黄钾铁矾生物合成的影响因素及其机制研究
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摘要
酸性矿山废水(Acid Mine Drainage, AMD)由于极端酸性和富含有毒有害元素对生态环境造成的巨大影响使其成为环境科学中研究的热点。目前,AMD的治理主要采用中和法、人工湿地法和微生物法等。其中,微生物法处理酸性矿山废水因具有成本低、适用性强、无二次污染等特点而引起了学术界的广泛重视。研究发现,在富含Fe和SO42-的AMD环境下,通过微生物或非生物的作用可形成铁的硫酸盐矿物进而除去其中的有毒有害元素。其中,黄钾铁矾作为AMD中最普遍、也是最为稳定的次生铁矿物形态,因具有较强的吸附和类质同象替换能力而成为一种倍受关注的新型环境矿物材料。本文围绕AMD的治理和次生矿物的形成,在实验室中模拟与AMD类似的酸性硫酸盐环境,通过改变嗜酸性氧化亚铁硫杆菌的反应条件、化学与生物成矿的对比、控制Fe2+氧化速率和外源添加糖类物质模拟细菌胞外多聚物(EPS)的方法,探讨了促进次生矿物形成的途径及其影响机制。
1、为了研究不同环境和条件对细菌活性和次生矿物形成的影响,本文考察了细菌接种量、休止细胞保存时间、反应起始pH值,添加(NH4)2SO4、NH4HCO3和KHCO3对矿物生成量、亚铁氧化率和总铁沉淀率等的影响,并借助X射线衍射(XRD)等方法对产物进行了分析与鉴定。结果表明：(1)细菌接种量大于75%时,铁沉淀率和矿物生成量已趋于稳定；(2) A.ferrooxidans LX5休止细胞在放置超过7d以后,其氧化Fe2+的能力会有一定程度的减弱,但对后续产物的生成量没有太大影响；(3)反应溶液的起始pH在3.0-2.25范围内对矿物生成基本没什么影响,当溶液的起始pH值降至2.0后,矿物的生成量有显著降低的趋势；(4)适当低浓度的添加NH4+可以为细菌的生长提供营养物质并促进矿物的生成,但提高NH4=浓度反而对矿物的合成有抑制的趋势；(5)向反应体系中添加NH4HCO3,在NH4+和HC03的共同作用下,可以通过调控溶液的pH值和为细菌生长提供氮源和C02的途径促进矿物产量。因此,适当提高细菌接种量、调整溶液pH值和添加NH4+HCO3有利于促进矿物的形成。
2、次生矿物的形成主要通过生物合成和化学合成两种方法,为了比较这两种方法对次生矿物形成的影响,本文通过A.ferrooxidans生物氧化和H202化学氧化FeSO4的方法合成次生矿物。结果表明：(1)采用生物方法合成的矿物结晶度较好,是纯净的不含其它杂质的黄钾铁矾；而化学方法合成的矿物结晶度较差,为黄钾铁矾和施氏矿物的混合物；(2)化学法氧化Fe2+迅速,可在10min内快速大量的合成矿物；生物法对Fe2+的氧化则相对缓慢的多,需几小时后才开始有矿物生成；(3)化学法合成矿物在反应72h时总铁沉淀率为26.46%,矿物颗粒多为轮廓圆滑的球形,尺寸在2μm左右；生物法合成矿物在反应72h时总铁沉淀率为71.58%,矿物颗粒多为棱角分明的长条形,尺寸在1.5-2μm左右,团聚现象十分明显。
3、尽管前面的研究表明不同Fe2+氧化方法能够显著影响矿物的形成,但是H202氧化速率过快,容易形成大量的杂质。本文将进一步通过缓慢添加H202的方法,研究H202快速氧化、慢速氧化和生物氧化途径对次生矿物的影响。结果表明：(1)A.ferrooxidans氧化和滴加H202缓慢氧化合成的矿物均为黄钾铁矾,而在反应开始后的一段时间内快速氧化合成的矿物与施氏矿物类似,随着反应时间的延长,H202快速氧化合成的矿物发生了由施氏矿物向黄钾铁矾的相转变。可见,在反应初期,Fe2+的氧化速率越慢越容易形成晶型的黄钾铁矾；而Fe2+的氧化速率过快则容易形成施氏矿物等结晶度较差的矿物,但随着反应时间的延长,会逐渐转变为黄钾铁矾；(2)H202慢速氧化体系中Fe2+的氧化速率和矿物形成量均显著高于生物氧化,在反应结束时,H202慢速氧化形成的矿物较生物氧化体系高约30%;(3)与H202氧化相比,生物氧化体系中含有大量的EPS,这可能是造成生物氧化体系矿物合成量较低的原因。本文采用高速离心剥离EPS的方法，分析了剥离EPS的A.ferrooxidans对Fe2+氧化和矿物生成量的影响。结果发现,剥离前和剥离后的A.ferrooxidans对Fe2+的氧化能力几乎没有差异,但是剥离后的A.ferrooxidans合成的矿物量却高于剥离EPS前的A.ferrooxidans.因此,生物氧化和H202氧化方式能够显著影响次生矿物的形成,并且嗜酸性氧化亚铁硫杆菌分泌的EPS对矿物的形成具有一定的抑制作用,使得矿物生成量和铁的去除率均低于缓慢氧化的反应体系。
