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C2 Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113 DOI 10.1179/037195504225004661
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
1 Eh–pH diagram at low reagent concentrations for: (a) Cu–NH 3–S2O32– system; and (b) Au–NH 3–S2O32– system
(conditions: 5 x 10–4 M Au; 0·1 M S2O 32–; 0·1 M NH3/NH4+, 5 x 10–4 M Cu2+)
proved to be too reactive with other ore minerals and kinetics and mechanism of leaching; and the leaching of
too expensive to operate. In the 1980s, attention various simple and complex gold ores. They have also
focused more on acidic Fe(III)/thiourea leaching and studied the in situ generation of thiosulphate from
significant R & D programmes were carried out at sulphide minerals and the adsorption/stripping of gold
CSIRO and at Murdoch University to investigate thiosulphate with various ion-exchange resins.
both the leaching and recovery of gold, and the This paper considers some of the issues that have
degradation of thiourea. By 1991, thiourea was listed been identified in various studies with thiosulphate
as a potential carcinogen and was considered too that have been reported in the literature, and some of
hazardous, so interest waned. Subsequent interest in the impediments that must be overcome before a
thiocyanate was brief because of its instability in viable and economic process is ready to replace
acidic Fe(III) solutions. cyanide. Only brief mention is made of some of the
More recently, world industry attention has tuned to sponsored work carried out by ourselves, and others
ammoniacal thiosulphate as a relatively cheap and non- in the Parker CRC, over the past 3 years which is yet
toxic reagent. Research and development over the past 20 to be publicly released.
years has focused on carbonaceous ores and copper–gold
ores where gold recovery is poor or cyanide consumption
THIOSULPHATE CHEMISTRY
is high. There were extensive investigations to semi-
commercial scale, using thiosulphate as an alternative Mechanism of gold leaching
lixiviant to cyanide. This was not driven by any particular The oxidation of metallic gold to the aurous Au+ ion
environmental or health and safety concerns about using in ammoniacal thiosulphate in the presence of Cu(II)
cyanide, but because cyanide was unable to extract gold can be simply represented as follows, although a more
effectively from certain ore resources. complex mechanism no doubt exists and needs further
However, increasing regulatory scrutiny of new investigation:
gold projects and a lowering of what is considered
Au + 5 S2O32– + Cu(NH3)42+ ®
acceptable levels of cyanide discharges are of
Au(S2O3)23– + 4 NH3 + Cu(S2O3)35– (1)
considerable concern to the industry. It is anticipated
that approval for any new gold project using cyanide Oxidation of gold in equilibrium with 10 M Au(I) –3
Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113 C3
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
Couple Standard
potential (V)
Cu(NH3)42+/Cu(S2O3)35– 0·22
Cu(NH3)42+/Cu(S2O3)23– 0·14
Cu(NH3)32+/Cu(S2O3)35– 0·36
Cu(NH3)32+/Cu(S2O3)23– 0·27
S2O32–/S4O62– 0·12
C4 Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113 C5
Table 3 Selection of ores and leaching conditions in literature (from Aylmore and Muir24)
Ore type Gold Temp. pO2 Retention S2O32– NH3 Cu2+ SO32– pH Recovery Consumption
(g/t) (°C) (kPa) (h) (M) (M) (M) (M) (%)
C6 Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113
15·2 g/t, 0·14% Cu, 0·91% S pH 9·5
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
Marchbank et al. (1996)38 Sulphide carbonaceous 3–7 55 Atm 4 0·02–0·1 2000 ppm 500 ppm 0·01–0·05 7–8·7 70–85
39
Yen et al. (1996) Gold–copper ore 7·26 Ambient Atm 24 0·4 0·2 0·03 … 11 90
1·4 g/t Ag, 0·3% Cu
Wan (1997)17 Sulphide carbonaceous 1–3 Ambient Atm …
40
Wan & Brierley (1997) Carbonaceous sulphide 1–3 Ambient Atm 91–116 days 0·1 0·1 0·005 … 9 50·7–65·7 5·2–8·4
41
Yen et al. (1998) Gold copper ores 7·2–7·9 Ambient Atm 24 0·5 6 0·1 … 10 95–97 30 kg/t
~0·36% Cu
Thomas et al. (1998)42 Pressure oxidised sulphide ore 2·5 45–55 Atm 12 0·03–0·05 ~500–1000 ppm 10-100 ppm 0·01–0·05 7·5–7·7 80–85
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
copper–gold ores. The earlier studies, using relatively of gold on iron from grinding media and the absorption
high concentrations of reagents, gave reasonable gold of gold onto some minerals. Decomposition of
extraction but consumed up to 40 kg t–1 thiosulphate. thiosulphate was also claimed to produce tetrathionate,
Later studies 35 established that comparable extraction polythionate and various unsaturated sulphur species
of gold could be achieved with dilute ammoniacal that could passivate the gold surface.
