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1.On-line Monitoring System of P5CDF Homologues in Waste Incineration Plants Using VUV-SPI-IT-TOFMS 2.Tobacco Waste/Industrial Sludge Based Desulfurization Adsorbents: Effect of Phase Interactions during Pyrolysis on Surface Activity 3.Determining Residence Patterns of Rainbow Trout Using Laser Ablation Inductively Coupled Plasma Mass Spectrometry (LA-ICP-MS) Analysis of Selenium in Otoliths 4.Kinetic Modeling of the Oxidation of p-Hydroxybenzoic Acid by Fenton's Reagent: Implications of the Role of Quinones in the Redox Cycling of Iron 5.Occurrence of Natural and Synthetic Glucocorticoids in Sewage Treatment Plants and Receiving River Waters 6.Low Concentrations of Surfactants Enhance Siderophore-Promoted Dissolution of Goethite 7.Rangeland Grazing as a Source of Steroid Hormones to Surface Waters On-line Monitoring System of P5CDF Homologues in Waste Incineration Plants Using VUV-SPI-IT-TOFMS Shigenori Tsuruga,* Takumi Suzuki, Yasuhiro Takatsudo, Katsuo Seki, Sumio Yamauchi, Shizuma Kuribayashi, and Shigeki Morii# Yokohama Research & Development Center, Mitsubishi Heavy Industries, Ltd., 1-8-1 Sachiura, Kanazawa-ku, Yokohama, 236-8515, Japan, Takasago Research & Development Center, Mitsubishi Heavy industries, Ltd., 2-1-1 Arai-cho shinhama, Takasago, Hyogo Prefecture 676-8686, Japan, Advanced Technology Research Center, Mitsubishi Heavy Industries, Ltd., 1-8-1 Sachiura, Kanazawa-ku, Yokohama, 236-8515, Japan, and MHI Solution Technologies Co., Ltd., 5-1 Eba-oki-machi, Naka-ku, Hiroshima 730-0837, Japan Received for review June 22, 2006 Revised manuscript received March 12, 2007 Accepted March 12, 2007 Abstract: It usually takes a few weeks to analyze dioxin concentrations and dioxin-TEQ (toxicity equivalency quantity) in fluegases from municipal solid waste (MSW) incinerators by a standard method provided by Japanese industrial standard (JIS 0311). To reduce the required time for analysis, we have developed a new on-line measuring system for furans homologues. This system is composed of a sensitive and robust vacuum ultraviolet (VUV) single-photon ionization (SPI) ion trap (IT) time-of-flight mass spectrometer (VUV-SPI-IT-TOFMS) and automatic sampling/concentrating process. In this work, pentachloro-dibenzofuran (P5CDF) was selected as an index homologue in chlorinated dibenzo-p-dioxin/furan homologues (DXNs) because its concentration and I-TEF (international toxicity equivalency factor), which are 2,3,4,7,8-P5CDF is 0.5 and 1,2,3,7,8-P5CDF is 0.05, are high and the concentration correlates closely with the total amount of dioxin-TEQ. The lowest detectable limit, 1 pg (0.001 ng-TEQ/m3 N) was demonstrated by laboratory tests. This system underwent a field test at several actual MSW plants and the tests revealed the following: (a) This system is applicable for dioxin-TEQ evaluation from actual MSW incinerators. (b) It can continuously monitor P5CDF in a fluegas for 7 months. (c) The frequency of the measurements is once every 2-6 h, depending on the concentration of P5CDF. -------------------------------------------------------------------------------- Tobacco Waste/Industrial Sludge Based Desulfurization Adsorbents: Effect of Phase Interactions during Pyrolysis on Surface Activity Mykola Seredych and Teresa J. Bandosz* Department of Chemistry, The City College of New York, City University of New York, 138th Street and Convent Avenue, New York, New York 10031 Received for review October 13, 2006 Revised manuscript received January 13, 2007 Accepted March 8, 2007 Abstract: Industrial waste derived adsorbents were obtained by pyrolysis of tobacco waste with either metal sludge or waste oil sludge from a shipyard. The materials were used as media to remove hydrogen sulfide at room temperature in the presence of moisture. The initial and exhausted adsorbents after the breakthrough tests were characterized using sorption of nitrogen, thermal analysis, XRD, elemental analysis, and surface pH measurements. It was found that mixing tobacco and industrial sludges results in a strong synergy, enhancing the catalytic properties of adsorbents. This synergy is observed in both surface chemistry and porosity. During pyrolysis, new mineral phases are formed as a result of solid-state reactions between the components of the sludges. They are highly dispersed on the surface of mesopores. A high volume of these pores is a result of activation of the carbon phase in the composite by alkaline earth metals and also by the release of water from the decomposition of an inorganic phase that is in the predominant quantity. A high temperature of pyrolysis is beneficial for the adsorbents due to the enhanced activation of the carbonaceous phase and the chemical stabilization of the inorganic phase. Samples obtained at low temperatures are sensitive to water, which deactivates their catalytic