含氯苯废水的超声降解研究

以氯苯模拟废水为考察对象,研究其浓度、pH、超声时间等因素对氯苯超声降解效率的影响。实验结果表明：超声反应时间小于5min,氯苯降解率很低;5－20min,氯苯降解率成线性增大;超过20min后,氯苯降解率增大缓慢。pH值的增大,氯苯降解率略有减小。水浴温度提高,氯苯降解率增大。反应时间小于15min,初始浓度低的溶液,降解率增加较快,反应时间大于15min,初始浓度高的溶液,降解率增加较快。     

Photochemistry of 1-nitro-2-phenylnaphthalene available to the environment

Photolysis (254 nm, 72h) of 1-nitro-2-phenylnaphthalene $\text{1}$ in methanol gave 2-phenyl-1,4-naphthoquinone-4-monoxime $\text{2}$, 2,2′-diphenyl-4,4′-binaphth-1,1′-diol $\text{3}$ and 2,2′-diphenyl-4,4′-binaphth-1,1′-dione $\text{4}$. Straightforward reactions available to the environment account for the formation of the products: (a) isomerisation of the nitro compound into a nitrite ester followed by either (a) migration of the nitroso group and isomerisation into the oxime $\text{2}$ or (b) oxidative coupling and solvolysis into the binaphthol $\text{3}$ and followed by oxidation into the binaphthone $\text{4}$.     

Photochemistry and environment IV- Photochemical behaviour of monochlorophenols in dilute aqueous solution

The photochemical behaviour of chlorophenols is different to that of non-halogenated phenols. In the former, the first step is a C-Cl bond scission, which is not influenced by oxygen. Chlorine is converted into hydrochloric acid. For monochlorophenols, the position of the chlorine on the ring strongly influences the transformation. In the molecular form, 2-chlorophenol is converted into pyrocatechol. In the anionic form however, it is reduced in a cyclopentadienic acid which dimerizes according to a Diels-Alder reaction. The irradiation of 3-chlorophenol leads to resorcinol whatever the pH. This would appear to suggest a photohydrolysis mechanism. With 4-chlorophenol, the photochemical conversion is not so specific. Hydroquinone is formed (mainly in aerated solution), along with polyphenolic oligomers. A radical mechanism is proposed.     

Studies on degradation of 14C-DDT in the marine environment.

Degradation of 14C-DDT was studied in a marine ecosystem for 60 days and in marine sediments under moist and flooded conditions using a continuous flow system for a period of 130 days. 14C-DDT residues were recovered in sediments of the marine ecosystem at uniform level of 60-65% of the applied 14C-activity throughout the incubation period. DDD was a major metabolite in sediments while DDMU was a major metabolite in clams. Clams brought about substantial degradation of DDT. However, 14C-residues recovered form clams are not suggestive of significant bioaccumulation. In the continuous flow experiment, under both moist and flooded conditions, DDT underwent degradation and about 22% of the applied 14C-activity was recovered as volatiles under both conditions. In sediments, extractable 14C-residues accounted for about 30 and 19% under moist and flooded conditions, respectively. DDT was the major compound in extractable residues as identified by TLC-autoradiographic procedures. More bound residues were formed under flooded than under moist conditions.     

Studies on degradation of 14C-chlorpyrifos in the marine environment.

Degradation of 14C-chlorpyrifos was studied in a marine ecosystem for 60 days and in marine sediment under moist and flooded conditions using a continuous flow system allowing a total 14C-mass balance for a period of 40 days. In the marine ecosystem, 14C-chlorpyrifos underwent rapid degradation and very little (1-2%) 14C-residues of the applied activity were detected after two months in sediments. Clams were major component of the ecosystem and played a significant role in degradation of the insecticide. In the continuous flow system chlorpyrifos did not undergo substantial mineralization. Volatilization accounted for 0.8-1% loss during first ten days of application. The amounts of extractable 14C-activity were higher in flooded sediments than in moist sediment. More bound residues were formed under moist conditions. TCP (3,5,6-trichloro-2-pyridinol) was the major degradation product formed under both moist and flooded conditions, its formation being higher in the latter conditions. These studies underline the role of clams in degradation of chlorpyrifos and lack of microbial degradation. In absence of clams, chlorpyrifos underwent abiotic degradation in marine sediment with formation of bound residues.     

Studies on photochemistry of aromatic hydrocarbons V: Photochemical reaction of chlorobenzene with nitrogen oxides in air

The investigations on the photochemical reaction of chlorobenzene with nitrogen oxides in air were carried out using the reaction vessels made of Pyrex glass and quartz, respectively. The irradiation of chlorobenzene in the Pyrex glass vessel gave m-chloronitrobenzene, 2-chloro-6-nitrophenol, 2-chloro-4-nitrophenol and 4-chloro-2-nitrophenol, while the irradiation of chlorobenzene in the quartz vessel resulted in m-chloronitrobenzene, p-nitrophenol, 2-chloro-4-nitrophenol, 3-chloro-2-nitrophenol, 3-chloro-6-nitrophenol and 3-chloro-4-nitrophenol.The formation mechanism of these chloronitrophenols was considered using the theory of the nitro-nitrite rearrangement of chloronitrobenzenes.     

