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1.
对石门4处典型不同种类的含砷尾矿进行样品采集,并采用1种氧化菌(氧化亚铁硫杆菌,Thiobacillus ferrooxidans,简称T.f)和2种还原菌(硫酸盐还原菌,sulfate reducing bacteria,简称SR;嗜酸铁还原菌,Acidiphilium cryptum JF-5,简称JF-5)分别对其进行作用,据此研究生物还原和氧化条件下原生和次生含砷矿物的释砷情况,进而确定潜在的释砷风险。ICP-OES定量分析显示,3种细菌作用后,雄黄矿和雌黄矿的砷释出浓度都不断升高。168 h氧化菌T.f作用后的砷释出顺序为雌黄矿>淋滤液次生含砷矿物>雄黄矿>含砷夹矸尾矿。LC-AFS原子荧光分析释出液砷形态结果表明:①T.f作用后,雄黄矿和雌黄矿表现出非常明显的差异;1.5 h作用后4种含砷矿物释放As(Ⅴ)的顺序为含砷夹矸尾矿>雄黄矿>淋滤液次生含砷矿物>雌黄矿;②2种还原菌作用后,SR更能促进雌黄矿释放的As(Ⅲ),其释放量是JF-5的2倍;雌黄矿释出As(Ⅲ)在168 h达到20.64 mg/L(SR)和9.54 mg/L(JF-5)。96 h SR作用后4种含砷矿物释放As(Ⅲ)的顺序为雌黄矿>淋滤液次生含砷矿物>含砷夹矸尾矿>雄黄矿。96 h JF-5作用后4种含砷矿物释放As(Ⅲ)的顺序为雄黄矿>雌黄矿>含砷夹矸尾矿>淋滤液次生含砷矿物。 相似文献
2.
土著微生物作用下含水层沉积物砷的释放与转化 总被引：4，自引：0，他引：4
在原位采集内蒙古河套平原高砷含水层中沉积物和土著微生物的基础上,进行了室内微生物淋滤实验研究。实验过程中,使用了3种水溶液(包括去离子水和2种人工配水)和2种营养条件(包括添加2%葡萄糖和未添加葡萄糖)。结果表明,葡萄糖可强化土著微生物的活性,使得悬浮液pH值明显降低,并增加悬浮液中As质量浓度。配水成分影响悬浮物中As质量浓度。在第9 d之后,添加葡萄糖的样品中存在一定强度的硫酸根还原作用,且这种脱硫酸作用受配水成分的影响较小。研究表明,土著微生物影响下砷的释放和转化过程包括沉积物中As(V)的释放、溶液中As(V)的还原以及沉积物中As(Ⅲ)的释放等。与溶液As(V)相比,As(Ⅲ)更有利于沉积物As的释放。在As释放的过程中,溶液中Fe/Mn含量同时增加,且呈很好的线性相关关系。这意味着土著微生物作用下Fe/Mn氧化物矿物的还原性溶解是导致沉积物As释放的主要原因之一。 相似文献
3.
矿渣和酸性矿山废水的排放会使矿区周围的农田受到污染。为研究厌氧条件下矿区农田中氮和砷之间的联系,本文通过摇瓶实验探究了含砷水铁矿在厌氧含氮农田中释放的砷形态的变化,通过柱实验探究了水稻生长对氮、砷形态和浓度的影响。研究结果发现,在厌氧条件下,外源氮的加入促进了砷污染水稻土中As(Ⅴ)的还原,使生成的As(Ⅲ)浓度最高达396μg/L;在柱实验模拟的厌氧农田不同层位中,水稻的生长过程促进了氮和砷的还原以及砷向下层位的迁移,使装置中的As(Ⅲ)浓度最高达517μg/L;摇瓶实验和柱实验在相近的厌氧条件下,NO-3的存在能够直接参与As(Ⅴ)还原。研究结果为农田砷污染的治理提供了一定的参考价值。 相似文献
4.