centers. -------------------------------------------------------------------------------- Determining Residence Patterns of Rainbow Trout Using Laser Ablation Inductively Coupled Plasma Mass Spectrometry (LA-ICP-MS) Analysis of Selenium in Otoliths Vincent P. Palace,* Norman M. Halden, Panseok Yang, Robert E. Evans, and George Sterling Department of Fisheries and Oceans, Freshwater Institute, Winnipeg MB, Canada R3T 2N6, Department of Geological Sciences, University of Manitoba, Winnipeg MB, Canada R3T 2N6, and Fish and Wildlife Division, Alberta Sustainable Resource Development, Edson AB Received for review November 27, 2006 Revised manuscript received March 8, 2007 Accepted March 13, 2007 Abstract: Toxicological studies are often hampered by concerns of fish residency in the industrial effluent being evaluated. Contaminants in muscle or visceral tissue are useful indicators of recent exposure, but depuration, metabolic transformation, and tissue recompartmentalization of contaminants makes their use as temporal markers tenuous. Otoliths are metabolically stable and can provide temporal resolution for exposure to some elements that are incorporated into their calcified structure, including the divalent cations Sr, Zn, and Mn. Here we provide the first determinations of selenium, an anion in biological systems, in the otoliths of rainbow trout captured from a site receiving runoff with elevated selenium from a coal mine operation. Concentrations of selenium in annual growth zones of otoliths suggest that fish from the mine-impacted system are recent immigrants from nearby reference streams not receiving selenium-bearing effluent. -------------------------------------------------------------------------------- Kinetic Modeling of the Oxidation of p-Hydroxybenzoic Acid by Fenton's Reagent: Implications of the Role of Quinones in the Redox Cycling of Iron Christopher K. Duesterberg and T. David Waite* School of Civil and Environmental Engineering, The University of New South Wales, Sydney, NSW 2052, Australia Received for review December 4, 2006 Revised manuscript received March 1, 2007 Accepted March 15, 2007 Abstract: As Fenton (and Fenton-like) chemistry is increasingly implicated in a variety of areas and applications, an understanding of the mechanism and rates governing the system becomes relevant for a growing number of disciplines and purposes. In this work a kinetic model capable of describing species concentrations measured experimentally during the Fenton-mediated oxidation of p-hydroxybenzoic acid (pHBA) is presented and discussed. Experiments were conducted in the dark at low pH using reagent and substrate concentrations ranging from 100 M to 2 mM. Analysis of the experimental and modeling results reveals that redox reactions between Fe and quinone or quinone-like compounds are essential for the model to qualitatively predict species concentration profiles observed in the laboratory. The quinone and quinone-like compounds generated as byproducts during the oxidation of pHBA act as reducing agents toward Fe(III), thereby assisting the redox cycling of Fe and increasing degradation of the target substrate. The experimental and kinetic modeling results presented highlight the role quinones play in the catalytic redox cycling of iron and the overall effect on the oxidative treatment performance of the system. -------------------------------------------------------------------------------- Occurrence of Natural and Synthetic Glucocorticoids in Sewage Treatment Plants and Receiving River Waters Hong Chang, Jianying Hu,* and Bing Shao College of Environmental Science, Peking University, Beijing, 100871 China, and Institute of Nutrition and Food Hygiene, Beijing Center for Disease Prevention and Control, Beijing, 100013 China Received for review November 17, 2006 Revised manuscript received March 8, 2007 Accepted March 19, 2007 Abstract: This paper first reports the occurrence of six glucocorticoids (prednisone, prednisolone, cortisone, cortisol, dexamethasone, and 6-methylprednisolone) in sewage treatment plants (STPs) and receiving rivers by establishing a method for analyzing glucocorticoids in complex environmental waters. For the various types of aqueous matrices considered, the absolute recoveries were from 73 to 99%, and limits of quantification were below 0.2 ng/L. Among the seven STPs studied, the average concentrations of prednisone, prednisolone, cortisone, cortisol, dexamethasone, and 6-methylprednisolone in influents were, respectively, 2.6 ± 2.1, 3.0 ± 1.6, 30 ± 21, 39 ± 26, 1.2 ± 0.70, and 0.62 ± 0.65 ng/L, and their percent removals were 99 ± 3.1, 78 ± 8.8, 99 ± 1.2, 98 ± 2.5, 99 ± 1.8, and 100 ± 0%, respectively. The lower removal of prednisolone was found to be due to its relatively low efficiency of biodegradation, especially in anoxic and aerobic units. The frequently detected glucocorticoids in effluents were prednisolone, cortisol, and