4、为了进一步验证EPS对矿物形成的影响,本文还采用葡聚糖模拟EPS的方法,研究在H202氧化Fe2+体系中不同浓度葡聚糖对次生铁矿物形成的影响。结果表明：(1)葡聚糖抑制了次生矿物的合成；(2)随着葡聚糖浓度的提高,次生矿物内的Fe含量降低,而S含量没有显著变化,且所有处理的K含量均较低；(3)没有葡聚糖处理的次生矿物的XRD特征峰与黄钾铁矾吻合,而添加葡聚糖后形成的次生矿物的特征峰与施氏矿物吻合,但是所有处理的次生矿物的结晶度都不高；(4)随着葡聚糖浓度的提高,次生矿物的颗粒尺寸降低,比表面积增加；(5)葡聚糖作为大分子有机物,所带的负电荷可以结合Fe3+形成配合物,使得参与生成矿物沉淀的Fe3+减少。因此,葡聚糖可以通过结合Fe3+与之形成配合物来抑制次生矿物的合成,并且阻止次生矿物由施氏矿物向黄钾铁矾的转变。
5、在EPS中除了含有大量的葡聚糖外,还含有一定量的葡萄糖。本文进一步通过采用葡萄糖模拟EPS的方法,研究在H202氧化Fe2+体系中不同浓度葡萄糖对次生铁矿物形成的影响。结果表明：(1)将Fe2(SO4)3溶解后,采用一定浓度的KOH溶液代替K2SO4,调高反应溶液的pH,同时为成矾提供一价阳离子,可在一定程度上推动由Fe3+在常温常压下合成黄钾铁矾的速率；(2)葡萄糖对H202氧化Fe2+成矿和起始供应Fe3+成矿均表现出一定的抑制作用。其中,葡萄糖对起始供应Fe3+成矿的抑制主要表现在培养初期(前72h内)；而对H202氧化Fe2+成矿的抑制更主要表现在培养后期(72-168h)。因此,葡萄糖也能在一定程度上抑制Fe2+的氧化和次生矿物的形成。
全文研究表明,在Fe2+氧化速率较快时,施氏矿物等结晶度较差的矿物是黄钾铁矾的前驱产物。A. ferrooxidans分泌的EPS对矿物的形成具有一定的抑制作用,其中的糖类组分可通过结合Fe3+、隔离分散结晶核、阻碍矿相转变等方式影响矿物的最终产量。由于生物法合成矿物受微生物条件的影响和制约,通过滴加双氧水缓慢氧化Fe2+是一种更为快速有效的沉矾除铁方法。
Acid mine drainage (AMD) is a hot research topic in environmental science area because of its extremely low pH and relatively high contents of heavy metals and metalloid. These characteristics of AMD can have a negative effect on the ecological environment. At present, the treatment of AMD is mainly focused on neutralization method, artificial wet land method, microbe method and so on. Microbe method has attracted much academic attention because of its low cost, high applicability and non-secondary pollution. Previous studies showed that iron sulfate minerals can precipitate in the AMD environment through the microbial or abiotic activity. Jarosite is the most common and stable secondary iron mineral in the AMD environment. As a new environment mineral material, jarosite has drawn special attention because of its strong adsorption and isomorphism replacement capacity.to heavy metals or metalloid.In this study, experiments were conducted in laboratory to study how to efficiently precipitate secondary minerals and its influence mechanism.
