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1.
为探析长江口沉积物-水界面砷的迁移转化机制,本文分析了2019年夏季长江口4个站位上覆水和间隙水中总As浓度及形态的剖面变化特征,耦合氧化还原敏感元素(Fe、Mn和S)的剖面变化剖析了沉积物-水界面砷循环的Fe-Mn-S控制机制,同时结合砷相关功能基因探讨了沉积物-水界面砷迁移转化的微生物调控过程,估算了沉积物-水界面总As的扩散通量。结果表明,除A7-4站位外,长江口其他3个站位间隙水总As以As3+为主要存在形态,且总As浓度均在上覆水中为最低值(0.748~1.57 μg·L-1),而在间隙水中随着深度增加而逐渐增加并在6~9 cm深度达到峰值(7.14~26.9 μg·L-1)。间隙水总As及As3+浓度的剖面变化趋势与溶解态Fe2+、Mn2+相似,其均在中间层出现高值,说明沉积物Fe/Mn还原带砷的释放可能是随固相Fe(Ⅲ)或Mn(Ⅳ)的还原而转移到间隙水中的。氧化层和Fe/Mn还原带过渡区间隙水砷浓度与砷异化还原菌功能基因arrA和arsC丰度存在对应关系(除A1-3站外),说明砷异化还原菌将溶解As5+或固相As5+还原为溶解As3+可能是该过渡层砷迁移转化的另一重要过程。硫酸盐还原带的间隙水总As和As3+浓度降低,但由于间隙水的低S2-浓度不利于砷硫化物生成,因此深层间隙水砷可能与铁硫矿物结合而被移除。底层环境氧化还原条件是影响沉积物-水界面砷迁移转化的重要因素,随底层水DO浓度的降低,砷迁移转化更倾向于微生物还原控制。长江口沉积物-水界面总As的扩散通量为1.18×10-7~2.07×10-7 μmol·cm-2·s-1,均表现为沉积物间隙水中总As向上覆水释放,即沉积物是研究区域水体总As的来源之一。  相似文献   

2.
思茅盆地江城含盐带勐野井地区在“二层楼”钾盐成矿理论的指导下,逐步在侏罗系钾盐资源调查中取得重要成果,但盆地内其他含盐带研究程度薄弱。本文以整董含盐带的磨黑L2井勐野井组(K1m)盐岩样品为研究对象,通过显微镜观察、扫描电镜能谱分析、石盐矿物元素含量电子探针微区原位测试方法的建立,精细研究了样品岩相学、石盐矿物学及元素含量特征。同时,测试了江城含盐带勐野井地区MK-1井花开左组(J2h)石盐样品。对比研究两个井样品中石盐矿物微量元素K和Br含量及103Br/Cl值(质量分数比)特征,结合研究区地质演化,取得以下认识。L2井K1m(含)泥砾盐岩中石盐矿物发育两类产状:一类是胶结碎屑颗粒的主体石盐,具塑性流变特征;另一类是析出在碎屑中被盐类或黏土矿物碎屑包裹的石盐,两类包裹体特征指示均属次生成因。电子探针测得L2井K1m的主体石盐、碎屑包裹和勐野井MK-1井J2h含钾盐层石盐的K含量分别为≤0.09%、≤0.18%和≤0.13%,Br含量分别为≤60×10-6、70×10-6~410×10-6和70×10-6~500×10-6,103Br/Cl值分别为≤0.10、0.12~0.71和0.12~0.85,主体石盐显著低于后二者,处于陆源或海陆混合源石盐阶段或重结晶石盐阶段,而后二者数值接近,大多处在海源石盐阶段,小部分处在海源母液结晶钾石盐阶段和光卤石阶段。推断磨黑L2井碎屑包裹的石盐属深部古盐体刺穿贯入的证据,可能的成矿模式为深部中侏罗统海相古盐体受盐底辟作用迁移到浅层下白垩统勐野井组后,部分被盆地内侧向迁移来的中侏罗世残留海水、盆地周缘汇入的陆源水以及深部热液的共同溶蚀淋滤和混染改造形成新的卤水,部分以固体古石盐砾保留下来,在早白垩世晚期新母液卤水蒸发成盐过程中被形成的盐类和陆源碎屑矿物包裹,后期在母液结晶的主体石盐胶结下沉积成岩和成矿。以上认识完善了“二层楼”成矿理论在整董含盐带的勘探实践。  相似文献   

