Journal of Geochemical Exploration 64 (1998) 215222

5. Results and discussion

The results show that some water quality criteria
are exceeded, (USEPA, 1976; OPS, 1987). Marmato
streams carry high levels of metals in solution, particularly Zn, Cd, Cu and As. The high concentrations
of cyanide and total suspended solids make the waters from the Marmato area unsuitable for drinking,
agricultural irrigation, aquatic life or industrial use
(cyanide 0.133.8 mg l 1 ; TS 942239,952 mg l 1 ).
The Aguas Claras stream, serving as a baseline,
shows the lowest values of TS (199 mg l 1 ), conductivity (259 S cm 1 ), and the lowest concentration
of heavy metals in its sediments. Its pH (7.5) is basic, and is explained by the presence of calcareous
minerals in this area.
In active mines, oxidation of sulphide minerals
takes place and produces acid mine drainage (DM1
pH 2.93.5 and DM2 pH 4.4) which are neutralized
by effluents of the milling and processing steps (E1
pH 4.48.7 and E2 pH 6.48.3). The effluents are
alkaline, probably due to residual carbonates, lime,
and organic additives of processing. The Marmato
stream that receives the entire drainage of the mining area and flows into the Cauca River is neutral,
showing that some buffering is taking place. The discharge of tailings and increased erosion in the area
are reflected in the high TS levels of the streams.
COD and NH3 show positive correlations to cyanide
concentrations, which imply that these parameters
reflect the decay of cyanides in the system.
Heavy metals are enriched in sediments and particulate suspended matter from the Marmato Area
(Table 1). Their levels have ranges as follows: 129
619 g g 1 , Cu; 330 g g 1 2.28%, Pb; 1365 g
g-1 1.18%, Zn; 7.6200 g g 1 , Ag; 2181850 g
g 1 , As; 6.856 g g 1 , Sb; 28240 g g 1 , Cd;
95370 ng g 1 , Hg, and 4306 g g 1 , Bi. The
highest values were found in the Marmato River.
The Arqua and Chirapoto streams have lower values. The elevated Marmato values reflect the mining
activities in the watershed, and reveal the contribution of sulphide minerals from the ore body (pyrite,
sphalerite cadmian, galena bismuthian, chalcopyrite,
arsenopyrite, argentopiryte, siderite, pyrrhotite, and
pyrargyrite).
In both the Marmato and Arqua streams, Sb and
Hg are low in bioavailability (0% mobilized by 0.1

217

N HCl) (Table 2). Among the other metals, As possesses the lowest mobility (3.214.2%); Cu has a
low mobile fraction except in the mining drainages;
while Cd, Bi, Zn, Ag and Pb exhibit an appreciable bioavailable fraction (8.290.9%). Chemical
speciation (Fig. 1, Table 3) shows that Cd, Zn, Pb
and Bi have the highest bioavailability potential and
could be transferred from sediments and suspended
matter into other environments. Copper is mainly
associated with the residual fraction (5690%) and
in lower percentages with carbonates (425%) and
organics and sulphides (425%). Lead is associated
to the reducible (1375%) and residual (1682%)
species, and to a lesser percentage with carbonates, sulphides and the exchangeable fraction. Zinc
is mainly associated with the organic and sulphide
fractions (1364%) and to a lesser proportion with
residual (947%) and reducible (1033%) forms.
Exchangeable or loosely held Zn is noticeable (up
to 6%). Cadmium is associated with the residual
fraction (3161%), with organics and sulphides (14
34%), and with the exchangeable fraction (414%).
Antimony is associated mainly with the residual
fraction (3986%), and to a lesser degree with carbonates (1440%). Bismuth is associated with the
reducible fraction (1873%) and to carbonates (13
50%).
The Cauca River shows lower metal concentrations than any of the streams and presumably this
reflects the contents of its tributaries (Table 1). The
Cauca River has values for solids (TS 208234
mg l 1 ) and turbidity (40.862.7 NTU) which is in
agreement with values for other natural rivers that
carry loads of erosive materials. Its pH is in the
neutral range for natural waters (7.27.4). Antimony,
Hg, and Bi do not show a mobile fraction in the
Cauca River (Table 2). Antimony is chiefly associated to the residual fraction (65100%), while Bi
is associated to carbonates and reducible and residual forms (2074%) (Table 3). In comparison to
Marmato, Pb and Cu exhibit greater mobility (Pb
up to 100% and Cu 2953%). Copper is associated
with the residual fraction (4962%), and in lower
percentages to the reducible and organic and sulphide fractions. Lead is mainly associated with the
reducible fraction (8092%), and shows a greater
association with the exchangeable or loosely held
fraction (1.36.5%). This latter relation possibly re-