含砷尾矿中砷(As)及伴生元素铊(Tl)等毒性元素易向周边水和土壤介质中迁移,揭示尾矿中毒性元素的矿相特征及其释放机制具有重要意义。本研究以某雄黄矿区含砷尾矿为研究对象,结合化学分析、矿物学表征等手段,通过静态浸出实验探究含砷尾矿中As和Tl的矿相特征及其释放机制。研究结果表明,含砷尾矿中As和Tl的环境行为明显受到其矿相特征及赋存形态影响。矿物学分析结果显示尾矿中As的主要矿物相为砷铂矿和砷铁矿,矿物解离度表明砷矿物处于风化状态,As释放风险较高;而Tl则以伴生元素形式存在于Ca、Mn和Mg等矿物相中,这些矿物的沉淀溶解控制着尾矿中Tl的释放。尾矿中As主要以铁锰氧化物结合态和有机结合态存在,Tl主要以铁锰氧化物结合态和残渣态存在。酸性浸出条件下金属的活性态比例增高,可交换态As由0.29%上升至1.67%,可交换态Tl从5.46%升高至8.67%;尾矿中As释放加强而Tl受到抑制,表明尾矿中As与Tl释放存在竞争关系。As的浸出符合双常数模型,为多因素控制的物理和化学过程;Tl的浸出符合抛物线扩散模型,由结构掺入和表面吸附等扩散机制控制。本研究明确了含砷尾矿As和Tl的释放特性、化... 相似文献
5.
微生物参与铁氧化物矿物的还原性溶解是高砷地下水形成的关键过程,其中具有砷还原功能的微生物如何参与含水层砷释放的生物地球化学过程亟待研究.利用从江汉平原典型高砷含水层中厌氧条件下分离出的四株细菌(Citrobacter sp.JH-1、Clostridium sp.JH-6、Exiguobacterium sp.JH-13、Paenibacillus sp.JH-33),通过室内厌氧模拟培养实验,查明其砷、铁还原能力,并通过分别与铁氧化物矿物及原位沉积物共同培养,探究原位含水层微生物参与的砷释放机理.结果表明:四株细菌均具有厌氧条件下砷、铁还原功能,Citrobacter sp.JH-1砷还原能力最强,96 h内还原的As(Ⅴ)浓度为2.22 μmol/L.其中Citrobacter sp.JH-1不仅可在厌氧和有氧条件下还原溶液中的As(Ⅴ),还可在厌氧条件下还原溶液中的Fe(Ⅲ)和无定型的水铁矿,在与含水层沉积物共培养12 d后,沉积物中铁与砷的释放量分别为510 mg/kg及1 150 μg/kg.江汉平原含水层中的原位微生物兼具砷/铁还原功能,在厌氧条件下可还原沉积物中的铁氧化物矿物并促进砷的释放,为深入揭示高砷地下水成因机理与地下水砷污染的防控提供重要科学依据. 相似文献
6.
毒砂是常见的含砷硫化物矿物,其化学式为FeAsS,它的氧化还原过程密切与砷的释放和滞留有关。本次研究采用氧化亚铁硫杆菌(Thiobacillus ferrooxidans)和嗜酸铁还原菌(A.CryptumJF-5)分别代表生物氧化过程和还原过程,将其与毒砂连续作用30 d,从地球化学和次生矿物学角度讨论氧化还原过程对毒砂中砷释放的影响。结果表明,Thiobacillus ferrooxidans与毒砂作用30 d其砷的释放浓度要比非生物条件高3倍,生物氧化作用后的毒砂红外光谱、X射线衍射仪和扫描电镜同时显示出现结晶度更好的黄钾铁矾(KFe_3(SO_4)~2OH)_6。这些氧化蚀变后的毒砂再与A.CryptumJF-5作用30 d,高活性的JF-5(pH=2)要高于低活性的JF-5(pH=3)80 mg/L。这表明还原过程能够引起氧化过程中释放-再固定的砷从次生矿物中释放出来。这些还原次生矿物的红外光谱在793 cm~(-1)波数出现一个弱振动,XPS结果表明微生物还原过程引起砷的价态从As(V)变为As(III)。SEM电镜揭示还原过程引起次生矿物形貌出现明显的变化。 相似文献
7.