3.
本文以阿尔金造山带南缘出露的高镁赞岐质闪长岩为研究对象,通过系统的野外地质工作、显微岩相学、年代学和全岩地球化学分析,探讨其成因类型和源区性质,限定了阿尔金造山带构造演化格架。闪长岩LA-ICP-MS锆石U-Pb测年结果表明其形成年龄为(445±3) Ma,属晚奥陶世。地球化学数据显示:闪长岩Al2O3含量为15.11%~16.19%,且具有高MgO(3.93%~5.29%)和K2O(1.68%~2.67%)含量的特征,属于高镁钙碱性准铝质岩石;闪长岩具有较高的Cr(29.3×10-6~140×10-6)、Ni(27.1×10-6~43.5×10-6)、Ba(606×10-6~936×10-6)、Sr(513×10-6~734×10-6)和Y(26.4×10-6~31.1×10-6)含量,与典型的高镁赞岐岩类地球化学特征一致;稀土配分图和微量元素蛛网图显示闪长岩样品富集轻稀土元素和大离子亲石元素(如Rb和K),而亏损高场强元素(如Nb、Ti和Zr),表现出与俯冲带环境岩浆岩相似的性质;高Ti/Zr比值(48~60)与Mg#(46.74~53.06)、高Cr(29.3×10-6~140×10-6)与高Ni(27.1×10-6~43.5×10-6)含量等暗示闪长岩岩浆源区来自遭受俯冲组分交代过的富集岩石圈地幔。岩石成因分析表明,阿尔金造山带南缘晚奥陶世高镁赞岐质闪长岩是后碰撞构造环境下俯冲板片断离诱发地幔楔发生减压熔融而形成,代表了早古生代最强烈的区域性幔源基性岩浆侵入事件。  相似文献   

4.
云南大丫口祖母绿常出现颜色环带,且伴随明显成分变化,而目前颜色环带的成因仍存争议,相关的多阶段成矿假说尚缺少明确证据。文章通过电子探针和激光剥蚀电感耦合等离子质谱仪对大丫口祖母绿的颜色环带及黑色矿物包裹体进行主微量元素成分分析,并对不同类型岩脉祖母绿中流体包裹体进行显微测温分析,进而探讨祖母绿颜色环带成因与多阶段成矿的联系。成分测试结果表明,从浅绿白核部至绿色边部,V(970×10-6→10 077×10-6)、Rb(9.6×10-6→27.4×10-6)、Cs(535×10-6→3 108×10-6)、Fe(1 376×10-6→2 199×10-6)和Ga(4×10-6→14.7×10-6)等微量元素的含量急剧增加。结合绿色晶体边部中同生黑色富钒电气石包裹体的分布,有力证明了大丫口祖母绿颜色分带的形成与晶体的多阶段成矿有关。流体包裹体测试结果表明,含矿长石-方解石脉、含矿石英脉和伟晶岩-变粒岩接触带中矿物的流体包裹体盐度范围分别为3.39%~10.36%(NaCleq)、5.71%~12.29%(NaCleq)和8%~18.72%(NaCleq),指示了伟晶岩脉中祖母绿的多阶段结晶,且表明随结晶阶段演变,成矿流体的盐度逐渐升高。同时,成矿流体盐度升高也是晚期云英岩化阶段致色元素含量剧增的原因。  相似文献   

