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Biodegradation of vapor-phase toluene in unsaturated porous media: Column experiments
2016
Khan, Ali M. | Wick, Lukas Y. | Harms, Hauke | Thullner, Martin
Biodegradation of organic chemicals in the vapor phase of soils and vertical flow filters has gained attention as promising approach to clean up volatile organic compounds (VOC). The drivers of VOC biodegradation in unsaturated systems however still remain poorly understood. Here, we analyzed the processes controlling aerobic VOC biodegradation in a laboratory setup mimicking the unsaturated zone above a shallow aquifer. The setup allowed for diffusive vapor-phase transport and biodegradation of three VOC: non-deuterated and deuterated toluene as two compounds of highly differing biodegradability but (nearly) identical physical and chemical properties, and MTBE as (at the applied experimental conditions) non-biodegradable tracer and internal control. Our results showed for toluene an effective microbial degradation within centimeter VOC transport distances despite high gas-phase diffusivity. Degradation rates were controlled by the reactivity of the compounds while oxic conditions were found everywhere in the system. This confirms hypotheses that vadose zone biodegradation rates can be extremely high and are able to prevent the outgassing of VOC to the atmosphere within a centimeter range if compound properties and site conditions allow for sufficiently high degradation rates.
Show more [+] Less [-]Effects of microplastics on European flat oysters, Ostrea edulis and their associated benthic communities
2016
Green, Dannielle Senga
Plastic pollution is recognised as an emerging threat to aquatic ecosystems, with microplastics now the most abundant type of marine debris. Health effects caused by microplastics have been demonstrated at the species level, but impacts on ecological communities remain unknown. In this study, impacts of microplastics on the health and biological functioning of European flat oysters (Ostrea edulis) and on the structure of associated macrofaunal assemblages were assessed in an outdoor mesocosm experiment using intact sediment cores. Biodegradable and conventional microplastics were added at low (0.8 μg L−1) and high (80 μg L−1) doses in the water column repeatedly for 60 days. Effects on the oysters were minimal, but benthic assemblage structures differed and species richness and the total number of organisms were ∼1.2 and 1.5 times greater in control mesocosms than in those exposed to high doses of microplastics. Notably, abundances of juvenile Littorina sp. (periwinkles) and Idotea balthica (an isopod) were ∼2 and 8 times greater in controls than in mesocosms with the high dose of either type of microplastic. In addition, the biomass of Scrobicularia plana (peppery furrow shell clam) was ∼1.5 times greater in controls than in mesocosms with the high dose of microplastics. This work indicates that repeated exposure to high concentrations of microplastics could alter assemblages in an important marine habitat by reducing the abundance of benthic fauna.
Show more [+] Less [-]Simultaneous removal of acid green 25 and mercury ions from aqueous solutions using glutamine modified chitosan magnetic composite microspheres
2016
Tao, Xue | Li, Kun | Yan, Han | Yang, Hu | Li, Aimin
In this current work, the magnetic composite microsphere containing glutamine modified chitosan and silica coated Fe3O4 nanoparticles (CS-Gln-MCM) has been successfully prepared and extensively characterized, which is a kind of biodegradable materials. CS-Gln-MCM shows enhanced removal efficiency for both acid green 25 (AG25), an amphoteric dye, and mercury ions (Hg²⁺) from water in the respective while measured pH range compared with chitosan magnetic composite microsphere (CS-MCM) without modification. It is due to the fact that the grafted amino acid provides a variety of additional adsorption active sites and diverse adsorption mechanisms are involved. In AG25 and Hg²⁺ aqueous mixture, the modified adsorbents bear preferential adsorption for AG25 over Hg²⁺ in strong acidic solutions ascribed to multiple interactions between AG25 and CS-Gln-MCM, such as hydrogen bonding and electrostatic interactions. While, in weak acidic conditions, an efficient simultaneous removal is observed for different adsorption effects involved in aforementioned two pollutants. Besides, CS-Gln-MCM illuminates not only short equilibrium time for adsorption of each pollutant less than 20.0 min but also rapid magnetic separation from water and efficient regeneration after saturated adsorption. Therefore, CS-Gln-MCM bears great application potentials in water treatment.