硫在铁和砷的生物地球化学循环中发挥着重要作用,但地下水系统中硫循环的中间产物S(0)对细菌转化铁和砷的影响尚不清楚.采用室内模拟实验,研究硫参与下细菌D2201对液相和载砷针铁矿中Fe(III)和As(V)的还原作用.结果表明:细菌D2201具有很强的铁还原能力,可以将液相中74%的Fe(III)还原;加入硫后,细菌还原S(0)产生的S(-II)使铁还原率提高到94%.但是,硫没有明显影响细菌对砷的还原.在实验初期,细菌明显加速了载砷针铁矿的还原,最终还原释放到液相中的Fe(II)浓度为32.12 μmol/L;硫的加入增强了细菌对载砷针铁矿的还原,还原溶解的Fe(II)增加至284.13 μmol/L,同时,砷的释放量也增加了1.6倍.这些结果表明硫显著促进了细菌对针铁矿的还原溶解并加速砷的释放.XRD和SEM-EDS结果显示,细菌还原针铁矿但不改变其矿相,而硫的加入也仅使矿物发生一定程度的团聚,并没有使其转变为其他矿物,也未导致砷的再吸附. 相似文献
8.
含水层沉积物中含铁矿物的特征与活性会影响砷的迁移转化行为。通过内蒙古含水层沉积物含铁矿物的溶解、还原动力学实验,研究了沉积物含铁矿物特征和活性及其与砷运移的关系。结果表明,沉积物中具还原活性的铁氧化物总量(m0)与岩性有关,细砂为52 μmol/g,黏土为45 μmol/g。初始还原速率k′均在10-5 s-1的数量级。表征活性均匀度的参数γ值介于合成铁氧化物矿物和表层沉积物之间。沉积物中Fe(Ⅲ)氧化物的还原活性主要介于人造纤铁矿与针铁矿的活性水平范围内。沉积物中可能存在两类活性水平不同的Fe(Ⅲ)氧化物。As更倾向于吸附在活性较强的Fe(Ⅲ)氧化物上。还原环境中,活性较强的Fe(Ⅲ)氧化物的还原性溶解,促进了沉积物中砷的释放。 相似文献
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10.
铁盐絮凝法对阳宗海湖泊水体的除砷效果及底泥的稳定性考察 总被引：1，自引：0，他引：1
2008年,昆明阳宗海受到严重砷污染,砷浓度高达0.134 mg/L。项目组充分考虑其受污染水体容量大、砷浓度低的实际情况,提出了安全、廉价、高效的FeCl3絮凝法治理方案。实验室小试结果表明,提出的FeCl3絮凝法对As(Ⅲ)及As(V)均有理想的去除效果,并且湖水中大量存在的阴离子HCO-3可使治理过程中水体pH值基本保持不变。因此该方案摒弃了文献普遍报道所需要的预氧化及调节pH值的工艺步骤,将固体FeCl3·6H2O溶解、用湖水稀释后通过喷洒船将最终浓度为1%左右的FeCl3水溶液喷洒到湖面上,使湖水中的AsO3-4及AsO-2与FeCl3水解过程产生的Fe(OH)3胶体絮凝形成稳定的沉淀物被固定于底泥中。在对阳宗海进行降砷工程化治理期间,2009年11月-2010年9月砷浓度从0.117 mg/L快速下降到0.021 mg/L并可持续达到Ⅱ-Ⅲ类水标准(<0.05 mg/L),总除砷率高达 82.05%。沉积物中的As绝大部分以残渣态的形式被固定在沉积物中,生态风险很低。 相似文献
11.
Mobilization of natural arsenic in groundwater: targeting low arsenic aquifers in high arsenic occurrence areas 
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下载免费PDF全文 研究表明饮用水中微小数量的砷会对人类健康产生不利影响.世界上居住在贫穷地区的人数超过了100万,目前他们正直接饮用来自含水层中砷离子含量(>10μg/L)非安全标准的地下水.砷有时称为毒中之王,在水环境中常常以五价氧化物形式出现.自2000年以来,许多国家开始执行更为严格的10μg/L(WHO认可的居民安全饮水标准)饮用水标准,可以确定地说,在世界范围内的饮用水中检测到砷的情况越来越多.亚洲地区砷中毒的人数比世界其他地区总和还多.最受影响的地区位于南亚和东南亚富砷带,环绕恒河一雅鲁藏布江-梅克纳河三角洲及恒河平原上游的冲洪积扇含水层、红河三角洲、湄公河和伊洛瓦底江;在中国境内包括内蒙黄河冲积盆地,山西大同盆地、新疆准噶尔盆地,其中的地下水富含砷和氟化物而引发砷中毒和氟中毒.尽管还未完全掌握其中的水文地质及生物地球化学作用的详细过程,但对大多数沉积介质含水层,在还原条件下砷离子容易从沉积介质转移到地下水中.孟加拉研究实例表明地质时期尺度的冲刷降低了沉积介质中的As和有机物含量从而形成低砷地下水.这一认识为孟加拉国的降砷策略提供了科学指导,是未来水文学,矿物学,地质学和生物地球化学方面很有意义的研究方向,并有利于地砷病区低砷地下水的可持续利用. 相似文献
12.
