Environmental Science and Pollution Research

https://doi.org/10.1007/s11356-020-11157-5

RESEARCH ARTICLE

Heavy metal pollution and mobility of sediment in Tajum River

caused by artisanal gold mining in Banyumas, Central Java, Indonesia
Wawan Budianta 1

Received: 15 May 2020 / Accepted: 5 October 2020

# Springer-Verlag GmbH Germany, part of Springer Nature 2020

Abstract
The heavy metals Cu, Pb, Zn, and Cd in the stream sediment of the Tajum River were studied based on 12 sediment samples
obtained from upstream to downstream. The artisanal mining activities in the study area generated mining processing waste
(tailing) and are the primary source of heavy metal pollution. The samples were analyzed for metal concentration as well as metal
mobility based on sequential extraction analysis. Heavy metal analysis for the concentration of the metals showed that the value
of Cu, Pb, Zn, and Cd in sediment samples transcends the mean crust. The change of the heavy metal concentrations in stream
sediment between the upstream and downstream areas showed that higher levels were located near mining activities in upstream
and that these decreased with distance to downstream. The result of the sequential extraction study revealed that Cu and Pb were
more found in the exchangeable and carbonate fraction of about 26% and 24%. Meanwhile, Zn and Cd were present in the Fe–
Mn oxide, an organic and residual fraction of about 90% and 85%, respectively. The mobility factor assessment revealed that the
heavy metals investigated had an average mobility factor of 25.89%, 23.9%, 14.4 %, and 9.24% for Cu, Pb, Zn, and Cd,
respectively. Overall, Zn and Cd in sediment in the study area were less mobile compared with Cu and Pb.

Keywords Heavy metals . Pollution . Mobility . River sediment . Artisanal . Mining

Introduction activities have negative effects on the environment, especially

Indonesia has a high number of artisanal gold mining facilities
(Aspinall 2001; Reilly et al. 2016), one of them located in the
Paningkaban area of the Banyumas District in Central Java,
Indonesia (Fig. 1). Artisanal mining processing activities in
the study area include rock crushing, grinding, milling, and
washing. This area is located in a hilly region and traversed by
the Tajum River, which is used by residents as a source of
irrigation water as well as for washing and bathing (Fig. 1). In
the study area, the tailings are collected into small pits or
ponds near to the processing plants. These ponds are built into
the ground, and the processing waste goes directly into the
river. Several studies indicated that artisanal gold mining
Responsible Editor: Philippe Garrigues
* Wawan Budianta
wbudianta@ugm.ac.id
1 2019; Santos et al. 2020). Therefore, this research was con-
Department of Geological Engineering, Faculty of Engineering,
Universitas Gadjah Mada, Jl. Grafika 2 Kampus UGM,
Yogyakarta, Indonesia
in aquatic systems located around the facility (Yolcubal et al.
2016; Li et al. 2011). The impact of mercury concentrations in
river water and stream sediment in the study area was well
documented in a previous investigation (Budianta et al. 2019).
In addition to mercury contamination, the activities of arti-
sanal gold mining can cause other heavy metal pollution, es-
pecially in river sediments around the facilities (Karbassi et al.
2008; Klubi et al. 2020; Aghili et al. 2018). Heavy metals in
the river sediment in high concentrations will disturb and con-
taminate aquatic biota in river systems (Li et al. 2020;
Xiaohong et al. 2019). Evaluation and assessment of metal
contamination and mobility must be investigated by
conducting sequential extraction analysis because measure-
ment of the total concentration of heavy metals in the sample
only is not sufficient (Naji et al. 2010; Khadhar et al. 2020;
Tüzen 2003; Tessier et al. 1979). Stream sediment in aquatic
systems is significant not only for serving as sinks of these
contaminants that release them under certain physical and
chemical but also to the adsorption of heavy metals (Li et al.
ducted to analyze the levels and mobility of heavy metals in
the Tajum River sediment in the study area.