Show more [+] Less [-]Environmental fate and effect assessment of thioridazine and its transformation products formed by photodegradation
2016
Wilde, Marcelo L. | Menz, Jakob | Trautwein, Christoph | Leder, Christoph | Kümmerer, Klaus
An experimental and in silico quantitative structure-activity relationship (QSAR) approach was applied to assess the environmental fate and effects of the antipsychotic drug Thioridazine (THI). The sunlight-driven attenuation of THI was simulated using a Xenon arc lamp. The photodegradation reached the complete primary elimination, whereas 97% of primary elimination and 11% of mineralization was achieved after 256 min of irradiation for the initial concentrations of 500 μg L−1 and 50 mg L−1, respectively. A non-target approach for the identification and monitoring of transformation products (TPs) was adopted. The structure of the TPs was further elucidated using liquid chromatography–high resolution mass spectrometry (LC–HRMS). The proposed photodegradation pathway included sulfoxidation, hydroxylation, dehydroxylation, and S- and N-dealkylation, taking into account direct and indirect photolysis through a self-sensitizing process in the higher concentration studied. The biodegradability of THI and photolytic samples of THI was tested according to OECD 301D and 301F, showing that THI and the mixture of TPs were not readily biodegradable. Furthermore, THI was shown to be highly toxic to environmental bacteria using a modified luminescent bacteria test with Vibrio fischeri. This bacteriotoxic activity of THI was significantly reduced by phototransformation and individual concentration-response analysis confirmed a lowered bacterial toxicity for the sulfoxidation products Thioridazine-2-sulfoxide and Thioridazine-5-sulfoxide. Additionally, the applied QSAR models predicted statistical and rule-based positive alerts of mutagenic activities for carbazole derivative TPs (TP 355 and TP 339) formed through sulfoxide elimination, which would require further confirmatory in vitro validation tests.
Show more [+] Less [-]Sequential biodegradation of complex naphtha hydrocarbons under methanogenic conditions in two different oil sands tailings
2016
Mohamad Shahimin, Mohd Faidz | Siddique, Tariq
Methane emissions in oil sands tailings ponds are sustained by anaerobic biodegradation of unrecovered hydrocarbons. Naphtha (primarily C6–C10; n- iso- and cycloalkanes) is commonly used as a solvent during bitumen extraction process and its residue escapes to tailings ponds during tailings deposition. To investigate biodegradability of hydrocarbons in naphtha, mature fine tailings (MFT) collected from Albian and CNRL tailings ponds were amended with CNRL naphtha at ∼0.2 wt% (∼2000 mg L−1) and incubated under methanogenic conditions for ∼1600 d. Microbial communities in both MFTs started metabolizing naphtha after a lag phase of ∼100 d. Complete biodegradation/biotransformation of all n-alkanes (except partial biodegradation of n-octane in CNRL MFT) followed by major iso-alkanes (2-methylpentane, 3-methylhexane, 2- and 4-methylheptane, iso-nonanes and 2-methylnonane) and a few cycloalkanes (derivatives of cyclopentane and cyclohexane) was observed during the incubation. 16S rRNA gene pyrosequencing showed dominance of Peptococcaceae and Anaerolineaceae in Albian MFT and Anaerolineaceae and Syntrophaceae in CNRL MFT bacterial communities with co-domination of Methanosaetaceae and “Candidatus Methanoregula” in archaeal populations during active biodegradation of hydrocarbons. The findings extend the known range of hydrocarbons susceptible to methanogenic biodegradation in petroleum-impacted anaerobic environments and help refine existing kinetic model to predict greenhouse gas emissions from tailings ponds.
