Geochemistry of leachates from the El Fraile sulfide tailings piles in Taxco, Guerrero, southern Mexico

Leachates from the El Fraile tailings impoundment (Taxco, Mexico) were monitored every 2 months from October 2001 to August 2002 to assess the geochemical characteristics. These leachates are of interest because they are sometimes used as alternative sources of domestic water. Alternatively, they drain into the Cacalotenango creek and may represent a major source of metal contamination of surface water and sediments. Most El Fraile leachates show characteristics of Ca–SO₄, (Ca+Mg)–SO₄, Mg–SO₄ and Ca–(SO₄+HCO₃) water types and are near-neutral (pH=6.3–7.7). Some acid leachates are generated by the interaction of meteoric water with tailings during rainfall events (pH=2.4–2.5). These contain variable levels of SO₄ ²⁻ (280–29,500 mg l⁻¹) and As (<0.01–12.0 mg l⁻¹) as well as Fe (0.025–2352 mg l⁻¹), Mn (0.1–732 mg l⁻¹), Zn (<0.025–1465 mg l⁻¹) and Pb (<0.01–0.351 mg l⁻¹). Most samples show the highest metal enrichment during the dry seasons. Leachates used as domestic water typically exceed the Mexican Drinking Water Guidelines for sulfate, hardness, Fe, Mn, Pb and As, while acidic leachates exceed the Mexican Guidelines for Industrial Discharge Waters for pH, Cu, Cd and As. Speciation shows that in near-neutral solutions, metals exist mainly as free ions, sulfates and bicarbonates, while in acidic leachates they are present as sulfates and free ions. Arsenic appears as As^(V) in all samples. Thermodynamic and mineralogical evidence indicates that precipitation of Fe oxides and oxyhydroxides, clay minerals and jarosite as well as sorption by these minerals are the main processes controlling leachate chemistry. These processes occur mainly after neutralization by interaction with bedrock and equilibration with atmospheric oxygen.     

UV/Fe3+/H2O2体系降解活性艳橙X-GN废水的研究

采用UV/Fe3 /H2O2体系光解活性艳橙X-GN模拟废水,考察了X-GN,Fe3 和H2O2的初始浓度、初始pH值及温度对光解的影响,探讨了X-GN的降解途径和机理.结果表明,在8W低压汞灯(λ＝254nm)照射下,UV/Fe3 /H2O2能够有效地降解X-GN,在pH=3.0,T=50 ℃,时间为120 min,Fe3 和H2O2的初始浓度分别为2.5×10-5 mol·l-1和1.5×10-4 mol·l-1时,对含200 mg·l-1 X-GN模拟废水的色度去除率和矿化率分别达到100%和90.15%.用IC和GC/MS对X-GN降解的中间产物和最终产物进行分析,推导出UV/Fe3 /H2O2体系中X-GN降解的途径和机理.     

溶液环境对纳米Fe2O3/水界面NOM吸附过程中疏水效应的影响

以腐殖酸和纳米Fe2O3为对象,着重研究了腐殖酸分子在纳米Fe2O3表面的吸附过程中的疏水效应,借助红外光谱和热重等分析方法研究了腐殖酸吸附前后的疏水性随溶液环境变化的规律。结果表明,当离子强度为0、0.005、0.01和0.05 mol/kg,pH从7变到12时,纳米Fe2O3吸附溶解性腐殖酸分子后形成的复合体的热失重量随着pH的升高先减小后增大。当pH从7升高到10时,亲水性降低,疏水性增强;当pH从10升高到12时,亲水性增强,疏水性降低。当离子强度为0.001 mol/kg,pH从7变到12时,复合体的热失重量随着pH的升高而减小,亲水性降低,疏水性增强。当pH为定值,离子强度变化时,纳米Fe2O3吸附溶解性腐殖酸分子后形成的复合体的热失重量随着离子强度的增加不断变化,曲线呈现出波动趋势,亲、疏水性在交替变化。红外光谱分析结果说明,对纳米Fe2O3吸附溶解性腐殖酸分子后形成的复合体的亲疏水性起主要影响的官能团可能是亲水性的羟基—OH、羰基CO和疏水性的CH2烷烃。     

用H_2O_2/Fe~(3+)处理高浓度含甲醛废水的研究

研究采用H2O2/Fe3+催化氧化处理高浓度含甲醛废水,探讨了双氧水和催化剂投加量、反应pH及反应温度等操作条件对处理效果的影响,并通过酸溶解回用失活催化剂.结果表明,较优的操作条件为:H2O2/COD(质量比)=2.2～2.6,Fe3+/H2O2(摩尔比)=0.048～0.058,反应pH 1.80～2.68,反应温度50℃,反应时间40 min;在上述操作条件下,甲醛去除率达到99%以上,COD去除率达到85%以上.失活的催化剂可通过稀酸溶解后循环使用,其效果与三价铁盐作催化剂的基本相同.采用H2O2/Fe3+处理含甲醛废水具有比采用H2O2/Fe2+较优的效果.     