Fig. 1 The location of the study area
Geology and hydrology
The rocks of the study area belong to the Halang formation,
which consists of turbidite sedimentary units (Djuri et al.
1996). Prihatmoko et al. (2002) reported that a quartz-
carbonate mineralization process occurred in the rock in the
Halang formation, which was of middle Miocene age. In the
study area, as reported by Hakim (2014), the rock unit area
consists of limestone, claystone–siltstone, and tuff clay (Fig.
Environ Sci Pollut Res
2). The ore deposits present in the research area are low
sulfidation epithermal type and occur in carbonate-based met-
al-gold mineralization systems (Hakim 2014). The sandstone
and siltstone unit is the host rock of epithermal gold mineral-
ization in the study area. Vein structures are present, indicat-
ing the accumulation of precious and other metals associated
to sulfide mineral such as pyrite, chalcopyrite, sphalerite, ga-
lena, and arsenopyrite (Hakim 2014). The heavy metals on
river sediment in this study area were derived from this accu-
mulation process. The study area is situated in a tropical area
subjected to a rainy season with high rainfall and a dry season.
Tajum River is the primary river, and the flow direction is
north-west, then turns south-west, and finally to the south
(Fig. 2). This pattern of river flow follows the morphology
of the area because of the influence of tectonic processes
and erosion, which have resulted in a narrow V-shaped river
valley. The Tajum River has a wide variety of discharge rate
during rainy and dry seasons. The sampling collection was
conducted during the dry season, with the stream discharge
relatively low.
Materials and methods
Twelve river sediment samples were taken in the study area
systematically from upstream to downstream in the Tajum
River, as shown in Fig. 2. A tailing sample was taken from a
tailing pond near mining processing site. Sample S-1
representing the natural background metal concentration value
was obtained from the furthest upstream, which was assumed
not to be contaminated by processing waste of artisanal min-
ing activities.
The river sediment samples were dried in an oven of 105
°C for 24 h. The sediment sample was sieved, and the fraction
< 63 μm was grounded to powder by using an agate mortar.
The powdered sample of approximately 0.5 g weight was then
transferred in a glass beaker with 10 mL aqua regia. The
samples were then heated to dryness. Hydrofluoric acid (5
mL) was added after the mixture was cooled at room temper-
ature. Later, the mixture was filtered by 0.45-μm membrane
filter. After filtering, the filtrates were placed into 50-mL vol-
umetric flasks after addition of 1 N HCl.
Chemical partitioning was investigated in sequential steps
as described by Tessier et al. (1979), which separate the sam-
ple in five fractions, namely exchangeable fraction, bound to
carbonates fraction, bound to Fe–Mn oxides fraction, bound
to sulfides and organic matter fraction, and residual fraction.
Before use, containers and sample bottles used in this exper-
iment were washed in HNO3 (10%) and then soaked with
distilled water. All metals (Cu, Pb, Zn, and Cd) were mea-
sured by an ICP-OES (inductively coupled plasma–optical
emission spectrometry). Calibration was conducted using a
reference material of the Canadian Certified Reference
Environ Sci Pollut Res

Fig. 2 Geological conditions (Hakim 2014) and sediment sampling location points

Materials Project (CRMs). A calibration blank (2% HNO3)
was run before the standards, and a multi-elemental solution
was used. The concentration corresponding to three times the
standard deviation of the intensities of the blank signals for
each component were used for detection limits determination.
processing waste generation (S-3 through S-9). The variability
indicates the significant impact of artisanal mining activities,
which generated processing waste. Processing waste of metal
ores can be a significant source of sediment pollution. Mining
processing, which involves grinding and milling, ore

Results and discussion Table 1 The heavy metal concentrations in river sediments and tailing
(mg/kg)
Heavy metal concentration Sample code Cu Pb Zn Cd

