International Journal of Mineral Processing 119 (2013) 27–33

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International Journal of Mineral Processing

journal homepage: www.elsevier.com/locate/ijminpro

Preg-robbing of gold from cyanide and non-cyanide complexes: Effect of fungi

pretreatment of carbonaceous matter
G. Ofori-Sarpong a, b,⁎, K. Osseo-Asare b, c
a
Department of Mineral Engineering, University of Mines and Technology, P. O. Box 237, Tarkwa, Ghana
b
Department of Energy and Mineral Engineering, Penn State University, University Park, PA 16802, USA
c
Department of Materials Science and Engineering, Penn State University, University Park, PA 16802, USA

a r t i c l e i n f o a b s t r a c t

Article history: Cyanide has been the universal reagent for gold leaching on counts of higher stability, lower cost and better
Received 6 April 2012 understood chemistry. However, its high toxicity and slow leaching kinetics have called for research into alter-
Received in revised form 4 December 2012 native leaching reagents, of which thiosulfate and thiourea appear to be promising. Unlike the cyanide system,
Accepted 13 December 2012
interaction of thiourea and thiosulfate systems with carbonaceous matter (CM) has not received much research
Available online 9 January 2013
attention. As non-cyanide reagents become important alternatives for gold leaching, it is imperative to assess the
Keywords:
degree of gold adsorption (preg-robbing) in these systems and find ways of reducing this effect.
Cyanide This paper presents the results of a study on reduction in gold uptake by CM in cyanide and non-cyanide systems
Non-cyanide reagents due to fungal-treatment. Comparison is made between cyanide and non-cyanide systems on the bases of changes
Carbonaceous matter in gold adsorption by surrogate CM and CM in refractory gold ores. The results indicate that gold adsorption by
Preg-robbing as-received surrogates is in the order of cyanide > thiourea> thiosulfate, whereas after fungal-transformation,
Biotransformation reduction in gold adsorption is more pronounced in cyanide than in thiourea and thiosulfate solutions. The de-
crease in gold adsorption on the CM is about 70–97% in cyanide, 60–92% in thiourea and 50–91% in thiosulfate.
In general, the results exhibit a potential technique for reducing preg-robbing in the processing of carbonaceous
gold ores with cyanide, thiourea and thiosulfate solutions.
© 2013 Elsevier B.V. All rights reserved.

1. Introduction bromine and thiocyanate (Brown and Deschenes, 1993; Grosse et al.,
2003; Hiskey and Atluri, 1988; Sparrow and Woodcock, 1995). Of the
1.1. Preferred lixiviants in gold extraction non-cyanide reagents, those that have the potential to replace cyanide,
and have been researched most in the past 30 years include thiourea
Cyanide has remained the preferred complexing agent in the and thiosulfate (Aylmore and Muir, 2001; Fleming et al., 2003;
leaching of gold for over a century though many other complexing Groenewald, 1976; Hiskey, 1984; Schmitz et al., 2001; Yen et al., 1998).
agents exist. The major reasons for the acceptance of cyanide over the
other lixiviants include higher chemical stability, lower cost and better
understood chemistry (Groenewald, 1976; Habashi, 1987; Hiskey and 1.2. Adsorption of gold complexes on carbon
Atluri, 1988; Muir and Aylmore, 2004; Osseo-Asare et al., 1984; Ritchie
et al., 2001; Senanayake, 2004; Wan et al., 1993; Xue and Osseo-Asare, The dissimilarities in complexing reagents present significant
1985). In addition, adsorption and desorption of gold cyanide complex differences in their interactions with carbon. Gold thiourea is cationic
onto and from the most widely used adsorbent, activated carbon, have with a +1 charge while cyanide and thiosulfate are anionic but with
been studied the most with great success (Adams and Flemings, 1989; charges of −1 and −3 respectively (Marsden and House, 2006; Muir
Ibrado and Fuerstenau, 1995; Jones et al., 1989; McDougall et al., and Aylmore, 2004; Osseo-Asare, 1988). The ability of activated carbon
1980; Rees and van Deventer, 2000). to adsorb these three gold complexes is in the order of Au(CN)2− >
In spite of the good attributes, the high toxicity of cyanide, the need Au(CS(NH2)2)2+ >Au(S2O3)23− (Arriagada and Gardia, 1997; Brown
for faster leaching kinetics and an environmentally friendly recovery and Deschenes, 1993; Gallagher, 1989; Gonen et al., 2007; Kononova
process for gold ores, have necessitated research into alternative et al., 2001; Marsden and House, 2006; Munoz and Miller, 2000). The
leaching reagents. These complexes include thiourea, thiosulfate, iodine, mechanism of adsorption of these complexes has been discussed exten-
sively in the literature (Adams and Fleming, 1989; Arriagada and
⁎ Corresponding author. Tel.: +233 546100599.
Gardia, 1997; Brown and Deschenes, 1993; Jones et al., 1989; Kongolo
E-mail addresses: [email protected], [email protected] et al., 1990; McDougall et al., 1980; Muir and Aylmore, 2004; Navarro
(G. Ofori-Sarpong), [email protected] (K. Osseo-Asare). et al., 2006; Zhang et al., 2004).

