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1.
在富氧条件下,研究了CH4、C3H8、C 3H6、C8H18、CH 3OH、C2H5OH,以及C3H6与CH3OH、C3H6与C2H5OH组合作还原剂时,在Ag/Al2O3催化剂上NO的还原活性.结果表明,不同碳氢化合物还原NO的活性温度存在较大的差异.SO2的存在会导致CH3OH还原NO的活性提高,而其他碳氢化合物还原NO的活性降低.随着还原剂浓度提高,NOx转化率增大,不过,过高的还原剂浓度对NO还原不利.组合使用CH3OH与C3H6或C2H5OH与C3H6作为还原剂,能显著拓宽活性温度范围.  相似文献   

2.
以膨胀珍珠岩为载体,采用溶胶凝胶法对其进行负载,制备出不同类型的光催化材料(TiO2-EP、Ag+-TiO2-EP),并在模拟日光条件下,研究其对甲基橙溶液的降解效果。结果表明,浸渍3次且担载0.04% Ag+的负载型TiO2光催化活性最高,在光催化剂用量为0.3 g,20 mL初始浓度为10 mg/L甲基橙溶液光照4 h后降解率可达81.6%,且甲基橙的光催化降解服从一级动力学方程。回收3次后仍有较强的活性,其2 h降解率为24.8%。  相似文献   

3.
We examined acute (2 h exposure of 5-day-old larvae) and subchronic (exposure from fertilization up to an age of 11 days) effects of NiCl(2).6H2O on embryos and larvae of zebrafish (Danio rerio), both alone and in combination with oxygen depletion. The following endpoints were recorded: acute exposure: locomotory activity and survival; subchronic exposure: hatching rate, deformations, locomotory activity (at 5, 8 and 11 days) and mortality. In acute exposures nickel chloride (7.5-15 mg Ni/L) caused decreasing locomotory activity. Oxygen depletion (or=10 mg Ni/L resulted in delayed hatching at an age of 96 h, in decreased locomotory activity at an age of 5 days, and increased mortality at an age of 11 days (LC20=9.5 mg Ni/L). The observed LOEC for locomotory activity (7.5 mg Ni/L) is in the range of environmentally relevant concentrations. Since locomotory activity was already affected by acute exposure, this parameter is recommended to supplement commonly recorded endpoints of toxicity.  相似文献   