1. In order to study effects of different growth environment and conditions on A.ferrooxidans LX5activity and secondary minerals formation, the effects of inoculating amount, the storage time of resting cells, initial pH of solution,(NH4)2SO4, NH4HCO3and KHCO3on precipitates, Fe2+oxidation rate and soluble Fe removal efficiency were investigated. The results showed that:(1) when inoculating quantity was more than75%, the precipitate weight and soluble Fe removal efficiency had remained stable;(2) although the oxidability of A.ferrooxidans had weakened after conservation in4℃for7d, there was no significant difference in precipitate weight between A.ferrooxidans cells before and after condervation;(3) similar precipitate weight was observed when solution initial pH value varied between2.25to3.0, but it would be significantly decreased when initial pH value was below2.0;(4) addition of appropriate low concentration NH4+could facilitate the formation of secondary mineral for providing nitrogen resources, but high concentration of NH4+would contrarily restrain the formation of secondary mineral;(5) because of their capacity in providing N and CO2resources and adjusting solution pH value, addition of NH4HCO3could facilitate the formation of secondary mineral.
2. Secondary minerals were mainly formed through chemical and biological methods, in order to study the effects of the two methods on secondary mineral formation, Fe2+was oxidated through both biological methods and addition of H2O2. The results showed that:(1) the precipitate synthesized by bacterial method was pure jarosite and has a high crystallinity, while the precipitates synthesized by chemical method were mixture of jarosite and schwertmannite;(2) the Fe2+oxidation rate in chemosynthesis system was much faster than that in biosynthesis system;(3) in the biosynthesis system, the soluble Fe removal efficiency was about71.58%at72h, while in the chemosynthesis system, it was only26.46%. The mineral particles formed in chemosynthesis system displayed an appearance of small spheroids with a diameter of2μm, while the mineral particles formed in biosynthesis system were angular with a diameter of1.5-2μm. Otherwise, the precipitate formed in biosynthesis system indicates an obvious tendency for its particles to agglomerate.
3. Although secondary minerals can be formed through chemical methods, there are plenty of impurities in minerals for quick oxidation rate. In this part, H2O2was added slowly to investigate the effects of H2O2oxidation rate on Fe2+oxidation rate and precipitate weight. The results showed that:(1) The XRD patterns and element composition of precipitates synthesized through the biooxidation and the slow oxidation treatments were well coincide with that of potassium jarosite, while precipitates at the initial stage of incubation in the rapid oxidation treatment showed a similar XRD patterns to schwertmannite. With the ongoing incubation, XRD patterns and element composition of the rapid oxidation treatment were transformed to that in the biooxidation and the slow oxidation treatments;(2) the precipitate weight was30%higher in H2O2slow oxidation treatment than in biological treatment;(3) in contrast with chemical oxidation treatment, there was plenty of EPS in biological treatment. That might be the reason for the decreased precipitate formation. In order to analysis the effects of EPS on Fe2+oxidation rate and precipitate weight, A. ferrooxidans was centrifuged to peel off EPS. The results showed that, there was no significant difference in Fe2+oxidation rate between A. ferrooxidans with and without EPS, but the precipitate weight formed by A. ferrooxidans without EPS was higher than formed by that with EPS. Therefore, with the inhibition of A. ferrooxidans and their EPS, the amount of precipitates and soluble Fe removal efficiency were lower in the biooxidation treatment than in the slow oxidation treatment.