Show more [+] Less [-]Experimental and in silico assessment of fate and effects of the antipsychotic drug quetiapine and its bio- and phototransformation products in aquatic environments
2016
Herrmann, Manuel | Menz, Jakob | Gassmann, Matthias | Olsson, Oliver | Kümmerer, Klaus
The antipsychotic drug quetiapine (QUT) has been frequently detected in sewage treatment plants. However, information on the fate of QUT in aquatic environments and its behavior during UV treatment is limited. In this study, QUT is shown not to be readily biodegradable in the Closed Bottle Test and the Manometric Respirometry Test according to OECD guidelines. The main biotransformation product (BTP) formed in the tests, a carboxylic acid derivative, was identified by means of high-resolution mass spectrometry. This BTP is presumably a human metabolite and showed higher detection rates than QUT in a river sampling campaign conducted in northern Germany. UV elimination kinetics of QUT at different initial concentrations (226.5, 45.3, 11.3, and 2.3 μmol L−1) were faster at lower initial concentrations. All seven phototransformation products (PTPs) could be still identified at initial concentration of 11.3 μmol L−1. The photolytic mixture generated after 128 min of photolysis of QUT was not better biodegradable than QUT. Initial UV treatment of QUT led to the formation of several additional BTPs. Four of them were identified. The bacterial cytotoxicity and genotoxicity before and after phototransformation of QUT in a modified luminescent bacteria test (LBT) and the umu-test (ISO/FDIS 13829) showed cytotoxic effects in the LBT for QUT. Furthermore, PTPs had similar cytotoxic effects on luminescent bacteria. The umu-test did not reveal any genotoxic activity for QUT or PTPs. In conclusion, the release of QUT into sewage treatment plants and aquatic environments could result in the formation of a main BTP. Additional UV treatment of QUT would lead to the formation of additional BTPs. Moreover, treatment did not result in lower toxicity to tested organisms. In conclusion, UV treatment of QUT should be considered critically as a potential treatment for QUT in aquatic systems.
Show more [+] Less [-]Effects of conventional and biodegradable microplastics on a marine ecosystem engineer (Arenicola marina) and sediment nutrient cycling
2016
Green, Dannielle Senga | Boots, Bas | Sigwart, Julia | Jiang, Shan | Rocha, Carlos
Effects of microplastic pollution on benthic organisms and ecosystem services provided by sedimentary habitats are largely unknown. An outdoor mesocosm experiment was done to realistically assess the effects of three different types of microplastic pollution (one biodegradable type; polylactic acid and two conventional types; polyethylene and polyvinylchloride) at increasing concentrations (0.02, 0.2 and 2% of wet sediment weight) on the health and biological activity of lugworms, Arenicola marina (Linnaeus, 1758), and on nitrogen cycling and primary productivity of the sediment they inhabit. After 31 days, A. marina produced less casts in sediments containing microplastics. Metabolic rates of A. marina increased, while microalgal biomass decreased at high concentrations, compared to sediments with low concentrations or without microplastics. Responses were strongest to polyvinylchloride, emphasising that different materials may have differential effects. Each material needs to be carefully evaluated in order to assess their risks as microplastic pollution. Overall, both conventional and biodegradable microplastics in sandy sediments can affect the health and behaviour of lugworms and directly or indirectly reduce primary productivity of these habitats.