紫外光降解气态氯苯的影响因素及其动力学研究

紫外光降解挥发性有机物(VOCs)是一种新型的废气处理技术.采用主波长为365 nm的500 W高压汞灯为光源,重点考察了空塔停留时间、氯苯初始浓度、反应介质等对氯苯光降解效果的影响.结果表明,在氯苯初始浓度较低时.氯苯去除率随着空塔停留时间的延长而呈线性升高.最大去除率达87%;而氯苯初始浓度过高时会使单位分子接受的光子和活性基团数量下降,引起氯苯去除率降低,空气介质中的O2和H2O在光照下可转化为活性基团.进而增强了光降解效果;而在氮气介质下光降解氯苯的效率大大降低,最大去除率仅为61%.在氯苯为0.36～8.64 mg/L时,紫外光降解氯苯遵循二级反应动力学方程.     

Speciation and persistence of doxycycline in the aquatic environment: Characterization in terms of steady state kinetics

The aim of the present work was to establish the kinetics for the degradation of doxycycline in the aquatic environment with a view to arriving at a kinetic model that can be used to predict the persistence of antibiotic with confidence. The degradation of doxycycline in both water and sediment phases of aquatic microcosm experiments, as well as in distilled water control experiments, was studied over a period of 90 days. An initial 21% loss due to adsorption by the sediment was observed in the microcosm experiment soon after charging. Biphasic zero-order linear rates of degradation, attributed to microbial degradation of the free and sediment or colloidal particle-adsorbed antibiotic, were observed for both water phase (2.3 × 10^?2 and 4.5 × 10^?3 μgg^?1 day^?1) and sediment phase (7.9 × 10^?3 and 1.5 × 10^?3 μgg^?1 day^?1) of the microcosm experiment. The covered distilled water control experiment exhibited a monophasic zero-order linear rate (1.9 × 10^?3 μgg^?1 day^?1) attributed to hydrolysis, while the distilled water experiment exposed to natural light exhibited biphasic liner rates attributed to a combination of hydrolysis and photolysis (2.9 × 10^?3 μgg^?1 day^?1) and to microbial degradation (9.8 × 10^?3 μgg^?1 day^?1). A kinetic model that takes into account hydrolysis, photolysis, microbial degradation as well as sorption/desorption by colloidal and sediment particles is presented to account for the observed zero-order kinetics. The implications of the observed kinetics on the persistence of doxycycline in the aquatic environment are discussed.     

An experimental and numerical study of the thermal oxidation of chlorobenzene

A combustion-driven flow reactor was used to examine the formation of chlorinated and non-chlorinated species from the thermal oxidation of chlorobenzene under post-flame conditions. Temperature varied from 725 to 1000 K, while the equivalence ratio was held constant at 0.5. Significant quantities of chlorinated intermediates, vinyl chloride and chlorophenol, were measured. A dominant C-Cl scission destruction pathway seen in pyrolytic studies was not observed. Instead, hydrogen-abstraction reactions prevailed, leading to high concentrations of chlorinated byproducts. The thermal oxidation of benzene was also investigated for comparison. Chemical kinetic modeling of benzene and chlorobenzene was used to explore reaction pathways. Two chlorobenzene models were developed to test the hypothesis that chlorobenzene oxidation follows a CO-expulsion breakdown pathway similar to that of benzene. For the temperatures and equivalence ratio studied, hydrogen abstraction by hydroxyl radicals dominates the initial destruction of both benzene and chlorobenzene. Chlorinated byproducts (i.e., chlorophenol and vinyl chloride) were formed from chlorobenzene oxidation in similar quantities and at similar temperatures to their respective analogue formed during benzene oxidation (i.e., phenol and ethylene).     

Conservation state of two paintings in the Santa Margherita cliff cave: role of the environment and of the microbial community

Environmental Science and Pollution Research - The conservation of ancient paintings sited in humid environments is an actual challenge for restorers, because it needs the knowledge of the...     

Studies of the oxidative photoinduced degradation of silicones in the aquatic environment

During irradiation of aqueous solutions of a mixture of oligomeric dimethylsiloxanes with artificial sunlight in the presence of nitrate ions, a reduction in the concentration of the siloxanes was demonstrated. This was verified by atomic absorption spectroscopy and proton nuclear magnetic resonance spectroscopy.In two separate tests, average halflives of 9 and 4 days, respectively, were determined after extraction of the aqueous solutions and analysis by atomic absorption spectroscopy.Silicate was demonstrated to be the final photodegradation product of these water soluble siloxanes. Photometric determination of silicate after 35 days showed nearly complete transformation, based on the original quantity of siloxanes.When an aqueous emulsion of high molecular-weight poly(dimethylsiloxane) was irradiated in the presence of nitrate ions under similar experimental conditions, a level of silicate corresponding to 1.7% of the original quantity of poly(dimethylsiloxane) was found after 5 weeks.     