218

G. Prieto / Journal of Geochemical Exploration 64 (1998) 215222

Table 1
Total concentration of metals in suspended sediments of the Marmato District, western Colombia (strong acid digestion)
Sample

Au (ppb) Ag (ppm) Cu (ppm) Pb (ppm) Zn (ppm) As (ppm) Hg (ppb) Cd (ppm) Sb (ppm) Bi (ppm)
(LD D 10) (LD D 0.2) (LD D 1.0) (LD D 1.0) (LD D 1.0) (LD D 2.0) (LD D 10) (LD D 1.0) (LD D 2.0) (LD D 2)

Sediments from Marmato first sampling (summer)

QAc
2580
21
133
450
QAc
2930
32
241
880
E1
1150
17
125
470
E1
1680
37.6
431
760
DM1
240
9
207
550
DM1
1380
11.4
164
352
QCa
15.22 a
55
551
1300
E2
1880
>200
578
2.28%
DM2
450
13.8
342
550
QPa
3120
45
619
2400
QM
2780
37
439
1280
QAr
110
1.4
60
98
QAr
2
81
104
QChi
20
<0.2
81
16

2750
4210
2390
1.8%
2750
5510
1.16%
5290
2740
5120
5720
234
262
162

Sediments from Marmato second

Range
Marmato 6703870 1235
DM1
3420
18
QCa
3280
28.4
E2
3870
35
QPa
2300
28.8
QM
670
12
QAr
590
2.4

43006140 4601400
4640
630
6140
1050
5780
940
5220
1400
4300
460
236
440

770
700
320
850
180
256
1610
1400
1100
1850
1600
180
140
10

550
190
70
120
300
60
110
310
510
160
130
160
160
130

52.5
83.5
46.5
308
81
110
240
118
48.5
111
119.5
3.5
4.5
1.0

8.8
10
6
9.2
8
5.6
9.2
56
15
15
11
13.5
11
3.6

4
16
10
22
10
2
30
306
8
22
22
<2
4
4

130540
540
130
290
380
190
160

95134
95
127
134
122
95.5
7.5

6.611
10
8
9.8
11
6.6
32

1634
16
18
34
34
16
<2

0.62.8
0.6
2.8
1.2
1.6
1.2

<22
<2
2.0
<2
<2
<2

1.211
1.2
1.2
1.6
11
1.6
1.8

<22
2
<2
<2
<2
<2
2

sampling (winter)
224396
224
283
396
322
334
93

4001700
540
760
1700
1340
400
270

Sediments from Cauca

Range
<10330
RcaM
<10
RCdM
330
RcaAr
20
RcaChi
70
RCdChi
<10

River first sampling (summer)

<0.22.2
3062
1268
<0.2
30
12
2.2
62
68
<0.2
33
20
1.0
55
40
<0.2
35
14

74732
74
732
210
418
174

490
4
90
14
42
18

50150
50
90
150
90
70

0.513
0.5
13
3.0
7.0
1.5

Sediments from Cauca

Range
20330
RCaM
100
RCdM
30
RCaAr
20
RCdAr
330
RCdChi
20
RCaArm
30

River second sampling (winter)

<0.28.8
2844
4224
<0.2
43
4
<0.2
41
16
0.2
37
16
8.8
28
224
<0.2
44
6
<0.2
38
4

124548
124
132
156
548
174
146

10256
10
12
20
256
12
14

601520
100
70
60
1520
120
70

0.54
0.5
1.5
2.0
4
1
2

a Concentration

ppm.
LD D limit of detemination, QAc D Aguas Claras stream, E1 D processing effluent, E2 D processing effluent, QPa D Pantanos
stream, DM1 D mine drainage, DM2 D mine drainage, QM D Marmato stream, QAr D Arqua stream, QChi D Chirapoto stream,
RCaM D Cauca River 2 km upstream Marmato, RCdM D Cauca River 0.5 km downstream Marmato, RCaAr D Cauca River 0.5 km
upstream Arqua and 2.8 km downstream Marmato, RCdAr D Cauca River 0.5 km downstream Arqua, RCdChi D Cauca River 0.5
km downstream Chirapoto and 12 km downstream Marmato, RCaArm D Cauca River 0.5 km upstream Armas River and 28.5 km
downstream Marmato (last sampling station).