4. In order to reconfirm our hypothesis that EPS can inhibit precipitate formation, different concentrations of dextran were supply and Fe2+oxidation rate and precipitate weight were investigated. The results showed that:(1) dextran restrained the formation of secondary minerals;(2) with increasing dextran concentrations, The content of Fe in secondary minerals was decreased, while the content of S did not vary significantly. The content of K in all treatments was extremely low;(3) XRD pattern of secondary minerals formed without dextran were well coincide with that of jarosite, while those formed with dextran were coincide with that of schwertmannite. But the crystallization of secondary minerals in all treatments was not very good;(4) with increasing dextran concentrations, the particle sizes of secondary minerals were decreased, while specific surface area was increased.(5) as a macromolecular organic substance, dextran can form complex with Fe3+which lead to the decrease of Fe3+participated in the formation of secondary minerals. Therefore, dextran depressed the formation of secondary minerals by forming complex with Fe3+, and restrained the transformation of schwertmannite to jarosite.
5. Except for dextran, there is also plenty of glucose in EPS. In this part, the effects of different glucose concentrations on the formation of secondary iron minerals were also investigated. The results showed that:(1) addition of KOH instead of K2SO4could not only provide monovalent cations, but also increased pH value of Fe2(SO4)3solution, which would hence facilitate the transformation of Fe3+to jarosite;(2) glucose restrained the formation of precipitate from both Fe2+oxidation system and Fe3+system. The inhibitory effect was observed in the first72h in Fe3+system, while it was observed between72and168h in Fe2+oxidation system. Therefore, glucose can efficiently inhibit secondary minerals formation.
It was concluded that Fe2+oxidation rate can efficiently affect the mineral phase of precipitates. When Fe2+oxidation rate is relatively high, amorphous minerals such as schwertmannite were the precursor of jarosite. The carbohydrates in the EPS can inhibit the precipitate weight through forming complex with Fe3+, separating crystal nucleus and preventing the transformation of mineral phase. By contrast, slow oxidation treatment is an effective method in jarosite formation with less environmental restriction.
1、为了研究不同环境和条件对细菌活性和次生矿物形成的影响,本文考察了细菌接种量、休止细胞保存时间、反应起始pH值,添加(NH4)2SO4、NH4HCO3和KHCO3对矿物生成量、亚铁氧化率和总铁沉淀率等的影响,并借助X射线衍射(XRD)等方法对产物进行了分析与鉴定。结果表明：(1)细菌接种量大于75%时,铁沉淀率和矿物生成量已趋于稳定；(2) A.ferrooxidans LX5休止细胞在放置超过7d以后,其氧化Fe2+的能力会有一定程度的减弱,但对后续产物的生成量没有太大影响；(3)反应溶液的起始pH在3.0-2.25范围内对矿物生成基本没什么影响,当溶液的起始pH值降至2.0后,矿物的生成量有显著降低的趋势；(4)适当低浓度的添加NH4+可以为细菌的生长提供营养物质并促进矿物的生成,但提高NH4=浓度反而对矿物的合成有抑制的趋势；(5)向反应体系中添加NH4HCO3,在NH4+和HC03的共同作用下,可以通过调控溶液的pH值和为细菌生长提供氮源和C02的途径促进矿物产量。因此,适当提高细菌接种量、调整溶液pH值和添加NH4+HCO3有利于促进矿物的形成。