Effect of arsenic concentration on microbial iron reduction and arsenic speciation in an iron-rich freshwater sediment 总被引：2，自引：0，他引：2
Stephanie S. Chow 《Geochimica et cosmochimica acta》2009,73(20):6008-6021
Depth profiles in the sediment porewaters of the Chattahoochee River (Georgia, USA) show that iron oxides scavenge arsenate in the water column and settle to the sediment-water interface (SWI) where they are reduced by iron-reducing bacteria. During their reduction, these particles seem to release arsenic to the porewaters in the form of arsenate only. Sediment slurry incubations were conducted to determine the effect of low concentrations of arsenic (?10 μM) on biogeochemical processes in these sediments. Experiments confirm that any arsenate (As(V)) added to these sediments is immediately adsorbed in oxic conditions and released in anoxic conditions during the microbial reduction of authigenic iron oxides. Incubations in the presence of ?1 μM As(V) reveal that arsenate is released but not concomitantly reduced during this process. Simultaneously, microbial iron reduction is enhanced significantly, spurring the simultaneous release of arsenate into porewaters and secondary formation of crystalline iron oxides. Above 1 μM As(V), however, the microbial reductive dissolution of iron oxides appears inhibited by arsenate, and arsenite is produced in excess in the porewaters. These incubations show that even low inputs of arsenic to riverine sediments may affect microbial processes, the stability of iron oxides and, indirectly, the cycling of arsenic. Possible mechanisms for such effects on iron reduction are proposed. 相似文献
13.
Control of organic and iron colloids on arsenic partition and transport in high arsenic groundwaters in the Hetao basin, Inner Mongolia 总被引：2，自引：0，他引：2
Due to the importance of colloids in regulating element transport and mobility in aquifers, As distribution in the colloidal fraction needs to be identified in high As groundwaters. Groundwater samples were filtered in the field through a progressively decreasing pore size (0.45 μm, 100, 30, 10, 5 kDa) using a filtration technique under a N2 atmosphere. Major and trace elements and organic C (OC) were measured in (ultra)filtrates. The studied groundwater samples have typical physio-chemical characteristics of the basin waters. Declines in concentrations of alkali (Na, K), alkaline-earth (Mg, Ca, Sr, Ba) elements, Mo, Si and Se during ultrafiltration are smaller relative to other elements. Arsenic, Cu, Cr, U and V are generally about 30% lower in 5 kDa ultrafiltrates in comparison with 0.45 μm filtrates. Around 50% of Fe, OC and Al are bound to colloids with grain size between 5 kDa and 0.45 μm. Two types of colloids, including large-size Fe colloids and small-size organic colloids, have been identified. Results indicate that As would be more likely to be associated with small-size organic colloids than Fe colloids. SEM images and EDS analysis and synchrotron XRF analyses confirm the association of As with NOM with molecular weights of 5-10 kDa. The better correlation between As(V) and OC in the 5-10 kDa fraction indicates that the small-size organic colloids have a greater affinity for As(V) than As(III). Arsenic associated with organic complexes may not be immobilized by adsorption, and, therefore, easily transported in the aquifer. Thus, the presence of As-containing colloidal complexes in high As groundwaters must be considered in the modeling of As transport in the aquifers. 相似文献
14.
