J. Cent. South Univ. (2020) 27: 1367-1372
DOI: https://doi.org/10.1007/s11771-020-4372-4
Sulfide mineral bioleaching: Understanding of microbe-chemistry assisted hydrometallurgy technology and acid mine drainage environment protection
LIAO Rui(廖蕤)1, 2, YU Shi-chao(于世超)1, 2, WU Bai-qiang(邬柏强)1, 2, ZHAO Chun-xiao(赵春晓)1, 2,
LIN Hao(林豪)1, 2, HONG Mao-xin(洪茂鑫)1, 2, WU Hai-yan(武海艳)1, YANG Cong-ren(杨聪仁)1,
ZHANG Yan-sheng(张雁生)1, 2, XIE Jian-ping(谢建平)1, QIN Wen-qing(覃文庆)1, 2,WANG Jun(王军)1, 2, QIU Guan-zhou(邱冠周)1, 2
1. School of Minerals Processing and Bioengineering, Central South University, Changsha 410083, China;
2. Key Laboratory of Biohydrometallurgy of Ministry of Education, Central South University,Changsha 410083, China
Central South University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020
Abstract: Bioleaching is regarded as an essential technology to treat low grade minerals, with the distinctive superiorities of lower-cost and environment-friendly compared with traditional pyrometallurgy method. However, the bioleaching efficiency is unsatisfactory owing to the passivation film formed on the minerals surface. It is of particular interest to know the dissolution and passivation mechanism of sulfide minerals in the presence of microorganism. Although bioleaching can be useful in extracting metals, it is a double-edged sword. Metallurgical activities have caused serious environmental problems such as acid mine drainage (AMD). The understanding of some common sulfide minerals bioleaching processes and protection of AMD environment is reviewed in this article.
Key words: bioleaching; sulfide minerals; microorganism; acid mine drainage
Cite this article as: LIAO Rui, YU Shi-chao, WU Bai-qiang, ZHAO Chun-xiao, LIN Hao, HONG Mao-xin, WU Hai-yan, YANG Cong-ren, ZHANG Yan-sheng, XIE Jian-ping, QIN Wen-qing, WANG Jun, QIU Guan-zhou. Sulfide mineral bioleaching: Understanding of microbe-chemistry assisted hydrometallurgy technology and acid mine drainage environment protection [J]. Journal of Central South University, 2020, 27(5): 1367-1372. DOI: https://doi.org/10.1007/ s11771-020-4372-4.
1 Introduction
Bioleaching, an optional technology for treating low-grade minerals, is of particular interest since it can decrease the production cost and reduce the pollution [1]. Nevertheless, the application of bioleaching is restricted for poor extractions and slow kinetics. There are some products formed on mineral surface during bioleaching such as polysulfide (Sn2-) and elemental sulfur (S0) [2]. These products, also known as passivation film, are thick and insoluble, therefore, making it hard for electrons to exchange between leaching medium and unreacted mineral. It is of importance to understand the dissolution process and mechanism of sulfide minerals, and to study the passivation components that hinder the bioleaching.
2 Leaching bacteria
In order to enhance the bioleaching process, the selection of high activity microorganism strains are essential. Some extreme acidophilic microorganisms which live in acidic natural environment and acidic mine drainage can provide nutrition and energy for their own growth and metabolism by oxidizing Fe2 +, S2-, S plasma or inorganic compounds. They are autotrophic bacteria and considered to be the main strains of biohydrometallurgy. Strains that have been reported to participate in bioleaching include Acidithiobacillus ferrooxidans, Acidithiobacillus thiooxidans, Leptospirillum ferrooxidans, etc [3].
