不同成因黄铜矿极端嗜热菌浸出差异性及机理研究
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摘要
本论文以斑岩型、海相火山岩型、矽卡岩型黄铜矿为研究对象,系统研究了三种成因黄铜矿极端嗜热菌浸出特性,在对极端嗜热菌进行种群鉴定和驯化的基础上,对不同pH值、不同矿浆浓度进行条件实验,研究三种成因黄铜矿的浸出差异,并从矿物性质、吸附机理和溶解途径三个方面对浸出差异性进行了分析,从而为系统开展黄铜矿极端嗜热菌浸出机制的研究奠定了基础。
研究了不同pH值、矿浆浓度下三种成因黄铜矿极端嗜热菌浸出特性,比较三种成因黄铜矿的浸出差异。不同pH值条件下,海相火山岩型黄铜矿浸出率均明显高于矽卡岩型黄铜矿和斑岩型黄铜矿,显示了海相火山岩型黄铜矿较易浸出。斑岩型黄铜矿菌体浓度和浸出率随着pH值升高先增高后降低,并在pH值为1.5时达到最高；而海相海相火山岩型和矽卡岩黄铜矿则是随着pH值升高不断增高。不同矿浆浓度条件下,三种成因黄铜矿浸出行为具有较大的差异。其中斑岩型和矽卡岩黄铜矿菌体浓度和浸出率随着矿浆浓度的升高均为先升高后降低,并在矿浆浓度为2.0%时达到最高,而海相火山岩型黄铜矿在矿浆浓度为0.5%时,菌体浓度和浸出率最高,随着矿浆浓度的升高而降低。通过条件实验分析发现,三种成因黄铜矿的浸出率与其菌体浓度完全成正相关性,为寻找适宜的浸出工艺参数提供依据。
通过晶体结构、电子结合能、穆斯堡尔谱Fe的价态和矿物组成(硫化矿物组分)等四个方面对三种成因黄铜矿的矿物性质进行了深入分析,从原矿本质上揭示了三种黄铜矿浸出差异的本源原因。海相火山岩型黄铜矿具有较小的晶格能和电子结合能、较高的Fe2+/Fe3+的含量,同时表面含有一部分有助于浸出进行的Cu(II),使得该类黄铜矿具有较好的浸出特性。此外,还研究了黄铜矿中所含硫化矿物组分对浸出的影响,研究发现黄铁矿、闪锌矿和铜蓝这三种硫化矿物对斑岩型和矽卡岩型黄铜矿的极端嗜热菌浸出具有阻碍作用,而对海相火山岩型黄铜矿的极端嗜热菌浸出具有一定的促进作用。
通过选择性吸附、电动性质和吸附作用力性质等方面对三种成因黄铜矿极端嗜热菌的吸附机理进行了深入分析,从吸附机理上揭示了浸出差异的过程原因。不同影响因素下极端嗜热菌在斑岩型、海相火山岩型、矽卡岩型黄铜矿表面的吸附规律表明,矿物单位面积微生物吸附量的大小顺序为：矽卡岩型>斑岩型>海相火山岩型。通过分析三种成因黄铜矿与极端嗜热菌作用后的Zeta电位,揭示了三种成因黄铜矿的等电点(IEP)与极端嗜热菌在其表面的吸附率高低相一致。利用EDLVO理论对微生物吸附行为的分析,进一步揭示了极端嗜热菌在三种成因黄铜矿表面的吸附受静电(EL)作用的控制。
通过浸出过程中氧化还原反应分析与浸出产物分析,揭示三种成因黄铜矿在极端嗜热菌浸出时的溶解途径,从而通过溶解途径的研究揭示浸出差异的本质原因。极端嗜热菌浸出时,质子(H+)与极端嗜热菌的共同作用,使得黄铜矿价带空穴和导带电子的转移同时发生。极端嗜热菌对黄铜矿浸出的作用,取决于其在矿物表面的吸附。斑岩型、海相火山岩型及矽卡岩型黄铜矿生成的产物分别为缺M-硫化物(CuFeS)与铜蓝、富M-硫化物(Cu2Fe2S)及缺M-硫化物(Cu4Fe4S5)与富M-硫化物(Cu3.5Fe4S2.5)。三种成因黄铜矿生成单质硫(S0)及黄钾铁矾。单质硫(S0)层阻碍了斑岩型及矽卡岩型黄铜矿进一步溶解,所以提高极端嗜热菌的菌体浓度,有利于这两种成因黄铜矿的溶解。而海相火山岩型黄铜矿的表面覆盖有黄钾铁矾层,因此降低浸出溶液的pH值,有利于海相火山岩型黄铜矿的溶解。此外,进一步描述了三种成因黄铜矿的溶解反应方程式,从而揭示了三种成因黄铜矿在极端嗜热菌浸出时的溶解机理。
The thermophiles bioleaching behaviours and mechanisms of chalcopyrite with distinct genetic types were studied in the present thesis. The chalcopyrite samples are from porphyry type, marine volcanic type, skarn type copper deposit. On the basis of identification and domestication, different thermophiles bioleaching conditions of experiments were carried out, such as different pH values and pulp concentration. To investigate the different bioleaching behaviours, the nature of minerals, the biosorption mechanism, and the dissolution were analyzed. This study provided the theoretical basis of the thermophiles bioleaching mechanisms of chalcopyrite.