4.
INTENTION, GOAL, SCOPE, BACKGROUND: Since the intermediate products of some compounds can be more toxic and/or refractory than the original compund itself, the development of innovative oxidation technologies which are capable of transforming such compounds into harmless end products, is gaining more importance every day. Advanced oxidation processes are one of these technologies. However, it is necessary to optimize the reaction conditions for these technologies in order to be cost-effective. OBJECTIVE: The main objectives of this study were to see if complete mineralization of 4-chlorophenol with AOPs was possible using low pressure mercury vapour lamps, to make a comparison of different AOPs, to observe the effect of the existence of other ions on degradation efficiency and to optimize reaction conditions. METHODS: In this study, photochemical advanced oxidation processes (AOPs) utilizing the combinations of UV, UV/H2O2 and UV/H2O2/Fe2+ (photo-Fenton process) were investigated in labscale experiments for the degradation and mineralization of 4-chlorophenol. Evaluations were based on the reduction of 4-chlorophenol and total organic carbon. The major parameters investigated were the initial 4-chlorophenol concentration, pH, hydrogen peroxide and iron doses and the effect of the presence of radical scavengers. RESULTS AND DISCUSSION: It was observed that the 4-chlorophenol degradation efficiency decreased with increasing concentration and was independent of the initial solution pH in the UV process. 4-chlorophenol oxidation efficiency for an initial concentration of 100 mgl(-1) was around 89% after 300 min of irradiation in the UV process and no mineralization was achieved. The efficiency increased to > 99% with the UV/H2O2 process in 60 min of irradiation, although mineralization efficiency was still around 75% after 300 min of reaction time. Although the H2O2/4-CP molar ratio was kept constant, increasing initial 4-chlorophenol concentration decreased the treatment efficiency. It was observed that basic pHs were favourable in the UV/H2O2 process. The results showed that the photo-Fenton process was the most effective treatment process under acidic conditions. Complete disappearance of 100 mgl(-1) of 4-chlorophenol was achieved in 2.5 min and almost complete mineralization (96%) was also possible after only 45 min of irradiation. The efficiency was negatively affected from H2O2 in the UV/H2O2 process and Fe2+ in the photo-Fenton process over a certain concentration. The highest negative effect was observed with solutions containing PO4 triple ions. Required reaction times for complete disappearance of 100 mgl(-1) 4-chlorophenol increased from 2.5 min for an ion-free solution to 30 min for solutions containing 100 mgl(-1) PO4 triple ion and from 45 min to more than 240 min for complete mineralization. The photodegradation of 4-chlorophenol was found to follow the first-order law. CONCLUSION: The results of this study showed that UV irradiation alone can degrade 4-CP, although at very slow rates, but cannot mineralize the compound. The addition of hydrogen peroxide to the system, the so-called UV/H2O2 process, significantly enhances the 4-CP degradation rate, but still requires relatively long reaction periods for complete mineralization. The photo-Fenton process, the combination of homogeneous systems of UV/H2O2/Fe2+ compounds, produces the highest photochemical elimination rate of 4-CP and complete mineralization is possible to achieve in quite shorter reaction periods when compared with the UV/H2O2 process. RECOMMENDATIONS AND OUTLOOK: It is more cost effective to use these processes for only purposes such as toxicity reduction, enhancement of biodegradability, decolorization and micropollutant removal. However the most important point is the optimization of the reaction conditions for the process of concern. In such a case, AOPs can be used in combination with a biological treatment systems as a pre- or post treatment unit providing the cheapest treatment option. The AOP applied, for instance, can be used for toxicity reduction and the biological unit for chemical oxygen demand (COD) removal.  相似文献   

5.
将生物选择性吸附和光催化技术耦合合成一种新型的多功能壳聚糖-二氧化钛吸附剂(CTA),这种新型的多功能壳聚糖-二氧化钛吸附剂能够同时吸附重金属和降解有机污染物。实验发现,CTA对银离子有较好的吸附容量,在初始浓度为1 000 mg/L时吸附容量为100.3 mg/g,且吸附了银离子的吸附剂对甲基橙有更好的降解效果。扫描电镜表明,CTA紫外条件下吸附银以后表面会有纳米银的生成,能谱显示纳米银颗粒在一定条件下可以由CTA表面自行脱落。  相似文献   

6.
Carbofuran is a toxic carbamate pesticide, and its use has increased in recent years. While marketing information indicates stability in different chemical media, carbofuran exhibits relative photolability. The aim of this research was to decompose carbofuran and to identify the photoproducts achieved when two different doped titania photocatalysts were employed under UV irradiation. The iron-doped TiO2 materials were obtained (a) via a hydrothermal method and (b) by an ultrasound-assisted sol–gel method. The precursors were TiOSO4?xH2O and Fe3(NO3)·9H2O. X-ray studies confirmed that the anatase phase of the iron-doped TiO2 resulted from the two preparation methods. The photocatalytic performance of the prepared materials was monitored by LC/ESI-QTOF-MS, enabling the identification of photoproducts: oxo-carbamates, hydroxylated benzofuranes, a carboxamide, and one amine. By using the iron-doped TiO2 materials, 2,2-dimethyl-2,3-dihydrobenzofuran-3,7-diol was the most abundant photoproduct, and N,2,2-trimethyl-2,3-dihydrobenzofuran-7-amine was the only compound that had not been previously reported in the photolysis and photocatalysis of carbofuran. The product 3-hydroxy carbofuran, a cholinesterase inhibitor, was quantified and was found to be transformed into compounds that lack this inhibitive property.  相似文献   