《Applied Geochemistry》2004,19(2):169-180
Arsenic is present in aqueous environments in +III and +V oxidation states. In oxidizing environments, the principle attenuation mechanism of As migration is its adsorption on Fe(III) oxide and hydroxides. The adsorption affinity is higher for As(V) under lower pH conditions and for As(III) under higher pH conditions. Ferric oxide and hydroxides can dissolve under low Eh and pH conditions releasing adsorbed As. Oxidation-reduction processes often involve high organic matter content in sediments and also contamination by organics such as BTEX. Arsenic may desorb under high pH conditions. Changes of pH can be related to some redox reactions, cation exchange reactions driving dissolution of carbonates, and dissolution of silicates. In very reducing environments, where SO4 reduction takes place, secondary sulfide minerals like As-bearing pyrite and orpiment, As2S3, can incorporate As. Geochemical modeling can be divided into two principal categories: (a) forward modeling and (b) inverse modeling. Forward modeling is used to predict water chemistry after completion of predetermined reactions. Inverse modeling is used to suggest which processes take place along a flowpath. Complex coupled transport and geochemistry programs, which allow for simulation of As adsorption, are becoming available. A common modeling approach is based on forward modeling with surface complexation modeling (SCM) of As adsorption, which can incorporate the effect of different adsorbent/As ratios, adsorption sites density, area available for adsorption, pH changes and competition of As for adsorption sites with other dissolved species such as phosphate. The adsorption modeling can be performed in both batch and transport modes in codes such as PHREEQC. Inverse modeling is generally used to verify hypotheses on the origin of As. Basic prerequisites of inverse modeling are the knowledge of flow pattern (sampling points used in model have to be hydraulically connected) and information about mineralogy including As mineral phases. Case studies of geochemical modeling including modeling of As adsorption are presented. 相似文献
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16.
《Chemical Geology》2007,236(3-4):217-227
The association of arsenate, As(V), and arsenite, As(III), with disordered mackinawite, FeS, was studied in sulfide-limited (Fe:S = 1:1) and excess-sulfide (Fe:S = 1:2) batch experiments. In the absence of arsenic, the sulfide-limited experiments produce disordered mackinawite while the excess-sulfide experiments yield pyrite with trace amounts of mackinawite. With increasing initially added As(V) concentrations the transformation of FeS to mackinawite and pyrite is retarded. At S:As = 1:1 and 2:1, elemental sulfur and green rust are the end products. As(V) oxidizes S(-II) in FeS and (or) in solution to S(0), and Fe(II) in the solid phase to Fe(III). Increasing initially added As(III) concentrations inhibit the transformation of FeS to mackinawite and pyrite and no oxidation products of FeS or sulfide, other than pyrite, were observed. At low arsenic concentrations, sorption onto the FeS surface may be the reaction controlling the uptake of arsenic into the solid phase. Inhibition of iron(II) sulfide transformations due to arsenic sorption suggests that the sorption sites are crucial not only as sorption sites, but also in iron(II) sulfide transformation mechanisms. 相似文献
17.
《Applied Geochemistry》2003,18(8):1267-1278
At the abandoned As mine in Nishinomaki, Japan, discharged water from the mining and waste dump area is acidic and rich in As. However, the As concentration in the drainage has been decreased to below the maximum contaminant level (0.01 mg/l for drinking water, Japan) without any artificial treatments before mixing with a tributary to populated areas. This implies that the As concentration in water from the waste dump area has been naturally attenuated. To elucidate the reaction mechanisms of the natural attenuation, analysis of water quality and characterization of the precipitates from the stream floor were performed by measuring pH, ORP and electric conductivity on-site, as well as X-ray diffraction, ICP-mass spectrometry and ion-chromatography. Selective extractions and mineral alteration experiments were also conducted to estimate the distribution of As in constituent phases of the precipitates and to understand the stability of As-bearing phases, respectively. The water contamination resulted from oxidation of sulfide minerals in the waste rocks, i.e., the oxidation of pyrite and realgar and subsequent release of Fe, SO4, As(V) and proton. The released Fe(II) transformed to Fe(III) by bacterial oxidation; schwertmannite then formed immediately. While the As concentrations in the stream were lowered nearly to background level downstream, those in the ochreous precipitates were up to several tens of mg/g. The As(V) was effectively removed by the formed schwertmannite and had been naturally attenuated. Although schwertmannite is metastable with respect to goethite, the experiments show that the transformation of schwertmannite to goethite may be retarded by the presence of absorbed As(V) in the structure. Therefore, the attenuation of As in the drainage and the retention of As by schwertmannite are expected to be maintained for the long term. 相似文献
18.