0301-7516/$ – see front matter © 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.minpro.2012.12.007
28 G. Ofori-Sarpong, K. Osseo-Asare / International Journal of Mineral Processing 119 (2013) 27–33

1.3. The application of fungi in reducing adsorption of gold complexes on Table 1

carbon Partial chemical analysis of as-received gold concentrates.

Constituent Grade, %
Loss of gold due to preg-robbing is a major setback in the cyanide
FC BFC
system, and for many years, researchers have had great interest in
Gold 30.2 g/t 39.3 g/t
finding ways to mitigate the problem (Abotsi and Osseo-Asare,
Organic carbon 3.6 3.7
1987; Adams and Burger, 1998; Amankwah and Yen, 2006; Brierley Total carbon 6.1 3.8
and Kulpa, 1993; Rees and van Deventer, 2000; Schmitz et al., Sulfide sulfur 14.9 3.0
2001). Considering the potential of thiourea and thiosulfate to replace Sulfate sulfur 4.6 4.5
cyanide or be used as alternatives, it is essential to assess the status of Total sulfur 19.5 7.5

preg-robbing in these systems and to find possible ways of lessening it.

The application of the fungus, Phanerochaete chrysosporium, in the
biotransformation of carbonaceous matter (CM) in gold ores has been contacted with 25 mL of 5 mg/L and/or 10 mg/L gold solutions and
discussed by Ofori-Sarpong et al. (2010, 2011a,b). In the study, biotrans- agitated at 150 rpm for 24 h. At the end of the contact time the residual
formation led to a reduction in aurocyanide uptake by CM and hence solution was filtered, and gold in the filtrate determined using Perkin-
preg-robbing in cyanide solutions. The current study therefore focuses Elmer Optima 5300 inductively coupled plasma–atomic emission spec-
on assessing the ability of P. chrysosporium to alter the gold adsorption trometer (ICP-AES). The difference between the concentration of gold
ability of CM in thiourea and thiosulfate solutions. in solution before and after the adsorption test was computed with re-
spect to the amount of carbon-containing material used for the adsorp-
2. Experimental investigations tion studies (Ofori-Sarpong et al., 2010, 2011a).