The effects of pH values and pulp density on the thermophiles bioleaching behaviours of chalcopyrite with distinct genetic types were studied. Under different pH values leaching conditions, the copper leaching yield of marine volcanic chalcopyrite was significantly higher than the porphyry type and skarn type. This result indicated that the marine volcanic type is easier to dissolve than the other two type chalcopyrite. As pH value increasing, the cell concentration and the copper leaching yield of porphyry chalcopyrite increased first and then decreased, and reached a maximum at pH1.5. However, the cell concentration and the copper leaching yield of marine volcanic type and skarn type increased with pH value increasing. Under different pulp density, there were greater differences between behaviours. As pulp density increasing, the cell concentration and the copper leaching yield of porphyry type and skarn type increased first and then decreased, and reached a maximum at pulp density2.0%. However, the cell concentration and the copper leaching yield of marine volcanic type decreased with pulp density increasing. These results suggested that the copper leaching yield of three type chalcopyrite was positive correlations with the cell concentration, which is very important for bioleaching process.
To reveal the different bioleaching behaviours of chalcopyrite essentially, the nature of chalcopyrite was studied by four aspects, crystal structure, electron binding energy, valence Fe (Mossbauer spectroscopy) and mineral composition (sulfide mineral). Marine volcanic chalcopyrite had smaller lattice energy and electron binding energy, the higher the Fe2+/Fe3+content, and Cu(II) on its surface, which caused this type chalcopyrite easier to dissolved. In addition, the effects of sulfide minerals on chalcopyrite bioleaching were also studied. The results showed that pyrite, sphalerite and covellite played a negative role in porphyry type and skarn type bioleaching, whereas they had a role in promoting marine volcanic chalcopyrite bioleaching.
To reveal the biosorption mechanism of chalcopyrite essentially, the selective attachment, Zeta potential and adsorption affinity were studied. The results showed that after biosorption reached equilibrium, mineral adsorption capacity per unit area of extreme thermophilic bacteria order:skarn type> porphyry type> marine volcanic type. The Zeta potential results indicated that after biosorption, the isoelectric point (IEP) of three type chalcopyrite were consistent with the biosorption order. Analysis of the adsorption behavior of extreme thermophilic bacteria by EDLVO theory, it was found that electrostatic force (EL) played an important role in biosorption.
To reveal the dissolution mechanism of chalcopyrite essentially, the redox reaction and leaching product were studied. When extreme thermophiles bioleaching, holes in conduction band and electrons in valence band simultaneously transferring, this meant that protons (H+) and extreme thermophilic bacteria attacked chalcopyrite simultaneously. Extreme thermophilic bioleaching depended on adsorption on mineral surfaces. It was found that the products of porphyry, marine volcanic and skarn chalcopyrite were M-lacking sulfide (CuFeS) and covellite, M-rich sulfide (Cu2Fe2S), M-lacking sulfide (Cu4Fe4S5) and M-rich sulfide (Cu3.5Fe4S2.5) respectively. Elemental sulfur (S0) layer hindered porphyry and skarn chalcopyrite further dissolution, so increasing the cell concentration was favor of these types chalcopyrite dissolved. The surface of the marine volcanic chalcopyrite covered with jarosite layer, thus reducing the pH value of the solution was conducive to marine volcanic chalcopyrite leaching. In addition, reaction equation described the dissolution of three type chalcopyrite, which revealed thermophilic bioleaching mechanism.