5.
松辽盆地中二叠统哲斯组发育一套暗色泥岩、灰色砂砾岩与灰岩沉积组合,灰岩中产海相腕足类和双壳类化石。由于受钻井进尺和取心资料限制,前人对盆地覆盖区晚古生代地层及其沉积环境研究较少。对采自松辽盆地杜101井、杜103井剖面哲斯组的白云质灰岩进行了系统的稳定同位素和微量元素、稀土元素分析,首次获取了盆地覆盖区中二叠统灰岩元素地球化学资料。测试结果显示碳同位素δ13CPDB值一般>0(均值为1.68‰),氧同位素δ18OPDB值全部<-15‰(均值为-19.98‰),碳、氧稳定同位素关系图解显示二者呈正相关关系,表明白云岩化作用对灰岩同位素改造作用明显。稀土元素(REE+Y)总量为56.88×10-6~143.72×10-6,均值为108.92×10-6,PAAS标准化后显示具有轻稀土相对于中稀土和重稀土亏损、δEu(均值0.94,最大值1.57)负异常、δCe(均值0.87,最大值1.06)普遍负异常和相对高的Y/Ho均值(均值34.59)等特点,与正常海相具有大体相同的稀土元素配分模式;而微量元素Ba(均值281.55×10-6)、Zn(均值71.91×10-6)、Y(均值17.44×10-6)、Zr(均值117.75×10-6)和Rb(均值66.84×10-6)等元素含量整体较高,Sr/Ba(均值2.91)、Th/U(均值2.75)、V/Cr(均值1.45)和V/(V+Ni)(均值0.66)等比值适中,指示研究区哲斯组沉积时期主体为一种频繁受陆源碎屑混染作用影响的碳酸盐台地或滨海岸环境。  相似文献   

6.
对辽东岫岩地区锉草沟黑云母二长花岗岩、刘家堡子二云母二长花岗岩进行了岩相学观察、LA-ICP-MS锆石U-Pb年代学和地球化学测试。测年结果显示锉草沟黑云母二长花岗岩的锆石年龄为(162.7±2.5) Ma,刘家堡子二云母二长花岗岩锆石年龄为(156.9±1.1) Ma,均形成于晚侏罗世。两个岩体具有相似的地球化学特征,主量元素具有富Si、Al和K以及贫Fe、Mg和Ca的特征,A/CNK值为1.01~1.15,A/NK值为1.13~1.33;微量元素亏损Nb、P和Ti等高场强元素,富集Rb、K和Hf等不相容元素,(La/Yb)N为7.10~41.13,Eu无负异常,具有高Sr (128×10-6~454×10-6)、低Y(3.03×10-6~12.10×10-6)和Yb(0.40×10-6~1.32×10-6)特征,表现为具有埃达克质亲和性的过铝质I型花岗岩。结合两个岩体的时空特点分析认为,在晚侏罗世时期,辽东岫岩地区花岗质岩浆作用的发生是太平洋Izanaqi板块向西俯冲、西伯利亚板块与华北板块碰撞挤压造成地壳增厚,进而引发下地壳物质部分熔融的结果。  相似文献   

7.
吉林西部地区高砷地下水砷的阈值分析及风险评价   总被引：1，自引：0，他引：1  
高砷地下水导致的砷中毒是吉林西部地区近年来新发现的地方病。为评价饮用水中砷对人体健康产生的潜在危害,在野外调查、采样分析的基础上,开展了水砷安全阈值分析 ,确定了砷的总质量浓度0.05 mg/L为研究区的水砷安全阈值,建立了地下水健康风险评价模型,进行了地下水砷健康风险评价。结果表明:研究区地下水砷引起的个人年均风险度最高达2.11×10-3 a-1,其中高砷的第四系承压水中97.06%的采样点水砷对人体的个人年均致癌风险度,大于国际辐射防护委员会(ICRP)推荐的最大可接受值5.0×10-5 a-1;作为备用水源的第三系大安组、泰康组承压水69.57%采样点砷的致癌风险度也超过最大可接受风险水平。通过对风险度评价结果与砷中毒病情等资料的对比分析,风险评价结果与砷中毒病情基本一致,验证了评价结果的合理性。  相似文献   

8.
宁夏银川平原是继河套平原之后,在黄河流域发现的又一个高砷地下水分布区.为了总结其高砷地下水的水化学特征,并探索水化学因素对地下水砷释放和富集的影响机制,本文以银川平原北部（银北平原）作为典型研究区,采取野外水文地质调查、水样采集与测试、砷与水化学组分散点图相关分析及水文地球化学方法进行了综合研究.结果表明,银北平原地下水砷含量在0.2~177 μg/L之间;高砷地下水（大于50 μg/L） pH值多在7.5~8.5,水化学类型主要为HCO3-Na·Ca、Cl·HCO3-Na及Cl·HCO3-Na·Ca型,Eh多在-200~-100 mV.银北平原砷含量较高的地下水中COD、NH4+、HCO3-含量相应也较高,而NO3-和SO42-含量较低.高砷富有机质的冲-湖积含水层经过长期演化,形成偏碱性的中强还原性地下水环境和特殊的水化学特征,也具备极大的砷释放能力.较高的pH导致砷从铁锰氧化物或氢氧化物等水合物或黏土矿物表面解吸.其次部分铁锰氧化物在高pH、低Eh条件下可被还原为低价态可溶性铁锰,从而使与其结合的砷也得以释放进入地下水中.此外重碳酸根与砷酸根、亚砷酸根的竞争吸附行为促使含水层砷的解吸.  相似文献   