The information on the metal concentrations in the river sed- S-1 87 34 85 2.5
iment samples is shown in Table 1. Sample S-1 referred to a S-2 95 56 350 3.5
control sample from an upstream point that was assumed not S-3 135 46 450 5
to be contaminated by mining processing waste generation S-4 190 78 480 5
(Fig. 2). S-5 210 81 550 6.5
The background of metal level (S-1 sample) was higher S-6 190 85 450 6
than the mean crust levels (Table 1) because of the presence S-7 130 85 350 7
of a mineralization zone in the study area that is enriched with S-8 120 110 250 6
metal sulfides. According to Hakim (2014), the mineralization S-9 100 76 400 5
type in the study area is typical of low epithermal sulfidation, S-10 91 75 90 3
especially for a carbonate-based metal-gold mineralization S-11 101 71 90 2.5
system. The heavy metal contents in the tailing sample was S-12 96 65 83 1.5
also higher than the average of heavy metals in sediments, and Min 87 34 83 1.5
tailings may therefore serve as the primary source of heavy Max 210 110 550 6.5
metal pollution in stream sediment in the study area. The Mean 128.75 71.83 286.5 4.46
lower sediment metal concentrations were found on S-1 and Tailing 267 143 785 8.9
S-2 samples (upper stream) and S-10 through S-12 (lower Mean crusta 25 14.8 65 0.1
stream). The higher concentrations were found in the middle,
a
which was located close to artisanal mining activities and Wedepohl (1995)

concentration, and tailings disposal, provides significant
sources of contamination in the stream sediment, along with
the discharge of processing waste (Dudka and Adriano 1997).
Consequently, streams transport high contents of Pb, Cu, Zn,
and Cd. It seems that stream sediment in the study area could
be polluted with heavy metals, in which processing mining
waste is the primary source that increases the content of heavy
metals disposed into the river water.
The variation in the metal concentrations in river sediment
from upstream to downstream is shown in Fig. 3. Generally,
the pattern of the metal concentrations in river sediment sam-
ples followed the highest concentrations located near the min-
ing activities, after which the metal concentrations were get-
ting lower. The decrease in metal concentrations along the
stream illustrated that the sediment transport follows the river
stream and slope of the river basin. This process contributes to
the dispersion of metals in sediments along the flow direction,
as shown in Fig. 2.
There were several artisanal mining facilities located in the
study area (Fig. 2) that date back more than 10 years. The
activity of these artisanal mining has generated processing
wastes, which are transported into the encompassing environ-
ment and release Cu, Pb, Zn, and Cd that were enriched in the
mineralized host rock.
Artisanal mining, as one of the anthropogenic activities,
has generated the transport of metals like Cu, Pb, Zn, and
Cd downgradient from their source, possibly as sorbed
constituent materials. Furthermore, the distribution pattern
of Cu, Pb, Zn, and Cd investigated in this study points to
metal dispersion over at least 4000 m to downstream by
river water flow (Fig. 3). Several studies reported that the
heavy metal accumulation in stream sediment around min-
ing areas was highest near to the mining activities
(Adewumi and Laniyan 2020; Chen et al. 2019; Niane
et al. 2014; Resongles et al. 2014).
Other studies indicate that the heavy metal concentration of
stream sediment in the downstream decreases, which may be
Fig. 3 The change of heavy metal
concentrations in upstream to
downstream of Tajum river
sediment
Environ Sci Pollut Res
attributed to physical and chemical processes such as dilution
of contaminated sediment, hydraulic sorting of channel bed
sediment, abrasion of polluted sediment grains, polluted sed-
iment particles in floodplain deposits repository, sorption or
co-precipitation of metals, and changes in metals in phases
such as Fe and Mn oxides in downstream (Macklin 1996;
Hudson-Edwards et al. 2001; Hudson-Edwards 2003).
The mobility of heavy metals
Metals’ chemical speciation based on sequential extraction is
important to their mobility, as stated by Tessier et al. (1979).
The fraction of heavy metals obtained from the extraction
varied extensively in the current study, as shown in Table 2
and Fig. 4.
The two first fractions represent the fraction of exchange-
able, reducible, and oxidizable elements. They likely contain
metals that may be mobilized to the aqueous phase by chang-
ing redox conditions, and contrary from oxidizing to reducing
conditions (Byrne et al. 2012). Heavy metals may be
transported to downstream of the river system in the dissolved
phase or change to another solid phase (Audry et al. 2010;
Byrne et al. 2012).
Sequential extraction revealed that Cu was mostly found
(about 26%) in the two first fractions, i.e. exchangeable and
bound to carbonate bound. The abundance of Cu in the Fe–
Mn oxide, organic, and residual fractions was about 74%. Pb
was found on the Fe–Mn oxide, organic, and residual frac-
tions, with an average level of about 76% (Fig. 4).
These findings indicate that Pb was more mobile than Cu.
Zn was primarily found in the Fe–Mn oxide, organic matter,
and residual fractions of all samples. In the Fe–Mn oxide,
organic matter, and residual fractions, the presence of Zn
was about 90% on average. In comparison, it was about
10% on average in the exchangeable and the carbonate frac-
tion (Fig. 4). These results indicate that Zn was more immo-
bile compared with the other metals.
 Environ Sci Pollut Res