G. Prieto / Journal of Geochemical Exploration 64 (1998) 215222

219

Table 2
Bioavailable fraction of metals in suspended sediments of the Marmato District, western Colombia (leached with 0.1 N HCl)
Sample

Ag (ppm)
Cu (ppm)
Pb (ppm)
Zn (ppm)
As (ppm)
Hg (ppb)
Cd (ppm)
Sb (ppm)
Bi (ppm)
(LD D 0.2) (LD D 1.0) (LD D 2.0) (LD D 1.0) (LD D 2.0) (LD D 10) (LD D 0.5) (LD D 2.0) (LD D 2)

Sediment from Marmato first sampling (summer)

QAc
9.0
27
378
QAc
14.0
92
330
E1
10.2
43
110
E1
2.4
14
600
DM1
6.6
165
38
DM1
5.6
43
80
QCa
7.6
61
732
E2
3.2
11
5880
DM2
12.8
209
196
QPa
7.8
28
204
QM
6.8
43
646
QAr
1.2
23
26
QAr
1.8
25
32
QChi
0.4
30
8

1530
2520
1210
3740
2320
3050
3270
1195
2470
1520
1780
106
102
50

48
54
12
44
28
34
66
58
42
74
56
6
<2
<2

<10
<10
<10
<10
<10
<10
<10
<10
<10
<10
<10
<10
<10
<10

Sediments from Marmato second sampling (winter)

Range Marmato
0.622
721
26432
DM1
2.2
21
26
QCa
1.8
21
318
E2
1.2
15
432
QPa
0.6
7
300
QM
0.6
16
190
QAr
0.2
16
30

2241720
1720
476
334
224
486
26

432
32
20
8
4
10
14

<10
<10
<10
<10
<10
<10
<10

Sediments from Cauca River first sampling (summer)

Range
<0.20.8
1633
<248
32298
RCaM
<0.2
16
<2
32
RCdM
0.8
18
48
298
RcaAr
<0.2
16
12
94
RcaChi
0.4
33
28
130
RcdChi
0.2
17
6
72

<24
<2
4
2
<2
<2

Sediments from Cauca River second sampling (winter)

Range
<0.21
610
290
RCaM
<0.2
10
4
RCdM
<0.2
7
2
RcaAr
<0.2
7
4
RcdAr
1
6
90
RcdChi
<0.2
9
4
RcaArm
<0.2
8
2

<218
<2
<2
<2
18
<2
<2

16136
26
16
16
136
18
16

<2
<2
<2
<2
<2
<2
<2
<2
<2
<2
<2
<2
<2
<2

7
10
2
12
2
3
21
25
3
20
16
<2
<2
<2

ND
ND
ND
ND
ND
ND
ND

<2
<2
<2
<2
<2
<2
<2

28
2
8
8
6
6
<2

<10
<10
<10
<10
<10
<10

<0.54
<0.5
4.0
1.0
1.5
0.5

<2
<2
<2
<2
<2
<2

<2
<2
<2
<2
<2
<2

<10
<10
<10
<10
<10
<10
<10

ND
ND
ND
ND
ND
ND
ND

<2
<2
<2
<2
<2
<2
<2

<2
<2
<2
<2
<2
<2
<2

25.5
49.5
22.0
14.0
74.5
55.5
67.0
24.0
39.0
30.0
33.5
3.0
3.5
0.5

LD D limit of determination.
Site abbreviations explained in legend for Table 1.

flects the contribution from gasoline combustion in

this region from automobile exhaust. Zinc shows
a mobile fraction between 1045% and is mainly
associated with the reducible (2341%) and residual (751%) fractions. The mobile fraction of Cd
ranges from 033% and is mostly associated with
the residual fraction (75100%).

6. Conclusions
In active mines near Marmato, oxidation of sulphides occurs and produces acid mine drainage
which is neutralized by processing effluents. Waters from Marmato, however, are not suitable for
drinking, agricultural irrigation, or industrial use.

220

G. Prieto / Journal of Geochemical Exploration 64 (1998) 215222

Fig. 1. Fractionation of metal concentrations in sediments and suspended matter of the Marmato District, western Colombia (Tessier et
al., 1979). QAc D Aguas Claras stream; QM D Marmato stream; QAr D Arqua stream; E2 D processing effluent; RCaM D Cauca river
2 km upstream Marmato; RCdChi D Cauca River 0.5 km downstream Chirapoto (left) and 12 km downstream Marmato (right); RCaArm
D Cauca River 0.5 km upstream Armas River and 28.5 km downstream Marmato (last sampling station); SM D suspended matter; F1 D
exchangeable; F2 D carbonitic; F3 D reducible (Fe, Mn oxides); F4 D sulphidic=organic; F5 D residual.