Ni/Fe/Al2O3·PVDF催化还原剂的表征及制备过程优化

在PVDF基体改性的基础上,采用浸渍法制备出Ni/Fe/Al₂O₃·PVDF催化还原剂。通过对一氯乙酸的脱氯效果研究,对交联液配比及交联时间、不同浓度硫酸镍浸渍时间、镍铁比等因素进行优化,实验优化结果表明,Ni/Fe/Al₂O₃·PVDF催化还原剂对一氯乙酸脱氯60 min脱氯率达到64%。经SEM表征,制备出的双金属在膜载体表面及断面分布均匀,呈球状和片状结构且双金属未发生团聚。     

负载型氧化铁对高毒气体PH3的催化分解

采用沉积-沉淀法制备了碳纳米管(CNTs)和二氧化硅(SiO2)负载的纳米Fe2O3催化剂,将其应用于高毒气体PH3分解反应.通过XRD,TEM,XPS,BET等一系列检测手段,对制备样品的相结构、形貌、组分和比表面积进行了表征.研究结果表明,在PH3催化分解反应过程,极少量的产物P迁移至Fe2O3中,形成金属磷化物FeP作为反应的活性相.与Fe2 O3/SiO2相比,Fe2O3/CNTs显示了较高的催化性能.在440℃反应温度下,Fe2O3/CNTs对PH3分解率达到99.8％.CNTs作为催化剂载体的优秀性能可归因于CNTs良好的导电性能和活性组分在其上的高度分散.     

六铝酸盐催化剂的催化还原脱硫脱硝性能

采用共沉淀法制备Cu和Fe掺杂的六铝酸盐催化剂(SrCuxFe1-xAl11O19-δ,x为0,0.2,0.4,0.5,0.6,0.8,1),通过XRD、TPR、BET等技术方法对催化剂的结构及性质进行了研究,并考察了以CO为还原剂的催化脱硝活性。结果表明,用碳酸铵作为沉淀剂在1 200℃焙烧4 h可以形成完整的六铝酸盐晶型,Cu和Fe能够取代Al3+,很好地促进六铝酸盐晶体结构的形成;SrCuxFe1-xAl11O19-δ催化剂有很好的脱硫脱硝催化活性,此类型的催化剂均使SO2、NO的转化率在空速为6 000 h-1下达到了80%和90%以上。向体系中加入氧气会对催化活性有较大影响。     

Arsenic(III) and iron(II) co-oxidation by oxygen and hydrogen peroxide: Divergent reactions in the presence of organic ligands

Iron-catalyzed oxidation of As(III) to As(V) can be highly effective for toxic arsenic removal via Fenton reaction and Fe(II) oxygenation. However, the contribution of ubiquitous organic ligands is poorly understood, despite its significant role in redox chemistry of arsenic in natural and engineered systems. In this work, selected naturally occurring organic ligands and synthetic ligands in co-oxidation of Fe(II) and As(III) were examined as a function of pH, Fe(II), H₂O₂, and radical scavengers (methanol and 2-propanol) concentration. As(III) was not measurably oxidised in the presence of excess ethylenediaminetetraacetic acid (EDTA) (i.e. Fe(II):EDTA < 1:1), contrasting with the rapid oxidation of Fe(II) by O₂ and H₂O₂ at neutral pH under the same conditions. However, partial oxidation of As(III) was observed at a 2:1 ratio of Fe(II):EDTA. Rapid Fe(II) oxidation in the presence of organic ligands did not necessarily result in the coupled As(III) oxidation. Organic ligands act as both iron speciation regulators and radicals scavengers. Further quenching experiments suggested both hydroxyl radicals and high-valent Fe species contributed to As(III) oxidation. The present findings are significant for the better understanding of aquatic redox chemistry of iron and arsenic in the environment and for optimization of iron-catalyzed arsenic remediation technology.     

Cd~(2+)、Pb~(2+)在湘江流域河床表层沉积物上的吸附特性研究

以湘江流域河床表层沉积物为吸附剂,用于去除水中Cd~(2+)、Pb~(2+),系统研究了沉积物对Cd~(2+)、Pb~(2+)的吸附规律,并探讨了其吸附Cd~(2+)、Pb~(2+)后的化学稳定性。结果表明,当2种离子单独存在时,沉积物对Cd~(2+)、Pb~(2+)均具有较好的吸附效果;当2种离子同时存在时,由于竞争作用,沉积物对Cd~(2+)和Pb~(2+)的吸附量分别减小了约40%和16%。对吸附平衡的溶液进行曝气和用双蒸水清洗吸附饱和的沉积物后,Cd~(2+)、Pb~(2+)的释放比例较小,说明湘江流域河床表层沉积物吸附Cd~(2+)、Pb~(2+)后,其化学稳定性较好。沉积物的SEM、FTIR和XRD分析发现,沉积物结构多孔,表面含有大量—OH、—NH,这些基团在吸附重金属阳离子过程中起重要作用。研究结果表明,湘江流域河床表层沉积物对去除水中的Cd~(2+)、Pb~(2+)有较好的效果,该成果对湘江流域重金属污染控制具有重要参考价值。     

Fe3+、PO43-在煤气化废水处理中的应用

针对煤气化废水的特点,通过投加Fe3 、PO43-的方法来强化多阶段水解-好氧工艺处理煤气化废水的能力,不加Fe3 、PO43-时,CODcr总去除率为78 88%,出水CODcr仍高达931mg/l,当投加Fe3 、PO43-后,出水CODcr降到245mg/l,去除率达到93 93%。