2、次生矿物的形成主要通过生物合成和化学合成两种方法,为了比较这两种方法对次生矿物形成的影响,本文通过A.ferrooxidans生物氧化和H202化学氧化FeSO4的方法合成次生矿物。结果表明：(1)采用生物方法合成的矿物结晶度较好,是纯净的不含其它杂质的黄钾铁矾；而化学方法合成的矿物结晶度较差,为黄钾铁矾和施氏矿物的混合物；(2)化学法氧化Fe2+迅速,可在10min内快速大量的合成矿物；生物法对Fe2+的氧化则相对缓慢的多,需几小时后才开始有矿物生成；(3)化学法合成矿物在反应72h时总铁沉淀率为26.46%,矿物颗粒多为轮廓圆滑的球形,尺寸在2μm左右；生物法合成矿物在反应72h时总铁沉淀率为71.58%,矿物颗粒多为棱角分明的长条形,尺寸在1.5-2μm左右,团聚现象十分明显。
3、尽管前面的研究表明不同Fe2+氧化方法能够显著影响矿物的形成,但是H202氧化速率过快,容易形成大量的杂质。本文将进一步通过缓慢添加H202的方法,研究H202快速氧化、慢速氧化和生物氧化途径对次生矿物的影响。结果表明：(1)A.ferrooxidans氧化和滴加H202缓慢氧化合成的矿物均为黄钾铁矾,而在反应开始后的一段时间内快速氧化合成的矿物与施氏矿物类似,随着反应时间的延长,H202快速氧化合成的矿物发生了由施氏矿物向黄钾铁矾的相转变。可见,在反应初期,Fe2+的氧化速率越慢越容易形成晶型的黄钾铁矾；而Fe2+的氧化速率过快则容易形成施氏矿物等结晶度较差的矿物,但随着反应时间的延长,会逐渐转变为黄钾铁矾；(2)H202慢速氧化体系中Fe2+的氧化速率和矿物形成量均显著高于生物氧化,在反应结束时,H202慢速氧化形成的矿物较生物氧化体系高约30%;(3)与H202氧化相比,生物氧化体系中含有大量的EPS,这可能是造成生物氧化体系矿物合成量较低的原因。本文采用高速离心剥离EPS的方法，分析了剥离EPS的A.ferrooxidans对Fe2+氧化和矿物生成量的影响。结果发现,剥离前和剥离后的A.ferrooxidans对Fe2+的氧化能力几乎没有差异,但是剥离后的A.ferrooxidans合成的矿物量却高于剥离EPS前的A.ferrooxidans.因此,生物氧化和H202氧化方式能够显著影响次生矿物的形成,并且嗜酸性氧化亚铁硫杆菌分泌的EPS对矿物的形成具有一定的抑制作用,使得矿物生成量和铁的去除率均低于缓慢氧化的反应体系。
4、为了进一步验证EPS对矿物形成的影响,本文还采用葡聚糖模拟EPS的方法,研究在H202氧化Fe2+体系中不同浓度葡聚糖对次生铁矿物形成的影响。结果表明：(1)葡聚糖抑制了次生矿物的合成；(2)随着葡聚糖浓度的提高,次生矿物内的Fe含量降低,而S含量没有显著变化,且所有处理的K含量均较低；(3)没有葡聚糖处理的次生矿物的XRD特征峰与黄钾铁矾吻合,而添加葡聚糖后形成的次生矿物的特征峰与施氏矿物吻合,但是所有处理的次生矿物的结晶度都不高；(4)随着葡聚糖浓度的提高,次生矿物的颗粒尺寸降低,比表面积增加；(5)葡聚糖作为大分子有机物,所带的负电荷可以结合Fe3+形成配合物,使得参与生成矿物沉淀的Fe3+减少。因此,葡聚糖可以通过结合Fe3+与之形成配合物来抑制次生矿物的合成,并且阻止次生矿物由施氏矿物向黄钾铁矾的转变。
5、在EPS中除了含有大量的葡聚糖外,还含有一定量的葡萄糖。本文进一步通过采用葡萄糖模拟EPS的方法,研究在H202氧化Fe2+体系中不同浓度葡萄糖对次生铁矿物形成的影响。结果表明：(1)将Fe2(SO4)3溶解后,采用一定浓度的KOH溶液代替K2SO4,调高反应溶液的pH,同时为成矾提供一价阳离子,可在一定程度上推动由Fe3+在常温常压下合成黄钾铁矾的速率；(2)葡萄糖对H202氧化Fe2+成矿和起始供应Fe3+成矿均表现出一定的抑制作用。其中,葡萄糖对起始供应Fe3+成矿的抑制主要表现在培养初期(前72h内)；而对H202氧化Fe2+成矿的抑制更主要表现在培养后期(72-168h)。因此,葡萄糖也能在一定程度上抑制Fe2+的氧化和次生矿物的形成。
全文研究表明,在Fe2+氧化速率较快时,施氏矿物等结晶度较差的矿物是黄钾铁矾的前驱产物。A. ferrooxidans分泌的EPS对矿物的形成具有一定的抑制作用,其中的糖类组分可通过结合Fe3+、隔离分散结晶核、阻碍矿相转变等方式影响矿物的最终产量。由于生物法合成矿物受微生物条件的影响和制约,通过滴加双氧水缓慢氧化Fe2+是一种更为快速有效的沉矾除铁方法。
Acid mine drainage (AMD) is a hot research topic in environmental science area because of its extremely low pH and relatively high contents of heavy metals and metalloid. These characteristics of AMD can have a negative effect on the ecological environment. At present, the treatment of AMD is mainly focused on neutralization method, artificial wet land method, microbe method and so on. Microbe method has attracted much academic attention because of its low cost, high applicability and non-secondary pollution. Previous studies showed that iron sulfate minerals can precipitate in the AMD environment through the microbial or abiotic