2.1. Materials 2.4. Petrographic analysis of gold concentrate

Coal (anthracite, bituminous, sub-bituminous and lignite) samples Petrographic evaluation and thermal maturity analysis on the
with particle size less than 850 μm were provided by the Coal Bank of organic carbon in the gold concentrate was conducted using Zeiss
the EMS Energy Institute, whereas fungal spores of P. chrysosporium Universal research microscope. Gold concentrate originally ground
ME446 were provided by Prof. Ming Tien of the Department of Biochem- to 80% passing — 75 μm was vacuum-impregnated in epoxy resin
istry and Molecular Biology, all in the Pennsylvania State University. The and placed in a centrifuge to establish a density/particle-size gradient.
gold-containing samples utilized were flotation concentrate (FC) and After hardening, the samples were cut longitudinally to expose the
bacterial-oxidized flotation concentrate (BFC). Samples FC and BFC, particle gradation, remounted in epoxy and polished for optical mi-
which had been milled to all passing 75 μm, were obtained from the croscopy. All samples were examined in white light employing an
sulfide treatment plant at Bogoso Mine of Golden Star Prestea-Bogoso oil immersion objective lens at 625 × magnification.
Resources, Ghana. Standard gold cyanide solution (50 μg/mL in
0.1% sodium hydroxide and 0.05% sodium cyanide) was supplied 3. Results and discussion
by High Purity Standards. Powdered gold (I) sodium thiosulfate
(Na3Au(S2O3)2·xH2O hydrate, 99.96% metal basis), gold flakes (APS 3.1. Effect of carbonaceous characteristics on gold adsorption from cyanide,
1.5−3.0 μm, 99.96% metal basis), thiourea, sodium thiosulfate, sodium thiourea and thiosulfate solutions onto surrogate carbonaceous matter
hydroxide and sulfuric acid were supplied by Alfa Aesar. The growth
media for the fungus, millet and wheat bran (MWB) were obtained The gold adsorption behavior of anthracite, bituminous, sub-
from Nature's Pantry shop in State College, Pennsylvania. Medium prep- bituminous and lignite coals from cyanide, thiourea and thiosulfate solu-
aration, incubation and harvesting of treated materials are as presented tions before and after a one-week biotransformation by P. chrysosporium
in Ofori-Sarpong et al. (2010). are presented in Figs. 1, 2 and 3 respectively.
Several theories have been proposed for gold cyanide adsorption but
2.2. Partial elemental analysis of gold concentrates currently there seems to be a consensus that adsorption of aurocyanide
ion (Au(CN)2−) onto carbon occurs without chemical change, and that
Gold in the samples was determined by conventional fire assaying the graphitic structure of carbon is of great importance (Cashion et al.,
while carbon and sulfur were determined by the volumetric combus- 1988; Ibrado and Fuerstenau, 1995; Jones et al., 1989; Klauber, 1991;
tion technique using the LECO Sulfur titrator SC-4444DR. Before deter- Sibrell and Miller, 1992). The maturity of coal, and thus, the extent of
mining the sulfide sulfur, sulfate sulfur and elemental sulfur were graphitization decrease in the order of anthracite>bituminous>
removed as outlined by Ciminelli and Osseo-Asare (1995) and Rait sub-bituminous> lignite. Conversely, the percentage of oxygen and hy-
and Aruscavage (2006). The results are presented in Table 1. drogen decreases in the opposite direction (van Krevelen, 1993). It has
been shown that gold cyanide adsorbs preferentially on anthracite
2.3. Gold adsorption experiments relative to the other coals due to a better developed graphitic structure
in anthracite (Amankwah and Yen, 2006; Ibrado and Fuerstenau, 1992;
Gold-cyanide solution of concentration 50 mg/L Au was diluted Ofori-Sarpong et al., 2011a). Correlating the carbon-to-oxygen ratios
with 1 g/L NaOH at pH 12.8 to obtain 5 and 10 mg/L gold solutions with gold adsorption, Ofori-Sarpong et al. (2010) inferred that the ad-
which were used for the adsorption studies. Gold thiosulfate solution sorption of gold cyanide on anthracite is due to its high carbon-to-
was prepared by dissolving 130 μg of gold (I) sodium thiosulfate in oxygen ratio of 42 compared to 5–11 for bituminous, sub-bituminous
500 mL of 0.1 M thiosulfate solution at pH of 10–11 to obtain 50 mg/L and lignite.
Au. To obtain 50 mg/L Au in thiourea solution, 50 μg of gold flakes It can be seen from Figs. 2 and 3 that gold adsorption from thiourea
was dissolved in 500 mL of 0.001 M thiourea solution at pH of 1–2 at and thiosulfate solutions follow similar trends as that observed in the
40 °C. Both thiosulfate and thiourea gold stock solutions were diluted cyanide solution (Fig. 1), with anthracite adsorbing about 5–20 times
appropriately to obtain 5 and 10 mg/L solutions, which were used for as much as the other coals. Whereas anthracite adsorbed much more
adsorption. in the cyanide solution than the thiourea solution, the opposite was
Triplicate samples of biomodified, control and as-received coals of true for lignite, sub-bituminous and bituminous coals, which adsorbed
various weights (0.1 g–1 g) and gold ores of 2 g–5 g each were more gold from the thiourea solution than the cyanide solution. The
 G. Ofori-Sarpong, K. Osseo-Asare / International Journal of Mineral Processing 119 (2013) 27–33 29

