Speciation of heavy metals in estuarine sediments in the northeast of Brazil

An analytical procedure involving a three-step sequential extraction was used to determine the chemical association of heavy metals (Zn, Cr, Mn and Fe) with the major phases (exchangable, reducible and oxidizable) in samples from a fishpond of estuarine sediments. The pond is located in the Capibaribe River estuary, within the boundaries of the city of Recife, in the State of Pernambuco in the northeast of Brazil. The total metal content was determined as well. All metals were extracted from the residual fraction at a percentage greater than 50%.     

FeCl3改性MOFs在低温下对Hg0的吸附性能

为提高吸附剂对Hg0（零价汞）的吸附效率,利用MOFs（金属有机框架）材料发达的孔隙结构和高比表面积（1 997.010 0 m2/g）,采用FeCl₃溶液浸渍改性,制备了吸附剂FeCl₃@MIL-101（Cr）用于脱除Hg0.在小型固定床反应器上考察了浸渍浓度、反应温度、氧含量等对Hg0去除的影响.结果表明:FeCl₃@MIL-101（Cr）在进口ρ（Hg0）为2×10-3 mg/L,c（FeCl₃）为0.2 mol/L,反应温度60℃,气体流速400 mL/min,φ（O₂）为1%的条件下,吸附穿透时间长达62 h,相应的吸附容量为14.27 mg/g.在此基础上,进一步利用BET（比表面积测试）、SEM（扫描电镜）-EDX（能量色散X射线光谱）、XRD（X射线衍射）、XPS（X射线光电子能谱）等常用表征手段研究了改性前后吸附剂的物理化学特性,证明了吸附剂FeCl₃@MIL-101（Cr）吸附零价汞是物理吸附与化学吸附共同作用的结果,含氯官能团在吸附Hg0过程中也发挥了相当大的作用,并且氧气可促进其吸附效果.最后,分析了其吸附机理.研究显示,该种吸附剂在低温条件下具有较为优良的脱汞性能,应用前景良好.      

厌氧条件下可溶性有机质对汞的还原与氧化作用

在沉积物、湿地和淹水的水稻土中天然可溶性有机质(DOM),如胡敏酸(HA)和富里酸(FA)处于还原状态,其介导Hg(Ⅱ)的还原,影响汞的转化及地球化学循环.本文通过模拟黑暗厌氧环境,研究还原态HA与FA对Hg(Ⅱ)的还原.结果表明,还原态HA与FA的还原容量高于对照氧化态HA与FA.还原态HA与FA对Hg(Ⅱ)的还原最佳浓度分别是0. 2mg·L~(-1)和1. 5 mg·L~(-1).而高于最佳浓度时,由于发生巯基竞争性络合作用,抑制Hg(Ⅱ)的还原;特别是还原态HA大于5mg·L~(-1)时,不能还原Hg(Ⅱ)为Hg(0).还原态HA与FA对Hg(Ⅱ)的还原反应动力学表明:有机碳(DOC)与Hg(Ⅱ)摩尔比DOC∶Hg(Ⅱ)=400∶1时,还原反应速率IHSS-HA FRC-HA FRC-FA;高摩尔比[DOC∶Hg(Ⅱ)=10 000∶1]时,还原态HA对Hg(Ⅱ)的还原反应停止,甚至向相反方向进行.还原态HA与FA对Hg(0)氧化结果表明,当还原态HA与FA浓度分别增加至5 mg·L~(-1)和10 mg·L~(-1)时,样品中检测不到Hg(0),还原态HA与FA对Hg(0)发生诱导性氧化络合作用.在汞的氧化还原与络合作用中,还原态DOM扮演双重角色,影响活性汞的可利用性,进而影响微生物汞的甲基化.     

蝉中汞含量及其分布特征研究

研究了葫芦岛氯碱-有色冶金化工区蝉汞、膜翅汞及蝉蜕汞的含量,比较了蝉与其它昆虫汞含量的差异,探讨了汞在蝉体内的分布特征.结果表明,蝉汞含量很高,平均值为2.64 mg.kg-1,远高于对照点地区蝉汞含量(平均为1.00 mg.kg-1);蝉中汞的分布特征为蝉汞膜翅汞(平均为0.98 mg.kg-1)蝉蜕(平均为0.50 mg.kg-1);不同性别蝉体质量、汞含量存在显著差异,雌性蝉体质量(平均为1.11 g)显著高于雄性(平均为0.54 g);雌性蝉汞含量(平均为1.34 mg.kg-1)要显著低于雄性汞含量(平均为3.38 mg.kg-1);不同采样点中蝉汞含量差异明显,但是膜翅汞含量差异较小;蝉汞含量与土壤汞含量之间不存在显著的相关关系.蝉汞含量低于生命周期较长的蜻蜓汞含量,但是却远高于生命周期较短的其它昆虫,反映了环境汞污染在长生命周期昆虫的累积效应.     

影响大气汞化学过程的敏感因子分析

为了分析汞在大气中的化学行为,在一个化学模式中加入汞的气相、气液平衡和液相反应,模拟大气汞及其化合物的演变规律,并分析了气象因子(云、光解率、温度)和化学因子(气态O3、H2O2、HO2、OH和气态零价汞Hg0(g))的初始体积分数对各形态汞及其化合物浓度和Hg0(g)转化率的影响.模拟结果表明,在中等大气污染条件下,Hg0(g)的每小时平均转化率为2.91%.敏感性试验结果表明,云量、光解率、温度、O3和Hg0(g)的初始体积分数对不同形态汞的影响较为显著.云量的增加、光解率的增加、臭氧初始体积分数的升高,各形态汞的平衡时间缩短,除气态氧化汞和一价汞离子外,其他形态汞的平衡浓度均会降低,Hg0(g)的转化率增加.温度增加将抑制Hg0(g)的转化.Hg0(g)的初始体积分数增加,各形态汞的浓度升高,但其平均转化率没有显著变化.不同因子对汞化学过程的相对作用对区域或全球大气汞的环境模拟具有指导意义.     