Community diversity and metabolic mechanism of leaching bacteria have always attracted researchers’ attention. LUO et al [3] and LIU et al [4] used genechip technology to investigate the genetic diversity of typical leaching microorganisms Acidithiobacillus ferrooxidans, and used metagenomics to study the iron and sulfur metabolism mechanism of leaching bacteria [5]. During the bioleaching process, microbial community structure and function shift [6]. It was generally believed that an interactive mechanism between minerals and microorganisms exists. XIAO et al [7, 8] used gene array and 16S rRNA sequencing to investigate the diversity of leaching microbial functional communities and phylogenetic diversity in the leaching heap and solution. The shift of microbial community metabolic functions during copper leaching was also studied [9]. Furthermore, the geochemical element cycle of the leaching microbial community during copper leaching was studied by X-ray diffraction and metatranscriptomics was also used to assess the gene expression in the process of copper leaching [10, 11].
The extreme acidophilic microorganism is considered to be an important participant in the cycle of global biogeochemistry. Investigations on its community diversity and the metabolic mechanism during the copper leaching are important for revealing the microbial driving mechanism of global biogeochemistry. But most of previous research concerned on the leaching bacteria cultured in the laboratory (isolated from the mine and expanded), rather than those directly isolated from the extreme environment, making it unable to reveal the environmental impact mechanism of microbial community diversity and metabolic function of leaching bacteria. Meanwhile, the mechanism of mineral-microbe interaction still has not been revealed.
3 Sulfide mineral bioleaching
By understanding the bioleaching nature and passivation mechanism, theoretical foundation for enhancing bioleaching can be provided. On this basis, the bioleaching processes of some common sulfide minerals are introduced below.
3.1 Chalcopyrite bioleaching
Chalcopyrite, with a stoichiometric equation of CuFeS2, is the most plentiful copper-bearing ore. However, the bioleaching efficiency is not ideal for the passivation film coated on the mineral surface. Silver was found to be an effective catalysis that can improve the bioleaching efficiency with a small amount of addition. However, silver is such expensive on the economic level that it is inappropriate for its usage in industry. ZHAO et al [12] found that not only silver ion but also silver-bearing tailing can catalyze the chalcopyrite bioleaching process, and silver extraction can be enhanced with the chalcopyrite added. Polysulfide was detected as the main sulfur intermediate species formed on the surface of chalcopyrite; however, the bioleaching was not hindered. It was reported that the oxidation-reduction potential (ORP) should be kept at an optimal range of about 380-480 mV (vs. Ag/AgCl) for improving the leaching efficiency. In their study, a higher copper extraction can be achieved even when the ORP was beyond the proposed region. Later, they investigated the selecting bioleaching of mixed ores of chalcopyrite and marmatite using silver-containing waste [13]. Marmatite was antecedently dissolved, and the electrochemical interactions between these two minerals have improved marmatite dissolution. Silver was believed to have changed the dissolution mechanism of chalcopyrite for the reason that ORP was no longer the determining factor influencing bioleaching process. The recovery of silver was likewise studied [14]. It was much easier to extract silver from the abandoned silver-bearing wastes after the bioleaching process. There was a synergic effect between chalcopyrite and silver-bearing solid waste.
3.2 Chalcocite bioleaching
Chalcocite is a common secondary copper mineral. The dissolution process of chalcocite heap leaching is divided into two leaching stages according to the difference in dissolution kinetics behavior. The chalcocite dissolution rate is fast in the first stage, and slow in the second stage (copper leaching rate greater than 45%) [15]. Copper leaching rate in the second stage is sensitive to temperature, and not sensitive to redox potential and Fe3+ concentration when Eh (ORP) exceeds 650 mV and Fe3+concentration is more than 1 g/L [16]. The mixed kinetics fitting results of chalcocite in the second dissolution stage show that the dissolution rate is affected mainly by two factors, diffusion control and chemical reaction control, and the chemical reaction limiting effect on dissolution is more obvious [17]. The mineralogical analysis results of the leaching residues in the second leaching stage show that the outer sulfur layer wrapped CuS shrinkage core, and the higher the heap leaching temperature is, the looser the structure of the sulfur layer appears on the surface. A dissolution model was proposed by NIU et al [16] as below. When the copper extraction rate was between 45% and 70%, the dissolution rate was mainly controlled by the chemical reaction on the surface of the sulfide minerals. When the copper extraction rate was higher than 70%, the diffusion layer constituted of element sulphur slowed the ions diffusion process, which in turn affected the dissolution rate. The density of the surface sulfur layer was affected by the reaction temperature, and copper ions with a mass ratio of about 10%-20% remain among the surface sulfur layers. The proposed dissolution model provides scientific basis for guiding the application of chalcocite and solving the problem of low reaction leaching efficiency. LEE et al [18] investigated the dissolution process and mineralogy of the composited ores from the Minera Yanacocha mine, Peru, using two ores samples with chalcocite and covellite separately as the main component, the conclusions are basically consistent with the kinetic theory research discussed above. The difference in bioleaching rate of ores sample with chalcocite as the main component at different temperatures was very small, but the bioleaching rate of ores sample with covellite was sensitive to temperature, and there was a long lag period under thermophilic bioleaching conditions in the initial period.