activity. Jarosite is the most common and stable secondary iron mineral in the AMD environment. As a new environment mineral material, jarosite has drawn special attention because of its strong adsorption and isomorphism replacement capacity.to heavy metals or metalloid.In this study, experiments were conducted in laboratory to study how to efficiently precipitate secondary minerals and its influence mechanism.
1. In order to study effects of different growth environment and conditions on A.ferrooxidans LX5activity and secondary minerals formation, the effects of inoculating amount, the storage time of resting cells, initial pH of solution,(NH4)2SO4, NH4HCO3and KHCO3on precipitates, Fe2+oxidation rate and soluble Fe removal efficiency were investigated. The results showed that:(1) when inoculating quantity was more than75%, the precipitate weight and soluble Fe removal efficiency had remained stable;(2) although the oxidability of A.ferrooxidans had weakened after conservation in4℃for7d, there was no significant difference in precipitate weight between A.ferrooxidans cells before and after condervation;(3) similar precipitate weight was observed when solution initial pH value varied between2.25to3.0, but it would be significantly decreased when initial pH value was below2.0;(4) addition of appropriate low concentration NH4+could facilitate the formation of secondary mineral for providing nitrogen resources, but high concentration of NH4+would contrarily restrain the formation of secondary mineral;(5) because of their capacity in providing N and CO2resources and adjusting solution pH value, addition of NH4HCO3could facilitate the formation of secondary mineral.
2. Secondary minerals were mainly formed through chemical and biological methods, in order to study the effects of the two methods on secondary mineral formation, Fe2+was oxidated through both biological methods and addition of H2O2. The results showed that:(1) the precipitate synthesized by bacterial method was pure jarosite and has a high crystallinity, while the precipitates synthesized by chemical method were mixture of jarosite and schwertmannite;(2) the Fe2+oxidation rate in chemosynthesis system was much faster than that in biosynthesis system;(3) in the biosynthesis system, the soluble Fe removal efficiency was about71.58%at72h, while in the chemosynthesis system, it was only26.46%. The mineral particles formed in chemosynthesis system displayed an appearance of small spheroids with a diameter of2μm, while the mineral particles formed in biosynthesis system were angular with a diameter of1.5-2μm. Otherwise, the precipitate formed in biosynthesis system indicates an obvious tendency for its particles to agglomerate.