thiosulphate and identified the catalytic role played by Early work reported the precipitation of copper
trace amounts of copper. Subsequent work carried out sulphide with high concentrations of reagents, but
by Newmont36 showed that it was possible to heap recent work by Freitas et al.43 found that copper
leach low-grade carbonaceous ores using dilute precipitated from solutions containing < 0·3 M
ammoniacal thiosulphate solutions with reasonable thiosulphate. Abbruzzese et al.6 found that increasing
reagent consumption around 2–4 kg t–1 thiosulphate. temperature decreased gold recoveries by 20% which
In both cases, no more than 0·2 M thiosulphate and was ascribed to passivation by cupric sulphide. On the
ammonia were used for leaching with about 60 ppm other hand, Bagdasaryan et al.44 and Pedraza et al.45
Cu(II) as catalyst. It was recognised that it was observed a sulphur layer as well as copper sulphide in
necessary to limit the concentration of copper in a thiosulphate–copper sulphate system. However,
solution because Cu(II) degrades thiosulphate and electrochemical impedence spectral studies have
leads to high reagent losses. shown that gold passivation can occur in thiosulphate
Several research groups have studied gold–copper ores solution even in the absence of copper.46
but generally find it difficult to control the extent of In some leach tests over an extended time there has
copper leaching and the degradation of thiosulphate (D. been evidence of re-precipitation of gold, silver and
B. Dreisinger, 2000, personal communication). Although copper and lower gold recovery. No doubt this reflects
70–90% of the gold could be leached from three Brazilian the build up of degradation products in solution and
ores, each ore responded differently, and each required possible precipitation of gold and silver sulphide.
different leach conditions for optimum recovery. In some Briones and Lapidus47 found precipitation of Ag2S
cases, copper partially precipitated from solution and gold occurred at low thiosulphate concentrations. However
extraction reached a maximum after about 8 h.43 Kerley26 and Perez and Galavis48 ascribe the precipitation
Lakefield Research also examined pressure-leached of Ag2S to the reaction of the silver thiosulphate complex
arsenopyrite ores from Barrick, and carried out a with metal oxide minerals. Once Ag2S is formed, it
large number of stirred tank tests at pH 8–9. Up to appears that the dilute thiosulphate solutions are unable
95% Au was extracted from the finely divided gold left to re-leach the sulphide. Recent studies on the leaching of
in the oxidised residue, but the gold recoveries pure silver sulphide 47 generally show < 50% Ag
generally varied from 50% to 95%.42 extraction with a range of ammoniacal thiosulphate
Recent studies have been made by ourselves on compositions containing up to 0·1 M Cu(II).
some relatively simple Australian oxide ores, using a Studies by Miura and Koh49 indicate that
range of dilute reagent compositions and conditions. tetrathionate decomposes to thiosulphate and sulphite
These have shown that whilst most of the gold and ion together with sulphoxylic acid (S(OH)2) and some
silver were readily leached in 2–4 h, a fraction of the sulphide ion (Eq. 5). Rabai and Epstein50 report that the
cyanide-soluble gold always remained in the fast redox reaction between Cu(II) and thiosulphate is
thiosulphate leach residue (Table 4). Although followed by slower side reactions which produce Cu2S
changes in reagent composition and leach conditions (Eq. 6). Abbruzzese et al.6 claim that CuS is formed by
affected the kinetics and percentage of gold recovery, the reaction between Cu(II) and thiosulphate (Eq. 7) –
no conditions were found that could match gold similar to the ‘copper boil’ reaction used in the Sherritt-
recovery by cyanide. Furthermore, the recovery of Gordon process for refining nickel matte.