Table 2 Chemical partitioning of heavy metals in river sediments in the study area (mg/kg)

Sample code Cu Pb Zn Cd

I II III IV V Sum I II III IV V Sum I II III IV V Sum I II III IV V Sum

S-1 8.0 17.2 22.0 30.5 9.0 86.7 2.0 6.2 7.0 9.0 10.0 34.2 2.0 10.0 17.0 12.0 31.3 72.3 0.1 0.1 0.3 1.0 0.9 2.4
S-2 22.0 13.7 32.0 15.0 12.0 94.7 4.0 14.2 8.0 15.0 15.0 56.2 5.0 45.0 45.0 80.0 175.2 350.2 0.6 0.7 0.4 0.6 1.3 3.6
S-3 11.8 23.0 45.0 21.0 34.0 134.8 9.0 9.1 8.0 9.0 12.0 47.1 9.0 12.0 98.0 99.9 231.0 449.9 0.4 0.4 1.1 1.0 2.0 4.9
S-4 33.8 24.7 56.3 34.0 41.0 189.8 8.0 12.1 6.0 18.0 34.0 78.1 11.0 45.0 43.0 167.2 214.0 480.2 0.1 0.3 1.1 1.1 2.3 4.9
S-5 12.1 44.1 51.0 47.0 56.0 210.2 6.0 6.1 13.0 27.0 29.0 81.1 18.0 32.0 70.0 212.0 223.2 555.2 0.1 0.8 1.1 2.0 2.7 6.7
S-6 20.0 56.0 44.0 34.0 36.0 190.0 4.0 23.1 13.0 23.0 21.0 84.1 9.0 12.0 67.0 189.2 173.0 450.2 0.1 0.5 0.5 1.0 1.8 3.9
S-7 6.1 30.8 47.0 12.0 33.7 129.6 7.1 21.0 12.0 21.0 24.0 85.1 10.0 10.0 34.0 167.2 129.0 350.2 0.0 0.9 3.1 1.8 1.1 6.9
S-8 4.1 21.1 39.0 33.0 23.0 120.2 2.0 16.8 12.0 12.0 67.0 109.8 4.0 10.1 15.0 31.0 190.0 250.1 0.1 0.9 2.0 1.3 1.8 6.1
S-9 14.0 11.7 34.0 28.0 12.0 99.7 7.9 12.0 21.0 23.0 12.0 75.9 8.0 9.1 12.0 153.0 218.0 400.1 0.0 0.1 0.7 1.9 2.2 4.9
S-10 2.9 27.0 17.8 12.0 31.0 90.7 4.1 9.0 18.0 21.0 23.0 75.1 4.0 5.1 15.0 21.0 45.0 90.1 0.1 0.2 0.2 0.8 1.6 2.9
S-11 4.0 11.1 34.0 19.0 32.0 100.1 3.1 8.0 23.0 19.0 18.0 71.1 4.0 6.2 21.0 23.0 36.0 90.2 0.1 0.1 0.4 0.6 1.2 2.4
S-12 5.0 8.9 45.0 18.0 19.0 95.9 4.0 3.1 25.0 17.0 16.0 65.1 6.0 5.0 10.0 43.0 19.3 83.3 0.0 0.1 0.3 0.4 0.6 1.4

I, exchangeable; II, bound to carbonates; III, bound to Fe–Mn oxides; IV, bound to sulfides and organic matter; V, residual