Show more [+] Less [-]Degradation of cyclophosphamide and 5-fluorouracil by UV and simulated sunlight treatments: Assessment of the enhancement of the biodegradability and toxicity
2016
Lutterbeck, Carlos Alexandre | Wilde, Marcelo Luís | Baginska, Ewelina | Leder, Christoph | Machado, Ênio Leandro | Kümmerer, Klaus
The presence of pharmaceuticals in the environment has triggered concern among the general population and received considerable attention from the scientific community in recent years. However, only a few publications have focused on anticancer drugs, a class of pharmaceuticals that can exhibit cytotoxic, genotoxic, mutagenic, carcinogenic and teratogenic effects. The present study investigated the photodegradation, biodegradation, bacterial toxicity, mutagenicity and genotoxicity of cyclophosphamide (CP) and 5-fluorouracil (5-FU). The photodegradation experiments were performed at a neutral to slight pH range (7–7.8) using two different lamps (medium-pressure mercury lamp and a xenon lamp). The primary elimination of the parent compounds was monitored by means of liquid chromatography tandem mass spectrometry (LC-IT-MS/MS). NPOC (non-purgeable organic carbon) analyses were carried out in order to assess mineralization rates. The Closed Bottle Test (CBT) was used to assess ready biodegradability. A new method using Vibrio fischeri was adopted to evaluate toxicity. CP was not degraded by any lamp, whereas 5-FU was completely eliminated by irradiation with the mercury lamp but only partially by the Xe lamp. No mineralization was observed for the experiments performed with the Xe lamp, and a NPOC removal of only 18% was registered for 5-FU after 256 min using the UV lamp. Not one of the parent compounds was readily biodegradable in the CBT. Photo transformation products (PTPs) resulting from photolysis were neither better biodegradable nor less toxic than the parent compound 5-FU. In contrast, the results of the tests carried out with the UV lamp indicated that more biodegradable and non-toxic PTPs of 5-FU were generated. Three PTPs were formed during the photodegradation experiments and were identified. The results of the in silico QSAR predictions showed positive mutagenic and genotoxic alerts for 5-FU, whereas only one of the formed PTPs presented positive alerts for the genotoxicity endpoint.
Show more [+] Less [-]Biocompatible poly(vinyl alcohol) nanoparticle-based binary blends for oil spill control
2016
Fouad, Rasha Refaat | Aljohani, Hind Abdullah | Shoueir, Kamel Rizq
In the current study, biocompatible and biodegradable blends based on poly(vinyl alcohol) nanoparticles – PVAn mixed with either chitosan (Ch) or starch (St) – were prepared and investigated as nanoabsorbents for oil elimination from wastewater. The use of water/dimethyl sulfoxide (DMSO) as a mixed solvent is the key factor for preparing aggregated PVAn, which is further mixed with Ch or St. Nanoblends were applied as oil absorbents, and the results showed that PVAn/St possess high adsorption capacity than PVAn/Ch and PVAn. The maximum sorption capacities (qg/g) of the PVAn/Ch sorbents for hydraulic oil, kerosene, and toluene were 33.6, 73.96, and 93.1g/g, respectively. The absorbed oil could be rapidly recovered by simple mechanical squeezing and reused without any other modification. The blends showed excellent reusability and could be reused for at least 10 times with minimal losses. The current study demonstrates the application of these blends as an ideal alternative sorbent for oil spillage cleanup.
Show more [+] Less [-]Microbial colonization and degradation of polyethylene and biodegradable plastic bags in temperate fine-grained organic-rich marine sediments
2016
Nauendorf, Alice | Krause, Stephan | Bigalke, Nikolaus K. | Gorb, Elena V. | Gorb, Stanislav | Haeckel, Matthias | Wahl, Martin | Treude, Tina
To date, the longevity of plastic litter at the sea floor is poorly constrained. The present study compares colonization and biodegradation of plastic bags by aerobic and anaerobic benthic microbes in temperate fine-grained organic-rich marine sediments. Samples of polyethylene and biodegradable plastic carrier bags were incubated in natural oxic and anoxic sediments from Eckernförde Bay (Western Baltic Sea) for 98days. Analyses included (1) microbial colonization rates on the bags, (2) examination of the surface structure, wettability, and chemistry, and (3) mass loss of the samples during incubation. On average, biodegradable plastic bags were colonized five times higher by aerobic and eight times higher by anaerobic microbes than polyethylene bags. Both types of bags showed no sign of biodegradation during this study. Therefore, marine sediment in temperate coastal zones may represent a long-term sink for plastic litter and also supposedly compostable material.
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