gold from different ores varied even more when
similar leach conditions were used (Table 4), 10 [S4O6]2– + 20 OH–
indicating other factors are more important. ® 10 [S2O3]2– + 10 S(OH)2 + 10 [SO3]2– (5a)
Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113 C7
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
C8 Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
Table 5 Summary of issues and impediments associated with thiosulphate leaching of gold ores and recovery from solution
Kinetics and Cu(II) catalyses both gold and thiosulphate oxidation High reagent consumption
mechanism Complex leach kinetics Copper in ore difficult to control; not understood
Chemically controlled Ag2S partially leached Dependent on Cu(II), T, NH3, S2O3
Possible passivation of gold; Au associated
with Ag not leached
Time Rate of oxidation S2O3 remains constant Large build up of polythionates for small increase
whilst gold extraction slows in gold
Gold deportment Coarse gold and gold in sulphide minerals slow to leach Long leach time builds up polythionates
Ore mineralogy Possible preg-robbing of copper and gold by clays, sulphides Recovery sensitive to ore type
Reactive sulphides consume oxygen and Cu(II) Leaching impaired or stopped
Recovery on resins Polythionates co-absorb on SB resin Low resin loading increases cost
Copper absorbs on resin Copper competes for gold
ossible precipitation of sulphides in resin
important to leach gold with the minimum of the recovery of gold from solution, the stability of the
thiosulphate. reagents and their release to the air or water. Clearly,
not all issues can be solved, but all criteria must be
Ammonia addressed and understood before an overall process
Ammonia poses environmental and toxic problems can be developed, tested and costed.
both as a gas in air and as a soluble solution. In air, the There is no doubt that, despite its shortcomings,
threshold limiting value (TLV) for ammonia gas is 14 thiosulphate is an attractive alternative to cyanide for
mg m–3, which is classified similar to HCN. In water, free processing carbonaceous ores where the recovery of
ammonia is classified similar to chlorine whilst ammon- gold is poor. It may also be attractive for processing
ium ion has low toxicity. Unfortunately, ammonia is copper–gold concentrates and ores that consume
difficult to break down and may eventually metabolise significant cyanide. However, for simple oxide ores,
to nitrate, which has the potential to promote algal further research is required to improve gold recovery
growth and to pollute ground-water. Thus, even more and lower reagent costs to match that of cyanide.
strict precautions have to be taken to control ammonia Further research is now being carried out under
emissions from tanks or heaps, and to prevent its release AMIRA sponsorship in the Parker CRC at Murdoch
into the environment. University and CSIRO Minerals to examine a range
of issues. This work aims to:
(i) Understand the speciation and conditions
SUMMARY AND FUTURE RESEARCH controlling the oxidation of gold and thio-
Table 5 summarises the issues and impediments sulphate to minimise reagent concentration and
discussed above with regard to the leaching gold ores, decomposition.
Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113 C9
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
(ii) Examine alternative redox systems to ammon- Singapore, Society for Mining, Metallurgy and
iacal copper to leach gold without oxidation of Exploration, Inc. Littleton, 1997, 159–162.
thiosulphate. 8. M. G. AYLMORE and D. M. MUIR: ‘Thermodynamic analysis
(iii) Understand why gold extraction varies with of gold leaching by ammoniacal thiosulfate using Eh/pH
and speciation diagrams’, J. Min. Metal. Process., 2001,
different ores.
18, 221–227.
(iv) Understand the effect of silver on extraction and
9. M. I. JEFFREY, P. BREUER and W. L. CHOO: ‘How rapidly do
recovery. alternative lixiviants leach gold?’ (eds. C. A. Young, L. G.