7.
在水源污染越来越严重、水质标准日益严格的背景下,超滤(UF)已逐渐成为替代饮用水常规处理技术的最佳选择之一。本研究中采用相转化法,将聚偏氟乙烯(PVDF)、聚乙二醇(PEG)和二氧化钛(TiO2)共混制得光催化复合分离膜并对其进行扫描电子显微镜(SEM)、原子力显微镜(AFM)和X射线能谱仪(EDS)等相应的表征。比较了有无光照条件下,PVDF-PEG和PVDF-PEG-TiO2膜对腐殖酸(HA)的截留和超滤过程中的膜污染情况。研究结果表明,TiO2光催化复合分离膜能提高对水中天然有机物的去除并同时降低膜污染。紫外光照强度越强,PVDF-PEG-TiO2膜的抗污染性能越好。另外,光催化能更有效地减少超滤初始浓度较低的腐殖酸溶液过程中的膜通量衰减。  相似文献   

8.
The Ostwald solubility coefficient, L of 17 volatile organic compounds (VOCs) from the gas phase into water and dilute aqueous ammonia solutions was determined by the equilibrium partitioning in closed system-solid phase micro extraction (EPICS-SPME) method at 303 K and at 0-2.5 mol dm(-3) ammonia concentrations. Ammonia increased the solubility of all VOCs nearly linearly, but to a different extent. The difference in the solubility values in aqueous ammonia solutions (Lmix) compared to pure water (L) is explained on the basis of a Linear Solvation Energy Relationship (LSER) equation made applicable for solvent mixtures, logLmix - logL = x((sNH3 - sH2O)pi2H + (aNH3 - aH2O)Sigma2H + (bNH3 - bH2O)Sigmabeta2H + (vNH3 - VH2O)Vx). sNH3 - sH2O, aNH3 - aH2O, bNH3 - bH2O, vNH3 - vH2O are the differences of solvent parameters, x is the mole fraction, pi2H is the solute dipolarity-polarizability, Sigmaalpha2H is the effective hydrogen bond acidity of the solute, Sigmabeta2H is the effective hydrogen bond basicity of the solute and Vx, the McGowan characteristic volume. The most significant term was v, the phase hydrophobicity. The solubility behavior was explained by the change in structure of the aqueous solution: the presence of ammonia reduces the cavity effect. These findings show that the presence of compounds such as ammonia, frequently observed in environmental waters, especially wastewaters, affect the fugacity of VOCs, having consequences for the environmental partitioning of VOCs and having technical consequences towards wastewater treatment technologies.  相似文献   

9.
Pinna MV  Pusino A 《Chemosphere》2011,82(6):817-821
The photodegradation of the aryloxyphenoxy propionic herbicide cyhalofop-butyl (2R)-2-[4-(4-cyano-2-fluorophenoxy)phenoxy]butylpropanoate (CyB), and of its primary metabolite (2R)-2-[4-(4-cyano-2-fluorophenoxy)phenoxy]propanoic acid (CyA) was studied in water at different irradiation wavelengths. The sunlight irradiation was investigated also in the presence of humic acid (HA), Fe oxide, titanium dioxide (TiO2) and zinc oxide (ZnO) as photocatalysts.CyB and CyA were rapidly degraded by UV irradiation. CyB afforded the butyl ester of 2-[3-(4-cyano-2-fluorophenyl)-4-hydroxy-phenoxy]propanoic acid (CyI), a metabolite arising from a photo-Fries rearrangement. Instead, CyA yielded (R)-2-4-(4-carboxyl-2-fluorophenoxy)phenoxypropanoic acid (CyD), a dicarboxylic acid arising from the photo-hydrolysis of cyano group via amide. CyB was stable in simulated sunlight also in the presence of the catalysts tested.The irradiation of a CyA solution, in the presence of HA or Fe oxide, with simulated sunlight did not produce any significant degradation. In the same experimental conditions, CyA was totally mineralized in the presence of TiO2 and ZnO.  相似文献   