研究了不同pH值、矿浆浓度下三种成因黄铜矿极端嗜热菌浸出特性,比较三种成因黄铜矿的浸出差异。不同pH值条件下,海相火山岩型黄铜矿浸出率均明显高于矽卡岩型黄铜矿和斑岩型黄铜矿,显示了海相火山岩型黄铜矿较易浸出。斑岩型黄铜矿菌体浓度和浸出率随着pH值升高先增高后降低,并在pH值为1.5时达到最高；而海相海相火山岩型和矽卡岩黄铜矿则是随着pH值升高不断增高。不同矿浆浓度条件下,三种成因黄铜矿浸出行为具有较大的差异。其中斑岩型和矽卡岩黄铜矿菌体浓度和浸出率随着矿浆浓度的升高均为先升高后降低,并在矿浆浓度为2.0%时达到最高,而海相火山岩型黄铜矿在矿浆浓度为0.5%时,菌体浓度和浸出率最高,随着矿浆浓度的升高而降低。通过条件实验分析发现,三种成因黄铜矿的浸出率与其菌体浓度完全成正相关性,为寻找适宜的浸出工艺参数提供依据。
通过晶体结构、电子结合能、穆斯堡尔谱Fe的价态和矿物组成(硫化矿物组分)等四个方面对三种成因黄铜矿的矿物性质进行了深入分析,从原矿本质上揭示了三种黄铜矿浸出差异的本源原因。海相火山岩型黄铜矿具有较小的晶格能和电子结合能、较高的Fe2+/Fe3+的含量,同时表面含有一部分有助于浸出进行的Cu(II),使得该类黄铜矿具有较好的浸出特性。此外,还研究了黄铜矿中所含硫化矿物组分对浸出的影响,研究发现黄铁矿、闪锌矿和铜蓝这三种硫化矿物对斑岩型和矽卡岩型黄铜矿的极端嗜热菌浸出具有阻碍作用,而对海相火山岩型黄铜矿的极端嗜热菌浸出具有一定的促进作用。
通过选择性吸附、电动性质和吸附作用力性质等方面对三种成因黄铜矿极端嗜热菌的吸附机理进行了深入分析,从吸附机理上揭示了浸出差异的过程原因。不同影响因素下极端嗜热菌在斑岩型、海相火山岩型、矽卡岩型黄铜矿表面的吸附规律表明,矿物单位面积微生物吸附量的大小顺序为：矽卡岩型>斑岩型>海相火山岩型。通过分析三种成因黄铜矿与极端嗜热菌作用后的Zeta电位,揭示了三种成因黄铜矿的等电点(IEP)与极端嗜热菌在其表面的吸附率高低相一致。利用EDLVO理论对微生物吸附行为的分析,进一步揭示了极端嗜热菌在三种成因黄铜矿表面的吸附受静电(EL)作用的控制。
通过浸出过程中氧化还原反应分析与浸出产物分析,揭示三种成因黄铜矿在极端嗜热菌浸出时的溶解途径,从而通过溶解途径的研究揭示浸出差异的本质原因。极端嗜热菌浸出时,质子(H+)与极端嗜热菌的共同作用,使得黄铜矿价带空穴和导带电子的转移同时发生。极端嗜热菌对黄铜矿浸出的作用,取决于其在矿物表面的吸附。斑岩型、海相火山岩型及矽卡岩型黄铜矿生成的产物分别为缺M-硫化物(CuFeS)与铜蓝、富M-硫化物(Cu2Fe2S)及缺M-硫化物(Cu4Fe4S5)与富M-硫化物(Cu3.5Fe4S2.5)。三种成因黄铜矿生成单质硫(S0)及黄钾铁矾。单质硫(S0)层阻碍了斑岩型及矽卡岩型黄铜矿进一步溶解,所以提高极端嗜热菌的菌体浓度,有利于这两种成因黄铜矿的溶解。而海相火山岩型黄铜矿的表面覆盖有黄钾铁矾层,因此降低浸出溶液的pH值,有利于海相火山岩型黄铜矿的溶解。此外,进一步描述了三种成因黄铜矿的溶解反应方程式,从而揭示了三种成因黄铜矿在极端嗜热菌浸出时的溶解机理。
The thermophiles bioleaching behaviours and mechanisms of chalcopyrite with distinct genetic types were studied in the present thesis. The chalcopyrite samples are from porphyry type, marine volcanic type, skarn type copper deposit. On the basis of identification and domestication, different thermophiles bioleaching conditions of experiments were carried out, such as different pH values and pulp concentration. To investigate the different bioleaching behaviours, the nature of minerals, the biosorption mechanism, and the dissolution were analyzed. This study provided the theoretical basis of the thermophiles bioleaching mechanisms of chalcopyrite.