G. Prieto / Journal of Geochemical Exploration 64 (1998) 215222

221

Table 3
Chemical speciation of metals in bottom sediment and suspended matter of the Marmato District, western Colombia (following Tessier
et al., 1979)
Sample

F1
Cu (g g

QAc
E2 (SM)
QM
QM (SM)
QAr
RCaM
RCdChi
RCdChi (SM)
RCaArm

F2

F3

F4

F5

F1

1)

7.9
<0.1
<0.1
<0.1
<0.1
0.6
<0.1
<0.1
<0.1

Pb (g g
7.9
<0.1
<0.1
<0.1
<0.1
0.6
<0.1
<0.1
<0.1

9.5
3.0
5.6
4.0
18.5
13.2
8.6
9.2
9.2

9.5
4.0
5.8
4.0
8.6
13.2
8.6
9.2
9.6

94
9.0
105
97
48
26
25
30
27

Zn (g g 1 )
QAc
E2 (SM)
QM
QM (SM)
QAr
RCaM
RCdChi
RCdChi (SM)
RCaArm

185
1.8
53
1.6
4.6
1
<0.1
<0.1
<0.1
<20
<20
46
<20
<20
<20
<20
<20
<20

F3

F4

F5

0.20
0.45
0.13
0.23
0.39
0.13
0.09
0.23
0.40

12
16
41
22
<5
<5
<5
<5
<5

93
154
268
164
22
8
6
6
5

1.7
3.3
2.7
5.5
1.1
<0.1
0.2
0.2
<0.1

1.7
3.3
2.7
5.5
1.1
<0.1
0.2
0.2
<0.1

3.1
0.75
1.22
0.65
1.91
0.51
0.69
0.74
0.8

511
34
105
108
141
<10
<10
<10
<10

Cd (g g 1 )
53
259
158
190
9
6
17
17
7

324
574
496
1092
66
50
40
52
31

1800
2000
2170
1884
26
20
34
36
28

800
292
963
618
93
50
7
75
69

Sb (g g 1 )
QAc
E2 (SM)
QM
QM (SM)
QAr
RCaM
RCdChi
RCdChi (SM)
RCaArm

F2
1)

800
345
850
430
300
<20
375
50
340

5.6
0.9
4.4
4.2
0.4
0.4
0.1
<0.1
<0.1

6.0
6.3
5.2
8.4
2.8
0.4
<0.5
<0.5
<0.5

23.8
8.5
22.5
10.8
2.7
2.4
2.4
2.7
2.9

Bi (g g 1 )
45
56
93
149
<25
<25
<25
<25
<25

<25
<25
290
<25
<25
<25
<25
<25
<25

3100
750
850
650
1910
510
690
740
800

30
20
30
<10
<10
<10
<10
<10
<10

720
311
774
389
272
<10
350
46
319

3500
400
3300
900
100
100
100
<50
100

<25
<25
238
<25
<25
<25
<25
<25
<25

1124
35
141
386
176
35
35
105
316

Site abbreviations explained in legend of Table 1. SM D suspended matter.

Heavy metals are enriched in sediments and

particulate matter from the Marmato region. Their
values reflect the mining activities and reveal the
contribution of sulphide minerals from the ore
body (pyrite, sphalerite cadmian, galena bismuthian,
chalcopyrite, arsenopyrite, siderite, pyrrhotite). Cadmium, Zn, Pb and Bi exhibit appreciable bioavailability while Sb and Hg are not mobile metals,
associated instead with the residual fraction.
Due to the high discharge (605641 m3 s 1 ) of
the Cauca River, mine effluent inputs have been
diluted to a significant extent. The fast rate of flow
and pH values mean that geochemical reactions in
this region of the Cauca Fiver are probably slower

than in other tropical river systems. Further, some

of these interactions are probably operating further
downstream from the Marmato area.

Acknowledgements
I gratefully acknowledge the financial assistance of the German Academic Exchange Service
DAAD as well as INGEOMINAS, Colombia. I
thank the professors and colleagues of the Universidade Federal do Para, Universidade Federal Fluminense, Brazil and Martin Luther Universitat, Institut
fur Geologische Wissenschaften, Germany. Special

222

G. Prieto / Journal of Geochemical Exploration 64 (1998) 215222

thanks to my professors Drs. Marcondes Lima da

Costa, Brazil and H. Pollmann, Germany. Also to the
administrative staff and colleagues from the Mining
and Chemistry Areas of INGEOMINAS. Thanks to
Drs. I.F. Brown, L.P. Gough and the anonymous referees for their constructive comments on the original
version of the manuscript.

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