Fig. 3. Effect of fungal-treatment on the gold adsorption ability of lignite, sub-bituminous,

Fig. 1. Effect of fungal-treatment on the gold adsorption ability of lignite, sub-bituminous,
bituminous and anthracite coals in thiosulfate (TS) solution. (Incubation conditions:
bituminous and anthracite coals in cyanide (CN−) solution. (Incubation conditions: 37 °C;
37 °C; pH 6.5; 60% solids; 1 week.)
pH 6.5; 60% solids; 1 week.)

positively-charged thiourea gold complex is reported to have better in- reported that the negatively charged carbon surface exerts a stronger
teraction with oxygen groups than does the aurocyanide complex, and electrostatic repulsion with the highly negative thiosulfate complex
this may explain the higher adsorption of gold thiourea by the lower compared to the other complexes (Aylmore and Muir, 2001; Grosse et
coal ranks which contain more oxygen groups (Arriagada and Gardia, al., 2003; Kononova et al., 2001; Muir and Aylmore, 2004).
1997; Nakbanpote et al., 2000; Ofori-Sarpong et al., 2010). Using acti- Fig. 4 compares the percentage reduction in gold adsorption due to
vated carbons of different precursors, Arriagada and Gardia (1997) fungal-treatment of the coals in all the gold solutions. After treatment of
noted that the carbons with oxygenated surface functional groups; the coals with P. chrysosporium, the adsorption capacity for the gold
carboxylic-like and phenolic or quinonic-like, had higher affinity for complexes generally decreased. For all the solutions tested, the average
gold thiourea complex than gold cyanide complex. reduction in gold adsorption was much more significant on anthracite
Comparing the gold complexes, it is clear that there was very low than the other coals. Average reduction in gold adsorption on all coals
adsorption from thiosulfate solution on all the coals, and this trend is in was highest in cyanide solution as depicted in Fig. 4.
agreement with what is reported in literature. Gold thiosulfate com- The comparison of gold adsorption on anthracite from cyanide,
plex, Au(S2O3)23− has been shown by many investigators to have signif- thiourea and thiosulfate solutions is presented in Fig. 5, whereas
icantly less affinity for carbon compared to gold cyanide and thiourea Fig. 6 presents data on control experiments to check the effect of
complexes (Fleming et al., 2002; Gallagher, 1989; Hemmati et al., the incubation medium on changes in the gold adsorption behavior
1989; Marsden and House, 2006; Navarro et al., 2006; Schmitz et al., of anthracite. Gold adsorption onto anthracite was highest in cyanide
2001; Wan and Brierley, 1997; Fleming, 1987). Gold thiosulfate com- solution at 4.5 μmol/g followed by thiourea at about 2.2 μmol/g as
plex has a high anionic charge resulting from the interaction between shown in Fig. 5. Fungal treatment reduced gold up-take from all the
gold cation and large thiosulfate anions. The low affinity of activated solutions to below 0.3 μmol/g. It is clear from Fig. 6 that the de-
carbon for Au(S2O3)23− complex is thus ascribed to the long pathway crease in gold adsorption was essentially due to biotransformation by
between the central gold atoms in the complex and the adsorbent P. chrysosporium as uptake by the controls was very close to that of the
surface, as created by the large thiosulfate ions. In addition, it is as-received samples.

Fig. 2. Effect of fungal-treatment on the gold adsorption ability of lignite, sub-bituminous, Fig. 4. Reduction in cyanide (CN), thiourea (TU) and thiosulfate (TS) gold adsorption
bituminous and anthracite coals in thiourea (TU) solution. (Incubation conditions: 37 °C; on lignite, sub-bituminous, bituminous and anthracite due to surface biotransforma-
pH 6.5; 60% solids; 1 week.) tion by P. chrysosporium. (Incubation conditions: 37 °C; pH 6.5; 60% solids; 1 week.)
30 G. Ofori-Sarpong, K. Osseo-Asare / International Journal of Mineral Processing 119 (2013) 27–33

0.7
As-Received FC

0.6 14-D Fungal-treated

Gold adsorbed, µmol/g carbon

0.5

0.4

0.3

0.2

0.1

0
AuCN AuTU AuTS
Gold Complexes

Fig. 5. Comparison of gold adsorption on anthracite from cyanide, thiourea and thiosulfate Fig. 7. Comparison of gold adsorption on flotation concentrate (FC) from cyanide, thiourea
solutions as a function of fungal-treatment time. (Incubation conditions: 37°C; pH 6.5; and thiosulfate solutions before and after fungal-treatment. (Incubation conditions: 37 °C;
60% solids; up to 3 weeks.) pH 6.5; 60% solids; 2 weeks.)