(v) Examine whether particular minerals ‘preg-rob’ Twidwell and C. A. Anderson) Cyanide: social, industrial
gold or copper, effect Eh/pH, or cause gold and and economic aspects, Warrendale, TMS, 2001, 441–454.
copper to precipitate from solution. 10. M. I. JEFFREY, P. BREUER and W. L. CHOO: ‘A kinetic study
(vi) Understand the effect of saline process water on comparing gold leaching in the cyanide, thiosulfate and
leaching and recovery. chloride systems’, Metal. Mater. Trans. B, 2001, 32,
(vii) Examine means of removing or decomposing 979–986.
polythionates without affecting thiosulphate. 11. P. L. BREUER, M. I. JEFFREY and W. L. CHOO: ‘Fundamental
(viii) Optimise the loading of gold and silver onto resins, aspects of the gold thiosulfate leaching process’, (eds. C. A.
Young, L. G. Twidwell and C. A. Anderson) Cyanide:
or modify the resin to minimise polythionate
social, industrial and economic aspects, Warrendale, TMS,
absorption.
2001, 455–468.
(ix) Examine the selective elution of copper and gold 12. P. L. BREUER and M. I. JEFFREY: ‘Electrochemical study of
from resin. gold leaching in thiosulphate solutions containing
(x) Examine alternative methods of recovery of gold ammonia and copper’, Hydrometallurgy, 2002, 65,
from eluates. 145–157.
Until some of these issues are overcome, there is little 13. M. I. JEFFREY: ‘Kinetic aspects of gold and silver leaching in
current economic incentive to switch existing plants from ammonia-thiosulfate solutions’, Hydrometallurgy, 2001,
cyanide to thiosulphate – except for the processing of 60, 7–16.
carbonaceous ores. However, the threat of increasing 14. M. G. AYLMORE and C. RAE: ‘Factors affecting the rate of
public concerns over cyanide management will ensure leaching of gold in ammoniacal thiosulfate and the
stability of the leach solution’, CSIRO Report DMR-
that companies will continue to strive for a viable
1493, 2001, 1–36.
alternative. The industry’s first endeavour with the
15. S. W. DHAWALE: ‘Thiosulfate’, J. Chem. Ed., 1993, 70,
thiosulphate system is to develop a robust overall process 12–14.
flowsheet that can be realistically used and costed for a 16. H. KAMETANI and A. AOKI: ‘Potential-pH diagrams of the
range of actual ores – including gold recovery, reagent re- SO2–H2O and S2O3–H2O systems at 90 degrees’, Trans.
cycling or destruction and impurity control. Natl. Inst. Metals, 1976, 18, 20–30.
17. R. Y. WAN: ‘Importance of solution chemistry for
thiosulfate leaching of gold’, Proceedings of the ‘World
ACKNOWLEDGEMENTS Gold ‘97’, Singapore, Society for Mining, Metallurgy and
This study was first presented at the Green Processing Exploration, Inc., Littleton, 1997, 159–162.
2002 Conference, 29–31 May 2002, organised by the 18. J. J. BYERLEY, S. FOUDA and G. L. REMPEL: ‘Kinetics and
mechanism of the oxidation of thiosulfate ions by copper
AusIMM. The authors wish to thank Normandy
(II) ions in aqueous ammonia solution’, J. Chem. Soc.
Mining, AngloGold and WMC Resources for their
Dalton Trans., 1973, 889–893.
interest and support of research in this area and for 19. J. J. BYERLEY, S. FOUDA and G. L. REMPEL: ‘The oxidation of
permission to publish this paper. thiosulfate in aqueous ammonia by copper (II) oxygen
complexes’, Inorg. Nuclear Chem. Lett., 1973, 9, 879–883.
20. J. J. BYERLEY, S. FOUDA and G. L. REMPEL: ‘Activation of
copper(II) amine complexes by molecular oxygen for the
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Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113 C11
Muir and Aylmore Thiosulphate as an alternative to cyanide for gold processing – issues and impediments
C12 Mineral Processing and Extractive Metallurgy (Trans. Inst. Min. Metall. C) March 2004 Vol. 113