Fig. 4 Cumulative value of
chemical partitioning of heavy
metals speciation in river
sediments in the study area
A similar pattern was also observed for Cd, which was
mostly bound to Fe–Mn oxide and organic matter with an
amount of 47% and present in the residual fraction with an
amount of about 38% average (Fig. 4). The amount of Zn and
Cd in other fractions was relatively low compared with Cu and
Pb. In the environment, Zn and Cd were more immobile com-
pared with the metals that were particularly found in Fe–Mn
oxide, organic, and residual fractions. Sequential extraction
revealed that the highest amount in the Fe–Mn oxide, organic,
and residual fractions was Cu–74%, Pb–76%, Zn–85%, and
Cd–90%. These findings were confirmed by the finding of
another researchers, in which Cd and Zn were primarily asso-
ciated with the residual phase (Ramirez et al. 2005; Sundaray
et al. 2011; El-Azim and El-Moselhy 2005; Li 2014;
Venkatramanan et al. 2015).
The mobility of sediment samples revealed that the abun-
dance of the Cd and Zn were strongly adsorbed in the organic
and residual fraction. Cd and Zn in sediment samples are
Environ Sci Pollut Res
incorporated in the crystal lattices of clay with strong bonds
and not efficiently released into the environment accordingly
(Violante et al. 2010).
Previous studies state that the high concentrations of the
heavy metals in the Fe–Mn oxide, organic, and residual frac-
tions in geochemical phase indicate that the metals that remain
in sediments were mainly of geogenic origin (Davutluoglu
et al. 2011). There is a potential risk of heavy metals becoming
chemically mobile caused by a change of environmental con-
ditions, since a significant amount of metals can be released
from the Fe–Mn oxides and organic phases (Davutluoglu et al.
2011; Wang et al. 2010; Papadopoulos et al. 1997).
Based on the results of the sequential extraction study, the
heavy metal investigated in this study was not only of
geogenic origin due to mining activities but also may be in-
fluenced by mining processing waste generation as an anthro-
pogenic factor. Generally, the slightly high amount in the Fe–
Mn oxide, organic, and residual fractions indicates that the
Environ Sci Pollut Res

metals were not derived from the anthropogenic origin
(Venkatramanan et al. 2015).
Heavy metal analysis revealed high concentrations com-
pared with reference samples because of anthropogenic influ-
ences on geogenic sources, such as artisanal mining activities,
which generated mining processing waste in the study area.
This confirms the conclusion of another study (Sims and
Francis 2010).
Mobility factor
Heavy metal mobility determination is calculated using pro-
portions of the metal fractions. The partitioning variation of
the metals was classified into two groups based on the level of
their affiliation with particular phases and would be used for
mobility index determination. The groups are the exchange-
able and carbonate fractions as a mobile group, while Fe–Mn
oxide, organic, and residual fractions represent the immobile
group. The heavy metal mobility index was determined as the
mobility factor (Mf), which is calculated referring to the equa-
tion by Kabala and Singh (2001).
M f ¼ ½ðM1 þ M2 Þ=ðM1 þ M2 þ M3 þ M4 þ M5 Þ  100 ð%Þ
The fractions are the exchangeable fraction (M1) and the
carbonate bound fraction (M2), which together from mobile
group. In contrast, the Fe–Mn oxide (M3) fraction, organic
(M4) fraction, and residual (M5) represent the immobile group.
The mobility index calculation is seen in Table 3, and the
result revealed highest mobility for Cu and the lowest mobility
for Cd.
Cu was mostly bound to the exchangeable and carbon-
ate fraction and had an average mobility factor of about
25.89%. Cu was mobilized easily to the condition of the
environment on the reducing and acidic conditions
(Calmano et al. 1993). Several studies show that the solu-
bility of Cu is increased under oxidizing conditions as a
chalcophile mineral that is primarily bound to sulfides
(Weisz et al. 2000; Tüzen 2003). The results were con-
firmed by other studies (Guevara et al. 2004; Tokalioğlu
et al. 2000), which state that Cu is associated with the
organic fraction in stream sediments on a high proportion.
Accordingly, Cu was more available and toxic in the envi-
ronment in comparison with specific metals that were mostly
found in the two last fractions. The mobility factor on the
average of Pb was 23.9%, and it becomes very available and
toxic in the environment because of the deterioration of or-
ganic matter under strongly oxidizing conditions. Zn and Cd
had the lowest mobility factor (14.4 % and 9.24%), indicating
that they were relatively immobile.
Heavy metals of anthropogenic sources generally are most-
ly found on the first step of sequential extraction analysis. On
the other hand, the geogenic source is predominantly present-
ed in the residual fraction as the last step of the sequential
extraction analysis (Ramirez et al. 2005). As shown in Fig. 4
and Table 3, the order of mobility factors for the samples
agreed with the percentage of mobility. Pb, Cu, Zn, and Cd
were released to the wash sediments as a result of the milling
process. Based on the processing mining waste (tailing) data
in Table 1, they have been enriched in wastes by the anthro-
pogenic influences during the milling process. The heavy met-
al concentration in stream sediment in the study area was
found above background concentrations, which reflected for
the redistribution of contaminants by sediment transport from
where the source point has occurred.