The mean maximum reflectance was 3.7% for FC and 3.6% for BFC, signi-
3.2. Effect of fungal biotransformation on the adsorption of gold complexes fying anthracite-grade maturity (Davis, 1978; van Krevelen, 1993).
onto gold concentrates Though the CM was characterized to have anthracite grade maturity,
it is clear from both Figs. 7 and 8 that the level of reduction in preg-
Having established the effect of fungal biotransformation of the robbing does not compare well with that of anthracite coal, which
surrogate carbonaceous materials on the adsorption of the gold was used as a surrogate material. This observation may be due to the
complexes, flotation concentrate (FC), and FC biooxidized with iron complex nature of the refractory gold ores with 3–4% organic carbon
and sulfur oxidizing bacteria (BFC) were also tested to ascertain the ex- and many other minerals constituting about 96–97%, in contrast to
tent to which their preg-robbing abilities change following fungal- anthracite which has more than 90% organic carbon. It is not clear
transformation. These results are presented in Figs. 7 and 8. at this point whether there was concurrent gold leaching during the
Within the boundaries established by the error bars, the levels of gold gold adsorption studies and/or if fungal-treatment activated some
adsorption for the as-received FC and BFC from each of the complexing other components in the ore to sorb gold. Nevertheless, preg-robbing
solutions were about the same. The above statement is also true for reduction of 50–70% in the refractory gold ore is promising.
adsorption after fungal treatment. This observation is based on the
fact that the organic carbon contents of the two samples, FC and
BFC were similar at 3.6% and 3.7% respectively (Table 1). 4. Adsorption of gold thiourea and thiosulfate on carbonaceous
Photomicrographs of the gold concentrates in Fig. 9 show carbon materials following fungal biotransformation
particles with sizes in the range of 5–40 μm. These were coarser than
those in refractory materials from the same geological area that were In contrast to the cyanide system, extensive research in gold adsorp-
analyzed by Afenya (1991) in which he obtained sizes of about 2 μm. tion by carbonaceous matter within the thiourea and thiosulfate sys-
Thermal maturity analysis revealed the presence of carbon-type tems is yet to be realized. This study is therefore important as it
grading from organic shale to graphite-like carbonaceous matter. reports for the first time, the extent of reduction in gold up-take in

Fig. 6. Gold adsorption on as-received, control and treated anthracite from cyanide, Fig. 8. Comparison of gold adsorption on bacterial-oxidized flotation concentrate (BFC)
thiourea and thiosulfate solutions. (Incubation conditions: 37 °C; pH 6.5; 60% solids; from cyanide, thiourea and thiosulfate solutions before and after fungal-treatment. (Incu-
1 week.) bation conditions: 37 °C; pH 6.5; 60% solids; 2 weeks).
 G. Ofori-Sarpong, K. Osseo-Asare / International Journal of Mineral Processing 119 (2013) 27–33 31

FC BCF

Organic Organic
Carbon Carbon

Pyrite

20 µm 20 µm

Fig. 9. Petrographic analysis of double refractory gold concentrate showing flotation concentrate (FC) and biooxidized FC (BFC).