The effects of pH values and pulp density on the thermophiles bioleaching behaviours of chalcopyrite with distinct genetic types were studied. Under different pH values leaching conditions, the copper leaching yield of marine volcanic chalcopyrite was significantly higher than the porphyry type and skarn type. This result indicated that the marine volcanic type is easier to dissolve than the other two type chalcopyrite. As pH value increasing, the cell concentration and the copper leaching yield of porphyry chalcopyrite increased first and then decreased, and reached a maximum at pH1.5. However, the cell concentration and the copper leaching yield of marine volcanic type and skarn type increased with pH value increasing. Under different pulp density, there were greater differences between behaviours. As pulp density increasing, the cell concentration and the copper leaching yield of porphyry type and skarn type increased first and then decreased, and reached a maximum at pulp density2.0%. However, the cell concentration and the copper leaching yield of marine volcanic type decreased with pulp density increasing. These results suggested that the copper leaching yield of three type chalcopyrite was positive correlations with the cell concentration, which is very important for bioleaching process.
To reveal the different bioleaching behaviours of chalcopyrite essentially, the nature of chalcopyrite was studied by four aspects, crystal structure, electron binding energy, valence Fe (Mossbauer spectroscopy) and mineral composition (sulfide mineral). Marine volcanic chalcopyrite had smaller lattice energy and electron binding energy, the higher the Fe2+/Fe3+content, and Cu(II) on its surface, which caused this type chalcopyrite easier to dissolved. In addition, the effects of sulfide minerals on chalcopyrite bioleaching were also studied. The results showed that pyrite, sphalerite and covellite played a negative role in porphyry type and skarn type bioleaching, whereas they had a role in promoting marine volcanic chalcopyrite bioleaching.
To reveal the biosorption mechanism of chalcopyrite essentially, the selective attachment, Zeta potential and adsorption affinity were studied. The results showed that after biosorption reached equilibrium, mineral adsorption capacity per unit area of extreme thermophilic bacteria order:skarn type> porphyry type> marine volcanic type. The Zeta potential results indicated that after biosorption, the isoelectric point (IEP) of three type chalcopyrite were consistent with the biosorption order. Analysis of the adsorption behavior of extreme thermophilic bacteria by EDLVO theory, it was found that electrostatic force (EL) played an important role in biosorption.
To reveal the dissolution mechanism of chalcopyrite essentially, the redox reaction and leaching product were studied. When extreme thermophiles bioleaching, holes in conduction band and electrons in valence band simultaneously transferring, this meant that protons (H+) and extreme thermophilic bacteria attacked chalcopyrite simultaneously. Extreme thermophilic bioleaching depended on adsorption on mineral surfaces. It was found that the products of porphyry, marine volcanic and skarn chalcopyrite were M-lacking sulfide (CuFeS) and covellite, M-rich sulfide (Cu2Fe2S), M-lacking sulfide (Cu4Fe4S5) and M-rich sulfide (Cu3.5Fe4S2.5) respectively. Elemental sulfur (S0) layer hindered porphyry and skarn chalcopyrite further dissolution, so increasing the cell concentration was favor of these types chalcopyrite dissolved. The surface of the marine volcanic chalcopyrite covered with jarosite layer, thus reducing the pH value of the solution was conducive to marine volcanic chalcopyrite leaching. In addition, reaction equation described the dissolution of three type chalcopyrite, which revealed thermophilic bioleaching mechanism.
引文
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