Fe-Ce/ZSM-5复合催化剂的制备及其催化性能

采用浸渍法制备了Fe-Ce/ZSM-5复合催化剂,并将其用于甲基橙的催化降解。利用单因素实验考察了溶液pH、初始甲基橙质量浓度、催化剂加入量、初始H_2O_2浓度及反应温度对准一级动力学方程反应动力学常数的影响,对催化剂的稳定性进行了测试,并探讨了甲基橙的催化降解机理。实验结果表明:在溶液pH 5.0、初始甲基橙质量浓度100 mg/L、催化剂加入量1.0 g/L、初始H_2O_2浓度20 mmol/L、反应温度20℃的优化条件下反应60min,反应动力学常数高达0.034 min~(-1),甲基橙降解率高达87%,铁离子流失量仅为0.019 mg/L;催化剂重复使用3次后,甲基橙降解率仍高于80%,保持了较高活性。     

H_4SiW_(12)O_(40)/TiO_2/空心微珠光催化降解联苯胺

采用复合型光催化剂H_4SiW_(12)O_(40)/TiO_2/空心微珠(cenospheres)光催化降解联苯胺,考察了联苯胺降解效果的影响因素,并运用FTIR和GS-MS技术分析了联苯胺光催化降解过程的主要中间产物,探讨了联苯胺可能的降解路径。实验结果表明:以125 W中压汞灯为光源,在溶液pH为6.3,初始联苯胺质量浓度为10 mg/L的条件下光反应240 min,联苯胺降解率达78%,比Ti_O2/空心微珠提高了24百分点;H_4SiW_(12)O_(40)/TiO_2/空心微珠光催化降解联苯胺符合表观一级动力学特征,且反应速率常数随初始联苯胺质量浓度的增加而减小;H_4SiW_(12)O_(40)/TiO_2/空心微珠具有较好的稳定性,易于分离,可重复利用;联苯胺光催化降解过程的主要中间产物为4-氨基联苯、4-氨基苯酚、对苯二酚和1,4-苯醌。     

回流指数在空气质量变化研究中的应用

将回流指数引入珠三角污染气象条件的研究中,尝试使用回流指数判别形成区域大气污染的机理.运用中尺度数值模式WRF得到珠三角精细化的回流指数时空分布,同时与边界层外场观测试验结果进行比对从而验证模式对边界层内风场的模拟效果.最后,分别对干湿季冷高压影响下的污染过程进行分析,湿季选取2013年4月13—16日的珠三角重污染过程,干季选取同年12月8—10日的污染过程.结果表明:在本研究的两次过程中,使用回流指数Rcritical=0.6作为阈值能较好地区分局地污染物回流堆积与上风向污染物输送两种因素在冷高压型污染过程中何者占主导,当区域中回流指数普遍低于0.6则是污染物局地回流堆积作用更明显,若普遍高于0.6则是受上风向污染物的输送影响更明显;在局地回流堆积为主要形成机理的污染过程中,地面污染物浓度与边界层整体回流系数呈反方向变化关系,地面污染物浓度峰值对应边界层回流系数谷值;在污染物输送为主要形成因素的污染过程中,边界层中低层回流系数达到峰值时代表该区域此时受上风向风场输送作用最显著,地面污染物浓度同时达到峰值.     

植物法改性类Fenton反应催化剂降解甲基橙

采用银杏叶和桑叶提取液制备了改性类Fenton反应催化剂并进行了表征分析,研究了溶液初始p H、反应温度、催化剂加入量、甲基橙初始质量浓度等因素对甲基橙降解率的影响,同时考察了催化剂的重复使用效果。表征结果表明:制备出的催化剂为Fe_2O_3和Fe OOH的混合物;桑叶改性催化剂的粒径分布较银杏叶改性催化剂均匀,粒径较小,比表面积较大。实验结果表明:在初始p H为6.23、反应温度60℃、催化剂用量1 g/L、甲基橙初始质量浓度100 mg/L的条件下,银杏叶改性催化剂的甲基橙降解率为99.40%,桑叶改性催化剂的甲基橙降解率为99.96%;碱性条件下,甲基橙降解率仍接近100%,扩宽了反应的p H适用范围,为碱性条件下处理偶氮染料提供了新思路;催化剂重复使用6次之后,甲基橙降解率仍可达到99%。根据反应前后溶液的紫外-可见吸收光谱,初步探讨了降解机理。     

WO_3/Ag_3VO_4复合光催化剂的制备及其可见光催化性能

采用超声辅助沉淀法—浸渍法制备了WO3/Ag3VO4复合光催化剂,对其进行了表征,考察了其在可见光条件下对罗丹明B的催化降解性能,并对催化机理进行了探讨。表征结果显示:WO3紧密包覆在Ag3VO4颗粒的表面,并未改变Ag3VO4的晶体结构;与Ag3VO4和WO3相比,WO3/Ag3VO4的吸收带边发生了红移。实验结果表明:w(WO3)为3.5%时,WO3/Ag3VO4对罗丹明B的可见光催化降解效果最好;在光催化剂加入量0.8 g/L、初始罗丹明B质量浓度10 mg/L的条件下,于室温下光照180 min时的罗丹明B去除率达95.76%,TOC去除率达96.5%;WO3与Ag3VO4在能带间的耦合作用下形成异质结结构,很好地抑制了光生电子-空穴对的复合。     