these systems as a result of biotransformation of carbonaceous matter to cyanide, might be due to the ability of thiourea to interact with ox-
by the fungus, P. chrysosporium. ygen groups, which increased after fungal-treatment (Arriagada and
Figs. 1–3 demonstrate that, in like manner to the cyanide system, Gardia, 1997; Nakbanpote et al., 2000). This is evident from Infrared
the graphitic structure of carbon is important for gold adsorption from studies indicating an increase in the presence of oxygen groups after
thiourea and thiosulfate systems (Amankwah and Yen, 2006; Ibrado fungal-anthracite interaction (Fig. 11). Noda and Ozaki (2004) attrib-
and Fuerstenau, 1992; Jones et al., 1989; McDougall et al., 1980; Miller uted the peak at 1032 cm−1 to the presence of C\O and the figure
and Sibrell, 1991). As in the case of cyanide, the reduction in gold ad- shows an increase in the intensity of that peak after fungal treatment.
sorption from the thiourea and thiosulfate media subsequent to fungal A similar increase in C_O groups following incubation with P.
treatment can thus be explained on one hand by the destruction in chrysosporium was observed using XANES analysis (Ofori-Sarpong et
the graphitic structure. On the other hand, reduction in gold adsorption al., 2010).
is due to an increase in the pore sizes of the anthracite following mi-
crobial action as shown in Fig. 10. From an initial value of 57.5 Å for
the as-received sample, the pore diameters of all samples subjected 5. Conclusions
to microbial treatment increased in the range of 80 Å to 110 Å with
an average of 95.7 Å. This constitutes a percentage increase in pore size This paper reports, for the first time, on preg-robbing of gold
of about 67%. thiourea and gold thiosulfate complexes by different grades of car-
Though adsorption on as-received carbon is highest in cyanide solu- bonaceous matter (CM), and the extent of reduction in preg-robbing in
tion, it can be seen in Fig. 4 that the percentage reduction in adsorption these systems as a result of biotransformation of CM by the fungus,
after fungal treatment is also higher in cyanide than in thiosulfate and P. chrysosporium. The adsorption of gold on the as-received CM oc-
thiourea. This observation could be due to the larger ionic sizes of the curred in the order of cyanide > thiourea > thiosulfate. After fungal
thiosulfate and thiourea which make it possible for them to be adsorbed biotransformation, reduction in gold adsorption was more evident
into relatively bigger pores available after the fungal treatment as dem- in cyanide (70–97%) than in thiourea (60–92%) and thiosulfate
onstrated in Fig. 10 (Muir and Aylmore, 2004; Nakbanpote et al., 2000; (50–91%) solutions depending on the type of CM. Biotransformation
Ofori-Sarpong et al., 2011a; Syna and Valix, 2003). of CM resulted in a decrease in graphitization of carbon, and increase
Another possibility for the relatively smaller reduction in gold ad- in oxygen content and average pore diameter, all of which militated
sorption after fungal-treatment in the case of thiourea, as compared against uptake of gold by CM. Comparing the gold concentrates (FC and
BFC) to the surrogate anthracite coal, gold up-take on one hand and re-
120
duction in gold up-take on the other by anthracite were much more
substantial than FC and BFC. This observation may be due to the complex
nature of the refractory gold ores having 3–4% organic carbon as against
Average pore size diameter ( Å)

100 90% organic carbon in anthracite. The above notwithstanding, preg-

robbing reduction of 50–70% in refractory gold ores is promising. These
80 results thus exhibit a potential technique for reducing preg-robbing
in the processing of carbonaceous gold ores with cyanide, thiourea
and thiosulfate solutions
60

40 Acknowledgments

20 The authors are grateful to the Golden Star Prestea-Bogoso Re-

sources (GSPBR), Ghana, for providing the gold ores, and Prof. Ming
Tien of the Department of Biochemistry and Molecular Biology, in the
0
As-Received Treated 1 Treated 2 Treated 3 Treated Avg Pennsylvania State University for the fungal spores of P. chrysosporium
Anthracite coal Sample ME446. The authors also acknowledge Prof. Yaw Yeboah of the EME
Department, Penn State University, USA, for his support and for
Fig. 10. Changes in pore size due to microbial action on anthracite. proofreading the manuscript.
32 G. Ofori-Sarpong, K. Osseo-Asare / International Journal of Mineral Processing 119 (2013) 27–33

0.8
Sample incubated for 10 days
As-received sample
0.75

Absorbance 0.7

0.65

0.6
1250 1200 1150 1100 1050 1000 950 900 850
Wave number, cm-1

Fig. 11. Infrared spectrograph of treated and as-received anthracite showing an increase in the intensity of the C\O group at 1032 cm−1.

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