9.
白垩纪碰撞后花岗岩是研究大别造山带碰撞后伸展垮塌的重要载体,西大别南缘的桥店花岗斑岩脉为约束大别山碰撞后构造机制转化提供了新的约束信息。SIMS和LA-ICP-MS锆石定年结果表明,桥店花岗斑岩脉侵位年龄约为129 Ma,并具有富集的锆石Hf同位素组成(εHf(t)=-24.5-14.7)和古元古代二阶段模式年龄(2.41.9 Ga)。矿物组成上,花岗斑岩脉以富含粗粒的长石斑晶为主要特征。它们具有变化的SiO2含量(63.07%73.22%)和A/CNK值(0.871.73),同时具有高的K2O(4.51%5.47%)、低的MgO (0.42%1.82%)含量,属于高钾钙碱性花岗岩类。岩石的轻稀土元素相对重稀土元素富集,具有Eu的负异常(Eu/Eu*=0.770.92);同时富集Rb、Ba和Pb,而亏损Nb、Ta和Ti。相较于典型埃达克质岩石,桥店花岗斑岩的Sr含量(78×10-6724 ×10 -6)变化较大,Y(11.8×10-614.8×10-6)和Yb(1.09×10-61.37×10-6)含量相对较高,对应的Sr/Y(6.755.5)和(La/Yb)N(29.634.2)比值较低。以上地球化学特征,结合古元古代的残留锆石和二阶段铪模式年龄,共同反映出桥店花岗斑岩是区内古元古代下地壳物质在中-低压力条件下部分熔融的产物。与区域上碰撞后岩浆岩的对比研究表明,桥店花岗斑岩的侵位指示了西大别地壳在约129 Ma已经开始减薄,西大别白垩纪加厚下地壳的拆沉及构造机制转换的时间可能在约130 Ma前后。  相似文献   

10.
西坞口矿床是江南隆起带安徽宁国市近年来发现的首个关键金属铷(Rb)矿床,与成矿有关的岩浆岩为花岗斑岩。矿床中发育两类铷矿体:矿体I赋存于花岗斑岩体内,矿体II产于花岗斑岩体顶部。两类矿体的矿物组合均为多硅白云母+石英。矿体I呈透镜体状产于花岗斑岩体顶部,多硅白云母含量可达70%,品位为0.25%;矿体II产于花岗斑岩体和地层接触带,品位为0.21%。前人对西坞口矿床的矿化特征、岩浆岩年代学、岩浆岩成因开展了研究,但关于铷的赋存状态及成矿机制尚不明确。本次工作分别对成矿岩体和两类矿体中的主要矿物开展了电子探针(EPMA)和激光剥蚀电感耦合等离子体质谱仪(LA-ICP-MS)研究,分析结果显示花岗斑岩中斜长石、钾长石和黑云母中Rb的平均含量分别为3.10×10-6、872×10-6和1 328×10-6,矿体I和II中多硅白云母的Rb平均含量分别为2 544×10-6和2 686×10-6。多硅白云母晶体化学计算表明,铷以Rb+→K+/Na+置换的方式进入多硅白云母晶格,在多硅白云母中以类质同象的形式赋存。结合矿床地质特征和区域岩浆岩对比分析,本文提出西坞口矿床成矿岩浆具有较高的Rb背景值以及氟(F)含量,矿物结晶作用使得Rb在残余岩浆含量升高,岩浆向热液过渡阶段的富F特征导致原先岩浆体系的架状硅酸盐结构变成层状,进而有利于结晶出大量富Rb的多硅白云母,并富集形成铷矿体。  相似文献   