J.M. Park J.S. Lee J.-U. Lee H.T. Chon M.C. Jung 《Journal of Geochemical Exploration》2006,88(1-3):134
The purpose of this study is to investigate the contamination level and chemical speciation of As in sediments from the Hwachon Au mine area, and to study the effects of indigenous bacteria on geochemical behavior of As in As-contaminated sediments from the mine. Concentrations of heavy metal and metalloids in one composite sample of 9 Hwachon sediments were 24.9 As mg/kg, 16.6 Cd mg/kg, 230 Pb mg/kg and 1080 Zn mg/kg. This indicates that this area was seriously contaminated with As, Cd and Zn. From the result of sequential extraction analysis, most of As (87.9%) existed as a phase of As which coprecipitated with Fe oxyhydroxides. Under aerobic condition, As concentration leached from sediments were 4 times higher in non-sterile than in sterile condition. This enrichment of As leaching could be caused by increase of pH and exudation secreted during microbial metabolism. On the other hand, under anaerobic condition, As concentration has dramatically increased in non-sterile solution with time. This As leaching has begun on 4–5th days of incubation and the highest concentration of 511 As μg/l was recorded on about 11th day. Arsenic leaching under anaerobic condition was caused by microbial enhancement of Fe leaching. Total Fe concentration increased from the 4th day, and this Fe leaching might cause lixiviation of As which had been coprecipitated with Fe oxyhydroxide. 相似文献
19.
X. Chris Le Xiufen LU Meiling LU Nicole Orr Zhongwen WANG Chungang YUAN 《中国地球化学学报》2006,25(B08):77-78
Arsenic is the 20th most abundant element in the Earth crust. Humans are exposed to naturally occurring and anthropogenic sources of arsenic compounds in the environment. A wide variety of adverse health effects have been attributed to chronic exposure to high levels of arsenic. More than two-dozen arsenic compounds （species） are present in the environment and in biological systems. The various arsenic species have dramatically different behavior and toxicity. This presentation briefly describes arsenic speciation analysis, human exposure to and metabolism of arsenic species. Environmental issues on arsenic in Canada are briefly discussed. These include （1） the arsenic waste left from previous gold mining and smelting activities; （2） the domestic use of wood treated with chromated copper arsenate; and （3） use of well water as the source of drinking water by approximately one third of the Canadian population. 相似文献
20.
Microorganisms play an important role in As mobilization into groundwater by directly influencing As speciation or indirectly inducing solubilisation from As-bearing phases, such as Fe, Mn and Al oxides. Iron oxide dissolution could also be induced by siderophores, small-molecule compounds produced by microorganisms to favour Fe uptake. Well waters exceeding the potable water limit of 10 μg As L−1 (0.133 μM) have been widely reported in geothermal areas. Mechanisms responsible for these high As concentrations have not yet been thoroughly elucidated and the complexity of As mobilization in volcanic aquifers is still open to multiple interpretations. The present study was based on batch release experiments aimed at verifying and quantifying the effect of siderophores on As mobilization from volcanic rocks (lava, tuff, peperino and fallout deposit) at different pH and ligand concentration. In the experiments the siderophore trihydroxamate desferroxamine B (Dfob) was used and its effect on As release from volcanic rocks was manifest after the first days. The most favourable pH for As release was pH 6 while concentrations above 250 μM Dfob considerably enhanced As and Fe concentrations in solution. The As release from rocks was between 2.0–10% at pH 6 and 2.4–8.8% at pH 8. The As/Fe ratio in solution changed with time suggesting different release mechanisms and higher mobility of As compared to Fe during the first phase of the experiment. The presence of siderophore increased Fe dissolution rates up to 10 orders of magnitude. The As release correlated with Al, Mn, Fe, Si, V, Ga and Sb and the release of all these elements increased with increasing Dfob concentration. In alkaline environments also Cu, Zn and Pb were mobilized. The presence of siderophores represents a possible trigger for As mobilization from iron binding minerals to the water phase, with interesting implications for groundwater quality, plant uptake and bacterial communities. 相似文献