含汞有害固体废弃物的固化/稳定化技术研究进展

总结了国外含汞有害固体废弃物固化技术的研究和应用发展现状。系统阐述了研究和应用较多的三种固化技术(水泥基、低温化学键磷酸盐陶瓷,硫聚合物)的固化过程原理、特征,研究和应用现状以及可得的操作数据。介绍了新兴的可能用于含汞固体废弃物的材料的研究数据。比较了各种技术的优缺点,应用上的局限性,为含汞固体废弃物的固化处理新技术的发展提供思路。     

污泥在堆肥及油污土壤修复中重金属形态的研究

污泥堆肥工艺是实现污泥减量化,无害化和资源化的重要手段。文章考察了污泥在堆肥前后四类重金属(铜、锌、铅和镉)形态的变化。结果显示,铜、锌、铅和镉在堆肥前后的总量变化不大,Cu、Zn主要以有机结合态和残渣态形式存在,而Pb、Cd主要以残渣态形式存在。堆肥处理过程中可交换态重金属都呈下降趋势,但各种重金属的可交换态变化幅度不同,以Zn和Cd下降幅度最大,Zn的可交换态由堆肥前的10.5%下降到堆肥后的4.8%;Cd的可交换态从堆肥前的3.2%下降到堆肥后的1.8%,下降比例超过和接近50%。随着向土壤中添加污泥及堆肥量的增加,小麦植株地上和地下部分重金属含量也相应增加,且地下部分含量高于地上部分,小麦中重金属含量在地下部与地上部之间的比值恒定,特别是Pd,Cd的地上和地下部分浓度比可分别达到130和15～20,经堆肥处理的污泥可以降低小麦对其中重金属的吸收。将污泥及堆肥腐熟品添加至石油污染土壤中,与对照相比土壤中的石油烃含量有一定幅度的下降,最大下降幅度为19.6%。处理一个月后重金属含量及其形态变化不大,Zn具有向铁锰氧化态转化的趋势。     

循环流化床干法脱硫除尘一体化工艺去除汞探讨研究

目前,由于人类污染源每年向大气排汞量日益增长,使国际上对汞排放的控制研究成为热点,本文通过理论计算及工程实例说明了循环流化床干法烟气脱硫除尘一体化工艺系统可以有效地控制燃煤电厂汞的排放。     

Evaluation of mercury speciation and removal through air pollution control devices of a 190 MW boiler

Air pollution control devices (APCDs) are installed at coal-fired power plants for air pollutant regulation. Selective catalytic reduction (SCR) and wet flue gas desulfurization (FGD) systems have the co-benefits of air pollutant and mercury removal. Configuration and operational conditions of APCDs and mercury speciation a ect mercury removal e ciently at coal-fired utilities. The Ontario Hydro Method (OHM) recommended by the U.S. Environmental Protection Agency (EPA) was used to determine mercury speciation simultaneously at five sampling locations through SCR-ESP-FGD at a 190 MW unit. Chlorine in coal had been suggested as a factor a ecting the mercury speciation in flue gas; and low-chlorine coal was purported to produce less oxidized mercury (Hg2+) and more elemental mercury (Hg0) at the SCR inlet compared to higher chlorine coal. SCR could oxidize elemental mercury into oxidized mercury when SCR was in service, and oxidation e ciency reached 71.0%. Therefore, oxidized mercury removal e ciency was enhanced through a wet FGD system. In the non-ozone season, about 89.5%–96.8% of oxidized mercury was controlled, but only 54.9%–68.8% of the total mercury was captured through wet FGD. Oxidized mercury removal e ciency was 95.9%–98.0%, and there was a big di erence in the total mercury removal e ciencies from 78.0% to 90.2% in the ozone season. Mercury mass balance was evaluated to validate reliability of OHM testing data, and the ratio of mercury input in the coal to mercury output at the stack was from 0.84 to 1.08.     

Efficiency of white lupin in the removal of mercury from contaminated soils： Soil and hydroponic experiments

This study examined the ability of the white lupin to remove mercury (Hg) from a hydroponic system (Hg concentrations 0, 1.25, 2.5, 5 and 10 μmol/L) and from soil in pots and lysimeters (total Hg concentration (19.2 ± 1.9) mg/kg availability 0.07%, and (28.9 ± 0.4) mg/kg availability 0.09%, respectively), and investigated the accumulation and distribution of Hg in different parts of the plant. White lupin roots efficiently took up Hg, but its translocation to the harvestable parts of the plant was low. The Hg concentration in the seeds posed no risk to human health according to the recommendations of the World Health Organization, but the shoots should not be used as fodder for livestock, at least when unmixed with other fodder crops. The accumulation of Hg in the hydroponically-grown plants was linear over the concentration range tested. The amount of Hg retained in the roots, relative to the shoots, was almost constant irrespective of Hg dose (90%). In the soil experiments, Hg accumulation increased with exposure time and was the greater in the lysimeter than in the pot experiments. Although Hg removal was the greater in the hydroponic system, revealing the potential of the white lupin to extract Hg, bioaccumulation was the greatest in the lysimeter-grown plants; the latter system more likely reflects the true behaviour of white lupin in the field when Hg availability is a factor that limits Hg removal. The present results suggest that the white lupin could be used in long-term soil reclamation strategies that include the goal of profitable land use in Hg-polluted areas.