11.
《Geochimica et cosmochimica acta》1999,63(19-20):3379-3394
The proposed JEB Tailings Management Facility (TMF) to be emplaced below the groundwater table in northern Saskatchewan, Canada, will contain uranium mill tailings from McClean Lake, Midwest and Cigar Lake ore bodies, which are high in arsenic (up to 10%) and nickel (up to 5%). A serious concern is the possibility that high arsenic and nickel concentrations may be released from the buried tailings, contaminating adjacent groundwaters and a nearby lake. Laboratory tests and geochemical modeling were performed to examine ways to reduce the arsenic and nickel concentrations in TMF porewaters so as to minimize such contamination from tailings buried for 50 years and longer. The tests were designed to mimic conditions in the mill neutralization circuit (3 hr tests at 25°C), and in the TMF after burial (5–49 day aging tests). The aging tests were run at, 50, 25 and 4°C (the temperature in the TMF). In order to optimize the removal of arsenic by adsorption and precipitation, ferric sulfate was added to tailings raffinates1 having Fe/As ratios of less that 3–5. The acid raffinates were then neutralized by addition of slaked lime to nominal pH values of 7, 8, or 9.Analysis and modeling of the test results showed that with slaked lime addition to acid tailings raffinates, relatively amorphous scorodite (ferric arsenate) precipitates near pH 1, and is the dominant form of arsenate in slake limed tailings solids except those high in Ni and As and low in Fe, in which cabrerite-annabergite (Ni, Mg, Fe(II) arsenate) may also precipitate near pH 5–6. In addition to the arsenate precipitates, smaller amounts of arsenate are also adsorbed onto tailings solids.The aging tests showed that after burial of the tailings, arsenic concentrations may increase with time from the breakdown of the arsenate phases (chiefly scorodite). However, the tests indicate that the rate of change decreases and approaches zero after 72 hrs at 25°C, and may equal zero at all times in the TMF at 4°C. Consistent with a kinetic model that describes the rate of breakdown of scorodite to form hydrous ferric oxide, the rate of release of dissolved arsenate to tailings porewaters from slake limed tailings: (1) is proportional to pH above pH 6–7; (2) decreases exponentially as the total molar Fe/As ratio of tailings raffinates is increased from 1/1 to greater than 5/1; and (3) is proportional to temperature with an average Arrhenius activation energy of 13.4 ± 4.2 kcal/mol.Study results suggest that if ferric sulfate and slaked lime are added in the tailings neutralization circuit to give a raffinate Fe/As molar ratio of at least 3–5 and a nominal (initial) pH of 8 (final pH of 7–8), arsenic and nickel concentrations of 2 mg/L or less, are probable in porewaters of individual tailings in the TMF for 50 to 10,000 yrs after tailings disposal. However, the tailings will be mixed in the TMF, which will contain about 35% tailings with Fe/As = 3.0, and 65% tailings with Fe/As = 5.0–7.7. Thus, it seems likely that average arsenic pore water concentrations in the TMF may not exceed 1 mg/L.  相似文献   

12.
In northern Saskatchewan, Canada, high-grade U ores and the resulting tailings can contain high levels of As. An environmental concern in the U mining industry is the long-term stability of As within tailings management facilities (TMFs) and its potential transfer to the surrounding groundwater. To mitigate this problem, U mill effluents are neutralized with lime to reduce the aqueous concentration of As. This results in the formation of predominantly Fe3+–As5+ secondary mineral phases, which act as solubility controls on the As in the tailings discharged to the TMF. Because the speciation of As in natural systems is critical for determining its long-term environmental fate, characterization of As-bearing mineral phases and complexes within the deposited tailings is required to evaluate its potential transformation, solubility, and long-term stability within the tailings mass. In this study, synchrotron-based bulk X-ray absorption spectroscopy (XAS) was used to study the speciation of As and Fe in mine tailings samples obtained from the Deilmann TMF at Key Lake, Saskatchewan. Comparisons of K-edge X-ray absorption spectra of tailings samples and reference compounds indicate the dominant oxidation states of As and Fe in the mine tailings samples are +5 and +3, respectively, largely reflecting their generation in a highly oxic mill process, deposition in an oxidized environment, and complexation within stable oxic phases. Linear combination fit analyses of the K-edges for the Fe X-ray absorption near edge spectra (XANES) to reference compounds suggest Fe is predominantly present as ferrihydrite with some amount of the primary minerals pyrite (8–15% in some samples) and chalcopyrite (5–15% in some samples). Extended X-ray absorption fine structure (EXAFS) analysis of As K-edge spectra indicates that As5+ (arsenate) present in tailings samples is adsorbed to the ferrihydrite though an inner-sphere bidentate linkage.  相似文献   