3. Although secondary minerals can be formed through chemical methods, there are plenty of impurities in minerals for quick oxidation rate. In this part, H2O2was added slowly to investigate the effects of H2O2oxidation rate on Fe2+oxidation rate and precipitate weight. The results showed that:(1) The XRD patterns and element composition of precipitates synthesized through the biooxidation and the slow oxidation treatments were well coincide with that of potassium jarosite, while precipitates at the initial stage of incubation in the rapid oxidation treatment showed a similar XRD patterns to schwertmannite. With the ongoing incubation, XRD patterns and element composition of the rapid oxidation treatment were transformed to that in the biooxidation and the slow oxidation treatments;(2) the precipitate weight was30%higher in H2O2slow oxidation treatment than in biological treatment;(3) in contrast with chemical oxidation treatment, there was plenty of EPS in biological treatment. That might be the reason for the decreased precipitate formation. In order to analysis the effects of EPS on Fe2+oxidation rate and precipitate weight, A. ferrooxidans was centrifuged to peel off EPS. The results showed that, there was no significant difference in Fe2+oxidation rate between A. ferrooxidans with and without EPS, but the precipitate weight formed by A. ferrooxidans without EPS was higher than formed by that with EPS. Therefore, with the inhibition of A. ferrooxidans and their EPS, the amount of precipitates and soluble Fe removal efficiency were lower in the biooxidation treatment than in the slow oxidation treatment.
4. In order to reconfirm our hypothesis that EPS can inhibit precipitate formation, different concentrations of dextran were supply and Fe2+oxidation rate and precipitate weight were investigated. The results showed that:(1) dextran restrained the formation of secondary minerals;(2) with increasing dextran concentrations, The content of Fe in secondary minerals was decreased, while the content of S did not vary significantly. The content of K in all treatments was extremely low;(3) XRD pattern of secondary minerals formed without dextran were well coincide with that of jarosite, while those formed with dextran were coincide with that of schwertmannite. But the crystallization of secondary minerals in all treatments was not very good;(4) with increasing dextran concentrations, the particle sizes of secondary minerals were decreased, while specific surface area was increased.(5) as a macromolecular organic substance, dextran can form complex with Fe3+which lead to the decrease of Fe3+participated in the formation of secondary minerals. Therefore, dextran depressed the formation of secondary minerals by forming complex with Fe3+, and restrained the transformation of schwertmannite to jarosite.
5. Except for dextran, there is also plenty of glucose in EPS. In this part, the effects of different glucose concentrations on the formation of secondary iron minerals were also investigated. The results showed that:(1) addition of KOH instead of K2SO4could not only provide monovalent cations, but also increased pH value of Fe2(SO4)3solution, which would hence facilitate the transformation of Fe3+to jarosite;(2) glucose restrained the formation of precipitate from both Fe2+oxidation system and Fe3+system. The inhibitory effect was observed in the first72h in Fe3+system, while it was observed between72and168h in Fe2+oxidation system. Therefore, glucose can efficiently inhibit secondary minerals formation.
It was concluded that Fe2+oxidation rate can efficiently affect the mineral phase of precipitates. When Fe2+oxidation rate is relatively high, amorphous minerals such as schwertmannite were the precursor of jarosite. The carbohydrates in the EPS can inhibit the precipitate weight through forming complex with Fe3+, separating crystal nucleus and preventing the transformation of mineral phase. By contrast, slow oxidation treatment is an effective method in jarosite formation with less environmental restriction.
引文
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