Since covellite dissolution is limited by kinetics factors as discussed in above, whether secondary covellite is responsible for the chalcopyrite passivation deserves to be explored. SASAKI et al [19] combined Raman spectroscopy, XRD and FTIR techniques to explore the formation of secondary minerals on the surface of chalcopyrite during bioleaching, and explored the corresponding passivation effect on the leaching process. During the early stage of leaching, the presence of covellite and elemental sulfur was detected on the surface, and remained until the middle and late stages; while a large amount of jarosite minerals formed on the surface, and converted from potassium-jarosite to ammonio- jarosite. According to the analysis, the tight jarosite minerals gradually formed on the surface during dissolution process, hindering the contact between sulfur-oxidizing bacteria and iron-oxidizing bacteria with covellite and sulfur, which led to passivation and also the presence of covellite and elemental sulfur on the surface in the late leaching stage. Covellite and elemental sulfur detected on the surface may not be the passivation components of chalcopyrite bioleaching.
The CdS/Cu2S solar cell with low cost and simple manufacturing process has been continuously concerned by researchers since it was proposed in 1950 [20]. Cu2-xS, as an important component of copper sulfide, has been widely investigated in the battery field due to its good semiconductor characteristics. In the field of materials research, the electrical and thermodynamic properties of copper sulfide nanocrystals (quantum dots) with different compositions such as Cu2S, Cu1.97S and CuS have been studied [21]. Also, in the bio- hydrometallurgical research of copper sulfide minerals, the semiconductor properties of copper sulfide ores and the common associated mineral pyrite also play an important role in the selective leaching of ores and the optimization of leaching conditions. After density functional theory (DFT) theoretical calculations, by controlling the potential stepwise, leaching of chalcocite and pyrite can be achieved, and the effectively separation of copper and iron ions can be attained in the leaching solution [22].
3.3 Bornite bioleaching
Except chalcopyrite and chalcocite, bornite is also an important resource of copper. Oxidative dissolution of bornite in the presence of Acidithiobacillus ferrooxidans has been investigated by BEVILAQUA et al [23] who suggested that bacterial leaching of bornite is a relatively fast reaction but also an acid-consuming reaction. Additionally, bioleaching of bornite by A. ferrooxidans involved ferric iron-dependent reaction, and regeneration of ferric iron and production of sulfuric acid from elemental sulfur are shown in Eqs. (1)-(3). Covellite was detected as a main secondary phase during the process.
Cu5FeS4+12Fe3+→5Cu2++13Fe2++4S0 (1)
4Fe2++O2+4H+→4Fe3++2H2O (2)
2S0+3O2+2H2O→2SO42-+4H+ (3)
In nature, bornite commonly exists with other sulfide minerals, such as chalcopyrite, sphalerite and pyrite. ZHAO et al [24] discovered the synergistic effect between chalcopyrite and bornite during bioleaching in the presence of A. ferrooxidans, and galvanic effect between chalcopyrite and bornite was responsible for this phenomenon. In the later stage of bioleaching, huge amount of elemental sulfur and jarosite could be the main passivation film inhibiting further dissolution. Similarly, synergetic effect was believed to exist between pyrite and bornite bioleaching by Leptospirillum ferriphilum [25]. The addition of pyrite increased solution ORP and accelerated the dissolution of bornite while the dissolution mechanism of bornite remained unchanged.