13.
《Applied Geochemistry》2004,19(2):251-255
Forty-one water samples were collected and analyzed from throughout the Verde Valley watershed to identify the source of As in well water used for domestic and agricultural purposes. Each water sample was analyzed for anions, cations and trace chemical constituents by atomic absorption spectroscopy, anion chromatography and traditional wet chemical procedures. Arsenic concentrations ranged from 10 to 210 μg/l, with the highest values observed for water pooled on tailings from an abandoned Cu mine. Geostatistical analysis of the data revealed the primary source of As to be groundwater in contact with the Supai and Verde formations, as opposed to runoff from the abandoned mine tailings. Montezuma Well, a collapsed travertine spring, contained the highest levels of naturally occurring As (> 100 μg/l). Arsenic in Montezuma Well water was shown to be 100% arsenate. X-ray absorbance near edge spectra (XANES) of Potomogeton illinoiensis, an endemic plant species of Montezuma Well, demonstrate that As is absorbed as arsenate, reduced to arsenite in the plant and retained as an organic glutathione complex. XANES spectra of Montezuma Well sediments show 4 forms of As present: arsenate (∼54%), As(III)-glutathione complex (∼32%) and an As-organic complex (∼14%) containing dimethylarsinic acid and arsenobetaine. This is the first report of As(III)-glutathione in sediments.  相似文献   

14.
Arsenic and antimony contamination is found at the Pezinok mining site in the southwest of the Slovak Republic. Investigation of this site included sampling and analysis of water, mineralogical analyses, sequential extraction, in addition to flow and geochemical modeling. The highest dissolved arsenic concentrations correspond to mine tailings (up to 90,000 μg/L) and the arsenic is present predominately as As(V). The primary source of the arsenic is the dissolution of arsenopyrite. Concentration of antimony reaches 7,500 μg/L and its primary source is the dissolution of stibnite. Pore water in mine tailings is well-buffered by the dissolution of carbonates (pH values between 6.6 and 7.0) and arsenopyrite grains are surrounded by reaction rims composed of ferric iron minerals. Based on sequential extraction results, most solid phase arsenic is in the reducible fraction (i.e. ferric oxyhydroxides), sulfidic fraction, and residual fraction. Distribution of antimony in the solid phase is similar, but contents are lower. The principal attenuation mechanism for As(V) is adsorption to ferric oxide and hydroxides, but the adsorption seems to be limited by the competition with Sb(V) produced by the oxidation of stibnite for adsorption sites. Water in mine tailings is at equilibrium with gypsum and calcite, but far from equilibrium with any arsenic and antimony minerals. The concentrations of arsenic and antimony in the surrounding aquifer are much lower, with maximum values of 215 and 426 μg/L, respectively. Arsenic and antimony are transported by ground water flow towards the Blatina Creek, but their loading from ground water to the creek is much lower compared with the input from the mine adits. In the Blatina Creek, arsenic and antimony are attenuated by dilution and by adsorption on ferric iron minerals in stream sediments with resulting respective concentrations of 93 and 45 μg/L at the site boundary south of mine tailing ponds.  相似文献   