Table 3 Mobility factor Conclusion

Sample code Mobility factor (%) This research evaluated the levels and mobility of Cu, Pb, Zn,
Cu Pb Zn Cd and Cd in the sediment of the Tajum River. This study con-
cludes that the average of metal concentration sediments in the
S-01 12.68 23.53 16.67 18.18 study area exceeded the mean crust because the metals were
S-02 36.56 32.14 14.29 37.14 released from the host rock and enhanced by milling process
S-03 25.93 38.30 4.67 16.00 of the extraction process of valuable metals. The changes in
S-04 31.05 25.64 11.67 8.00 the heavy metal concentrations in the Tajum River sediment
S-05 26.67 14.81 8.99 13.85 between the upstream and downstream areas indicate that
S-06 40.00 32.14 4.67 15.00 higher concentrations were located near the mining activities.
S-07 28.46 32.94 5.71 12.86 These results indicate that artisanal mining as anthropogenic
S-08 20.83 17.27 5.60 16.67 activity has triggered the release and transport of metals from
S-09 26.00 26.32 4.25 2.00 their source location in the upstream point in the research area.
S-10 32.97 17.33 10.00 10.00 These results allow to conclude that the extraction of precious
S-11 15.00 15.49 11.11 12.00 metals by artisanal mining activity and waste disposal prac-
S-12 14.58 10.77 13.25 6.67 tices polluted sediments to the downstream area from the
Average 25.89 23.89 14.03 9.24 source point. The mobility study revealed that Zn and Cd were
present to be more abundant in the Fe–Mn oxide, organic, and

residual fractions, demonstrating that the metals were more
strongly retained in the minerals and were, therefore, more
immobile. The mobile fractions including the exchangeable
and carbonate fractions were more established in Cu and Pb
compared with Zn and Cd, indicating that they have higher
mobility. The concentrations of Cu and Pb were relatively
high in the river sediment in the study area. This is an envi-
ronmental risk and requires future attention.
Acknowledgments The author thanks the Geoscience Center Georg-
August-Universität Göttingen, Germany, for the laboratory facility for
part of analyzing the samples under Erasmus project by European
Union on research fellowship program. The author also thanks to Hans
Ruppert, Wiebke Fahlbusch, Volker Karius, and Benedikt Sauer for valu-
able discussion. The author thanks Eska Rutana for picture editing in the
manuscript and Fraga L. Fahmi for help conducting sediment sampling in
the field. The author thanks Fahmi Hakim for the sharing of a geological
map. The author also thanks Hinode Laboratory, Tokyo Institute of
Technology Japan, for providing facility on the sample analysis. The
author thanks respected reviewers for their valuable comments in improv-
ing the manuscript.
Author contribution The author conducted all research work and wrote
the manuscript. The author read and approved the final manuscript.
Data availability Not applicable
Compliance with ethical standards
Competing interests The author declares that he has no competing
interests.
Ethics approval and consent to participate Not applicable
Consent for publication Not applicable
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