3.4 Arsenopyrite bioleaching
Gold, an essential non-renewable precious resource, plays an important role in human society. It usually encapsulates in sulfide minerals due to its tiny particles in nature. Arsenopyrite, one of the most important gold-bearing minerals, the pre-treatment of which is necessary to release the contained gold liberated for subsequent process. However, traditional cyanide leaching has forced environment to be subjected a series of pollution questions. The acidophilic microorganisms, such as Leptospirillum ferriphilum, are able to withstand high concentration of As(III) and As(V) [26]. In addition, arsenopyrite often intergrows with other sulfides in nature. Among them, pyrite is also a gold-bearing mineral [27]. The resting potential of arsenopyrite is lower than that of pyrite. Under acidic conditions, galvanic interactions occur when they are in contact, with arsenopyrite dissolved as the anode and pyrite was protected as the cathode [28]. The formation of scorodite caused the passivation on the arsenopyrite surface at relatively low pH and high redox potential [29], which was hindered with the addition of pyrite, due to galvanic interaction and the control of pH and redox potential [30]. Hence, it is no surprise that the development of synergetic effect of pyrite on strengthening arsenopyrite bioleaching has been targeted as the breakthrough point of gold beneficiation processing.
4 Environment problems caused by metallurgical activities
Although bioleaching can be useful in metal extraction, it is a double-edged sword. Metallurgical activities have caused serious environmental problems, such as acid mine drainage (AMD), acid rock drainage (ARD) formed by biological and non-biological oxidation of sulfide deposits [31], which pollutes groundwater and surface water, destroys the ecosystem and reduces water consumption for human activities [32]. Mine waste is a source of trace element soil contamination of the environment that may affect local vegetation [33]. Although the chemical composition of AMD varies from place to place, it usually has the characteristics of low pH value, high concentration of sulfate and heavy metal [34].
Chalcopyrite is an important cause of AMD due to its wide distribution and large mining demand. Chalcopyrite mining produces a large number of mineral wastes, most of which are stored on the surface of the mining area. These wastes can be dissolved by bacteria or chemical oxidation to produce a large amount of AMD [35]. Microbial activity can increase the oxidation rate of chalcopyrite by up to three orders of magnitude relative to pure weathering. One mine can lead to the formation of hundreds to thousands cubic meters of AMD [32].
5 Conclusions
The understanding of bioleaching process is both important for metal extraction and environment protection. However, to date, there is no consensus recognition about the leaching mechanism and intermediate products. Further research on bioleaching is essential and still required to promote the commercial application.
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(Edited by YANG Hua)
中文导读
硫化矿物生物冶金:微生物-化学协同湿法冶金过程及酸性矿山废水的环境保护情况
摘要:生物冶金是用于处理低品位矿物的一项必要的技术,与传统的火法冶金方法相比,它具有成本低和环境友好的优势。然而,生物浸出过程中矿物表面有钝化膜生成,使得其浸出效率较低。因此,对微生物存在下硫化矿物的溶解和钝化机理的研究有着重要意义。生物冶金有利于金属的提取,但它也是一把双刃剑,会引起一系列严重的环境问题,例如产生酸性矿山废水等。本文概述了一些常见硫化矿物生物浸出过程的研究以及对酸性矿山废水的环境保护情况。
关键词:生物冶金;硫化矿物;微生物;酸性矿山废水
Received date: 2020-05-04; Accepted date: 2020-05-15
Corresponding author: WANG Jun, PhD, Professor; Tel: +86-731-88876557; E-mail: wjwq2000@126.com; ORCID: 0000-0003-0931- 3946