15.
Speciation and colloid transport of arsenic from mine tailings   总被引：2，自引：0，他引：2  
In addition to affecting biogeochemical transformations, the speciation of As also influences its transport from tailings at inoperative mines. The speciation of As in tailings from the Sulfur Bank Mercury Mine site in Clear Lake, California (USA) (a hot-spring Hg deposit) and particles mobilized from these tailings have been examined during laboratory-column experiments. Solutions containing two common, plant-derived organic acids (oxalic and citric acid) were pumped at 13 pore volumes d−1 through 25 by 500 mm columns of calcined Hg ore, analogous to the pedogenesis of tailings. Chemical analysis of column effluent indicated that all of the As mobilized was particulate (1.5 mg, or 6% of the total As in the column through 255 pore volumes of leaching). Arsenic speciation was evaluated using X-ray absorption spectroscopy (XAS), indicating the dominance of arsenate [As(V)] sorbed to poorly crystalline Fe(III)-(hydr)oxides and coprecipitated with jarosite [KFe3(SO4, AsO4)2(OH)6] with no detectable primary or secondary minerals in the tailings and mobilized particles. Sequential chemical extractions (SCE) of <45 μm mine tailings fractions also suggest that As occurs adsorbed to Fe (hydr)oxides (35%) and coprecipitated within poorly crystalline phases (45%). In addition, SCEs suggest that As is associated with 1 N acid-soluble phases such as carbonate minerals (20%) and within crystalline Fe-(hydr)oxides (10%). The finding that As is transported from these mine tailings dominantly as As(V) adsorbed to Fe (hydr)oxides or coprecipitated within hydroxysulfates such as jarosite suggests that As release from soils and sediments contaminated with tailings will be controlled by either organic acid-promoted dissolution or reductive dissolution of host phases.  相似文献   

16.
A minesoil has developed over 5 years oxidative exposure on sulphide concentrate tailings (ca. 1 wt.% As) at the Macraes mesothermal gold mine, New Zealand. The minesoil has a dry crust which has formed due to evaporative drying. This dry crust is enriched in arsenic (ca. 5 wt.% As) as scorodite (FeAsO4·2H2O) because of upward mobility of dissolved arsenic during drying. Similar enrichment of arsenic has occurred along the walls of desiccation cracks which extend over 1 m into the minesoil. Capping of the tailings and minesoil with wet tailings (pH=8) results in dissolution of scorodite and remobilization of arsenic on the millimetre scale. Experimental capping of the minesoil with wet calcium carbonate remobilized some arsenic from scorodite on the centimetre scale, but much original arsenic enrichment was preserved after 400 days. A layer of gypsum (CaSO4·2H2O) and iron oxyhydroxide cementation developed at the interface between the minesoil and the experimental calcium carbonate cap, restricting water flow. This layer was ca. 1 mm thick after 400 days. Theoretical comparison between advection and diffusion in the minesoil suggests that diffusion is an important mechanism for chemical mobility on the 1–50-year time scale. However, advection can be important in secondary porosity of the dry crust of the minesoil and water penetrates this zone at a rate of 1.5 mm/day.  相似文献   

17.
The tailings dam breach at the Ajka alumina plant, western Hungary in 2010 introduced ∼1 million m3 of red mud suspension into the surrounding area. Red mud (fine fraction bauxite residue) has a characteristically alkaline pH and contains several potentially toxic elements, including arsenic. Aerobic and anaerobic batch experiments were prepared using soils from near Ajka in order to investigate the effects of red mud addition on soil biogeochemistry and arsenic mobility in soil–water experiments representative of land affected by the red mud spill. XAS analysis showed that As was present in the red mud as As(V) in the form of arsenate. The remobilisation of red mud associated arsenate was highly pH dependent and the addition of phosphate to red mud suspensions greatly enhanced As release to solution. In aerobic batch experiments, where red mud was mixed with soils, As release to solution was highly dependent on pH. Carbonation of these alkaline solutions by dissolution of atmospheric CO2 reduced pH, which resulted in a decrease of aqueous As concentrations over time. However, this did not result in complete removal of aqueous As in any of the experiments. Carbonation did not occur in anaerobic experiments and pH remained high. Aqueous As concentrations initially increased in all the anaerobic red mud amended experiments, and then remained relatively constant as the systems became more reducing, both XANES and HPLC–ICP-MS showed that no As reduction processes occurred and that only As(V) species were present. These experiments show that there is the potential for increased As mobility in soil–water systems affected by red mud addition under both aerobic and anaerobic conditions.  相似文献   