Relative rates and partial combustion products from the burning of chlorobenzenes and chlorobenzene mixtures

Relative rates of burning were determined and partial combustion products identified for several chlorobenzenes and benzene-chlorobenzene and chlorobenzene-chlorobenzene mixtures. The results show that both the rate and product distribution depend on the feed stream atomic ratios and are insensitive to the specific chemicals.     

The changing state of contamination in the Lagoon of Venice. Part 2: heavy metals

In order to verify whether pollution is increasing or decreasing, in 25 locations uniformly distributed in the central part of the Lagoon of Venice, a transitional environment suffering from man's urban and industrial activities, the same sampling scheme was repeated three times (in 1987, 1993 and 1998) over a 12-year period during which the lagoonal environment underwent substantial changes. Superficial sediments were sampled and analysed for heavy metals and total organic carbon contents, grain size and density. In general heavy metal contents were found to be correlated, with concentrations above the background level, e.g., for Hg, a concentration factor of 24 was observed in 1987. A temporal decrease in concentrations was observed for most of the metals. Detailed analysis on a smaller spatial scale showed that contamination significantly decreases from the inner border of the lagoon seawards, as highlighted in contour maps. The role of the Porto Marghera industrial zone as a source of pollutants at the border of the Lagoon was confirmed. The decrease in contamination could not be attributed only to a decrease in the intensity of sources, but also to erosion processes, worsened by intensive harvesting of clams with hydraulic dredges.     

The changing state of contamination in the Lagoon of Venice. Part 1: organic pollutants

The Lagoon of Venice is a transitional environment suffering from industrial, urban and agricultural impact. Recently the mechanical clam fishing, preventing a regular deposition of sediments has made sampling of cores suitable for radiodating very problematic. Therefore, in this study, in order to assess temporal and spatial trends of contamination, the same sampling scheme was repeated three times over a 12-year period. The concentrations of PCBs, PAHs and organochlorine pesticides were measured in the uppermost 5 cm of sediments collected in 25 sites in the central portion of the lagoon during three campaigns conducted in 1987, 1993 and 1998. Analytical results, validated statistically, indicated that, while PCB and pesticide concentrations tend to decrease during the considered period of time, PAH do not, showing that the input rate of these compounds to the lagoon environment is still important. A spatial trend of pollution was also found in the lagoon for PCBs and pesticides, which decrease from the sources, namely the industrial zone and the mouths of rivers, to areas closer to the sea: a reduction up to 80% and 90%, respectively, was monitored. PAH contamination, originating chiefly from incomplete combustion of fossil fuels, as inferred from ratios of congeners, was mainly located around the historical center of Venice, where most of the boat traffic is concentrated and has an increasing trend.     

Relationship between the ATP content of subsurface material and the rate of biodegradation of alkylbenzenes and chlorobenzene

The rate of biotransformation of toluene in unconsolidated subsurface material from sites at Lula, Oklahoma, and Conroe, Texas, was compared to the ATP (adenosine triphosphate) content of these materials. The rate of toluene degradation decreased with decreasing ATP content. When ATP contents were at or less than 0.05 ng g⁻¹, biotransformation of toluene could not be detected (less than 1% of the initial concentration was degraded per week). At intermediate concentrations of ATP, 0.37 and 0.16 ngvg⁻¹, the rates of toluene degradation were 18 ± 4.5% and 25 ± 10% of the initial concentration per week. At ATP concentrations above 1 ng g⁻¹, the rates of toluene degradation exceeded 90% of the initial concentration per week. There was no simple relationship between ATP content and chlorobenzene degradation. Subsurface material that had been exposed to creosote wastes, and which degraded toluene rapidly, also degraded benzene, o-xylene, and m-xylene.     

Nature and COVID-19: The pandemic,the environment,and the way ahead

The COVID-19 pandemic has brought profound social, political, economic, and environmental challenges to the world. The virus may have emerged from wildlife reservoirs linked to environmental disruption, was transmitted to humans via the wildlife trade, and its spread was facilitated by economic globalization. The pandemic arrived at a time when wildfires, high temperatures, floods, and storms amplified human suffering. These challenges call for a powerful response to COVID-19 that addresses social and economic development, climate change, and biodiversity together, offering an opportunity to bring transformational change to the structure and functioning of the global economy. This biodefense can include a “One Health” approach in all relevant sectors; a greener approach to agriculture that minimizes greenhouse gas emissions and leads to healthier diets; sustainable forms of energy; more effective international environmental agreements; post-COVID development that is equitable and sustainable; and nature-compatible international trade. Restoring and enhancing protected areas as part of devoting 50% of the planet’s land to environmentally sound management that conserves biodiversity would also support adaptation to climate change and limit human contact with zoonotic pathogens. The essential links between human health and well-being, biodiversity, and climate change could inspire a new generation of innovators to provide green solutions to enable humans to live in a healthy balance with nature leading to a long-term resilient future.