cortisone with average concentrations 0.56 ± 0.06, 0.50 ± 0.33, and 0.26 ± 0.10 ng/L. In the receiving waters, the Tonghui and Qing Rivers, the concentrations of these compounds in some samples were much higher than those in their corresponding STP effluents; these differences depended on the sampling date, suggesting that there was random discharging of untreated wastewaters into these rivers. In addition, the ratio between the combined concentrations of two natural glucocorticoids (cortisol and cortisone) and the concentration of one synthetic glucocorticoid, prednisolone, was found to be a potential index to reflect the wastewater discharging. -------------------------------------------------------------------------------- Low Concentrations of Surfactants Enhance Siderophore-Promoted Dissolution of Goethite Naraya Carrasco, Ruben Kretzschmar,* Marie-Laure Pesch, and Stephan M. Kraemer Institute of Biogeochemistry and Pollutant Dynamics, Department of Environmental Sciences, ETH Zurich, CHN, CH-8092 Zurich, Switzerland, and Department of Environmental Geosciences, University of Vienna, Althanstrasse 14, A-1090 Vienna, Austria Received for review December 6, 2006 Revised manuscript received March 6, 2007 Accepted March 8, 2007 Abstract: Surface-active agents (surfactants) are released by many soil bacteria and plant roots and are also important as environmental contaminants. Their presence at interfaces could influence important biogeochemical processes in soils such as ligand-controlled dissolution, an important process in biological iron acquisition. To investigate their potential influence on ligand-controlled dissolution of iron oxides, we studied the dissolution kinetics of goethite (-FeOOH) at pH 6 in the presence of the bacterial siderophore desferrioxamine B (DFOB) and the anionic surfactant sodium dodecyl sulfate (SDS). The adsorption isotherm of SDS on goethite showed an increase in the slope at concentrations ranging between 300 and 400 M SDS in solution. This increase in slope suggested the onset of admicelle formation. Adsorption of DFOB onto goethite increased strongly with increasing concentrations of adsorbed SDS. Small concentrations of SDS (5 M) resulted in a 3-fold acceleration of DFOB-controlled goethite dissolution in the presence of 80 M DFOB, compared to the suspensions without SDS. The effects of SDS on the goethite dissolution rates were less pronounced at higher SDS concentrations, and became negligible above 600 M total SDS. The dissolution rates of goethite were not proportional to the adsorbed DFOB concentrations, as would be expected for ligand-controlled dissolution. We speculate that increasing concentrations of adsorbed SDS result in a change in DFOB surface speciation from inner-sphere to outer-sphere complexes and, consequently, the ligand-controlled dissolution rates are not linearly related to the adsorbed DFOB concentration. Our results provide the first evidence for an important role of biosurfactants in biological iron acquisition involving siderophores. -------------------------------------------------------------------------------- Rangeland Grazing as a Source of Steroid Hormones to Surface Waters Edward P. Kolodziej and David L. Sedlak* Department of Civil and Environmental Engineering, 657 Davis Hall, University of California, Berkeley, California 94720 Received for review December 21, 2006 Revised manuscript received March 6, 2007 Accepted March 13, 2007 Abstract: Cattle and other livestock excrete endogenous steroid hormones, including estrogens, androgens, and progestins; therefore, allowing grazing livestock direct access to surface waters can result in the release of steroids in agricultural watersheds. Elevated concentrations of steroids are problematic because low concentrations of certain steroids can affect fish reproduction. To assess the occurrence and transport of steroids arising from grazing cattle, gas chromatography-tandem mass spectrometry (GC/MS/MS) was used to quantify a suite of estrogens, androgens, and progestins in small creeks impacted by rangeland grazing. Steroids were detected in 86% of samples from rangeland creeks where cattle had direct access to the water, with concentrations as high as 44 ng/L observed shortly after rain events at the beginning of the winter wet season. Estrogens were present at concentrations above the predicted no-effect concentrations for fish in 10-20% of the samples, and androstenedione was detected at concentrations higher than response thresholds for pheromonal communication in fish. The results suggest that, in certain cases, measures such as stream fencing in rangeland areas to limit direct discharge of animal wastes to surface waters or better manure management practices might be merited to protect ecosystem health. [ Last edited by danmong on 2007-4-16 at 12:58 ] |
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