新型类Fenton催化剂表征及其降解染料废水的试验研究

钴基和铜基类Fenton催化剂是近年来的研究热点,对新型类Fenton催化剂进行SEM,EDS,XPS表征,得知催化剂中的金属元素主要为钴和铜。通过单因素分析法,研究影响该催化剂处理甲基橙模拟废水效果的因素。结果表明:该催化剂在pH为3~9的范围内均表现出较好的催化降解能力;当双氧水的添加量达到20 mL/L时,催化降解能力不再增加;催化剂的投加量影响催化降解能力达到最大的时间;此外,双氧水的投加方式影响降解所需的时间而对最终的处理效果影响不大。     

无机沉淀对土壤有机质吸附疏水有机污染物的影响

土壤有机质对疏水性有机污染物的吸附解吸是影响其在土壤中迁移、转化和归趋的重要因素之一。老化是有机污染物和土壤等介质长时间相互作用的结果,它影响着污染物的生物有效性。已有的老化研究注重有机污染物被土壤等介质吸附隔离的机制,很少考虑土壤等吸附剂自身演化对有机污染物吸附的影响。本文通过无机沉淀处理方法来模拟自然环境过程吸附剂自身的演化对土壤有机质吸附能力的影响,从而证明吸附剂自身的变化也是影响老化效应的一个重要因素。结果表明,不同无机沉淀包裹和填充的碱提土样品比原始碱提土样品具有更小的吸附能力,同时无机沉淀处理后的样品的吸附性能随着无机沉淀离子浓度增加而降低。这可能是无机沉淀覆盖碱提土样品的内外表面积和填充碱提土样品的微孔所引起的,同时也可能是无机沉淀占据了吸附有机污染物的高能点位所致。     

中国东中西部经济带的水环境库兹涅茨假说实证及其影响因素研究

“八五”至“十二五”期间,中国取得巨大的经济成果的同时带来了严重的水环境污染问题.文章分析了东中西部三大经济带经济发展及COD和氨氮两种主要水污染排放的差异,及其与经济发展的关系进行了EKC假说的实证研究.研究结果表明,部分污染物的拟合曲线尚处于上升阶段,未能出现典型的倒U型曲线,可能导致水环境质量恶化.环境基础设施建设、人口分布和产业结构等因素与COD和氨氮的排放量密切相关,因此,中国必须采取各种环境管理和技术手段,促使区域水污染物排放量指标与经济发展的拟合曲线出现转折点,改善水环境质量.     

Topical application of synthetic pyrethroids to cattle as a source of persistent environmental contamination

Abstract

Following the application of permethrin or cyhalothrin to cattle for the control of ectoparasites, the occurrence and persistence of these chemicals was assessed on the animals and in their environment. The release of permethrin from ear tags containing 1g of the drug on cattle was followed for 65 days and lead to concentrations of 5 to 35 μg of permethrin per gram of hair on the shoulders. On the flanks of the animals, the corresponding values were 10 times lower. Across the 1.5 acre pasture, high concentrations of permethiin were measured at various locations and long after treatment: 6 μg/g on bark of a birch after one week, 5 μg/g on a pole of the fence after two weeks, 1 μg/g in grass from a resting site of the animal after six weeks, and 0.5 μg/g in bark of a pine tree after three month and two weeks after the animals had left the pasture. In similar assays, cyhalothrin applied to milk cows as a pour‐on preparation was monitored. One week following treatment with 0.2 g/animal, hair cut from the shoulders contained 5 μg/g of the insecticide, which disappeared with a half‐life of 12 days. Dust collected two weeks after the pour‐on treatment from the milk barn where the cows were milked twice daily contained 47 μg/g of cyhalothrin, which disappeared with a half‐life of 44 days. These results show that synthetic pyrethroids used on farm animals can be the source of widespread and persistent contamination.     

Repeated batch and continuous degradation of chlorpyrifos by Pseudomonas putida

The present study was undertaken with the objective of studying repeated batch and continuous degradation of chlorpyrifos (O,O-diethyl O-3,5,6-trichloropyridin-2-yl phosphorothioate) using Ca-alginate immobilized cells of Pseudomonas putida isolated from an agricultural soil, and to study the genes and enzymes involved in degradation. The study was carried out to reduce the toxicity of chlorpyrifos by degrading it to less toxic metabolites. Long-term stability of pesticide degradation was studied during repeated batch degradation of chlorpyrifos, which was carried out over a period of 50 days. Immobilized cells were able to show 65% degradation of chlorpyrifos at the end of the 50th cycle with a cell leakage of 112 × 10³ cfu mL^?1. During continuous treatment, 100% degradation was observed at 100 mL h^?1 flow rate with 2% chlorpyrifos, and with 10% concentration of chlorpyrifos 98% and 80% degradation was recorded at 20 mL h^?1 and 100 mL h^?1 flow rate respectively. The products of degradation detected by liquid chromatography–mass spectrometry analysis were 3,5,6-trichloro-2-pyridinol and chlorpyrifos oxon. Plasmid curing experiments with ethidium bromide indicated that genes responsible for the degradation of chlorpyrifos are present on the chromosome and not on the plasmid. The results of Polymerase chain reaction indicate that a ~890-bp product expected for mpd gene was present in Ps. putida. Enzymatic degradation studies indicated that the enzymes involved in the degradation of chlorpyrifos are membrane-bound. The study indicates that immobilized cells of Ps. putida have the potential to be used in bioremediation of water contaminated with chlorpyrifos.