18.
Windblown and vehicle-raised dust from unvegetated mine tailings can be a human health risk. Airborne particles from As-rich abandoned Au mine tailings from Nova Scotia, Canada have been characterized in terms of particle size, As concentration, As oxidation state, mineral species and texture. Samples were collected in seven aerodynamically fractionated size ranges (0.5–16 μm) using a cascade impactor deployed at three tailings fields. All three sites are used for recreational activities and off-road vehicles were racing on the tailings at two mines during sample collection. Total concentrations of As in the <8 μm fraction varied from 65 to 1040 ng/m3 of air as measured by proton-induced X-ray emission (PIXE) analysis. The same samples were analysed by synchrotron-based microfocused X-ray absorption near-edge spectroscopy (μXANES) and X-ray diffraction (μXRD) and found to contain multiple As-bearing mineral species, including Fe–As weathering products. The As species present in the dust were similar to those observed in the near-surface tailings. The action of vehicles on the tailings surface may disaggregate material cemented with Fe arsenate and contribute additional fine-grained As-rich particles to airborne dust. Results from this study can be used to help assess the potential human health risks associated with exposure to airborne particles from mine tailings.  相似文献   

19.
《Applied Geochemistry》2003,18(11):1733-1750
The Rabbit Lake U mine in-pit tailings management facility (TMF) (425 m long×300 m wide×91 m deep) is located in northern Saskatchewan, Canada. The objectives of this study were to quantify the distribution of As phases in the tailings and evaluate the present-day geochemical controls on dissolved As. These objectives were met by analyzing pore fluid samples collected from the tailings body for dissolved constituents, measuring Eh, pH, and temperature of tailings core and pore fluid samples, conducting sequential extractions on solid samples, conducting geochemical modeling of pore fluid chemistry using available thermodynamic data, and by reviewing historical chemical mill process records. Dissolved As concentrations in 5 monitoring wells installed within the tailings body ranged from 9.6 to 71 mg/l. Pore fluid in the wells had a pH between 9.3 and 10.3 and Eh between +58 and +213 mV. Sequential extraction analyses of tailings samples showed that the composition of the solid phase As changed at a depth of 34 m. The As above 34 m was primarily associated with amorphous Fe and metal hydroxides while the As below 34 m was associated with Ca, likely as amorphous poorly ordered calcium arsenate precipitates. The change in the dominant As solid phases at this depth was attributed to the differences in the molar ratio of Fe to As in the mill tailings. Below 34 m it was <2 whereas above 34 m it was >4. The high Ca/As ratio during tailings neutralization would likely precipitate Ca4(OH)2(AsO4)2:4H2O type Ca arsenate minerals. Geochemical modeling suggested that if the pore fluids were brought to equilibrium with this Ca-arsenate, the long-term dissolved As concentrations would range between 13 and 126 mg/l.  相似文献   

20.
Nearly half a century after mine closure, release of As from the Ylöjärvi Cu–W–As mine tailings in groundwater and surface water run-off was observed. Investigations by scanning electron microscopy (SEM), electron microprobe analysis (EMPA), synchrotron-based micro-X-ray diffraction (μ-XRD), micro-X-ray absorption near edge structure (μ-XANES) and micro-extended X-ray absorption fine structure (μ-EXAFS) spectroscopy, and a sequential extraction procedure were performed to assess As attenuation mechanisms in the vadose zone of this tailings deposit. Results of SEM, EMPA, and sequential extractions indicated that the precipitation of As bearing Fe(III) (oxy)hydroxides (up to 18.4 wt.% As2O5) and Fe(III) arsenates were important secondary controls on As mobility. The μ-XRD, μ-XANES and μ-EXAFS analyses suggested that these phases correspond to poorly crystalline and disordered As-bearing precipitates, including arsenical ferrihydrite, scorodite, kaňkite, and hydrous ferric arsenate (HFA). The pH within 200 cm of the tailings surface averaged 5.7, conditions which favor the precipitation of ferrihydrite. Poorly crystalline Fe(III) arsenates are potentially unstable over time, and their transformation to ferrihydrite, which contributes to As uptake, has potential to increase the As adsorption capacity of the tailings. Arsenic mobility in tailings pore water at the Ylöjärvi mine will depend on continued arsenopyrite oxidation, dissolution or transformation of secondary Fe(III) arsenates, and the As adsorption capacity of Fe(III) (oxy)hydroxides within this tailings deposit.  相似文献   

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