10.
This work describes the nitration of aromatics upon near-UV photolysis of nitrate and nitrite in aqueous solution and upon photocatalytic oxidation of nitrite in TiO2 suspensions. Phenol is used in this work as a model aromatic molecule and as a probe for *NO2/N2O4. The photoinduced nitration of phenol in aqueous systems occurs upon the reaction between phenol and *NO2 or N2O4, and is enhanced by the photocatalytic oxidation of nitrite to *NO2 by TiO2. Aromatic photonitration in the liquid phase can play a relevant role in the formation of nitroaromatics in natural waters and atmospheric hydrometeors, thus being a potential pathway for the condensed-phase nitration of aromatics. Furthermore, the photoinduced oxidation of nitrite to nitrogen dioxide suggests a completely new role for nitrite in natural waters and atmospheric aerosols.  相似文献   

11.
The production of N2 gas by denitrification may lead to the appearance of a gas phase below the water table prohibiting the conservative transport of tracer gases required for groundwater dating. We used a two-phase flow and transport model (STOMP) to study the reliability of 3H/3He, CFCs and SF6 as groundwater age tracers under agricultural land where denitrification causes degassing. We were able to reproduce the amount of degassing (R2 = 69%), as well as the 3H (R2 = 79%) and 3He (R2 = 76%) concentrations observed in a 3H/3He data set using simple 2D models. We found that the TDG correction of the 3H/3He age overestimated the control 3He/3He age by 2.1 years, due to the accumulation of 3He in the gas phase. The total uncertainty of degassed 3H/3He ages of 6 years (± 2 σ) is due to the correction of degassed 3He using the TDG method, but also due to the travel time in the unsaturated zone and the diffusion of bomb peak 3He. CFCs appear to be subject to significant degradation in anoxic groundwater and SF6 is highly susceptible to degassing. We conclude that 3H/3He is the most reliable method to date degassed groundwater and that two-phase flow models such as STOMP are useful tools to assist in the interpretation of degassed groundwater age tracer data.  相似文献   

12.
Sun C  Zhao J  Ji H  Ma W  Chen C 《Chemosphere》2012,89(4):420-425
There have been serious concerns about polybromodiphenyl ethers (PBDEs) in the environment because of their global distribution and bioaccumulation. Owing to strong hydrophobicity of PBDEs, the regular photocatalytic system, in which the substrate is solvated in the bulk solution, is not applicable to the removal of the PBDEs in water. In this work, the photocatalytic reduction degradation of decabromodiphenyl ether (BDE209), the most-used PBDEs, was investigated in aqueous system, by pre-adsorbing it on the surface of photocatalyst. It was found that the preloaded BDE209 underwent efficient reductive debromination in aqueous system under irradiation with wavelength larger than 360 nm in the presence of electron donors such as methanol. Our experiments further show that such a preloaded system exhibits different characteristics from that in the organic solution. The meta-debrominated intermediate is predominant in the present system, while the ortho-debrominated one is the main nona-BDE products in the organic solution. In addition, different from other photocatalytic system, the pH has little effect on the photocatalytic reaction. We propose that these differences are originated from the formation of overlayer of hydrophobic BDE209 to limit the motion of BDE209 and the access of water and H+/OH to the TiO2 surface.  相似文献   

13.
Collection of atmospheric H2O2 was performed by a cold trap method using dry ice-acetone as the refrigerant. The air was drawn by a pump into a glass gas trap immersed in the dry ice-acetone slush in a dewar flask at a flow rate of 2.5 l min-1 for approximately 2 h. Collection efficiency was > 99% and negligible interferences by O3, SO2 or organic matter with the collected H2O2 in the trap were observed. This method was compared with the air impinger bubbling method which has been previously described (Kok et al., 1978a, b, Envir. Sci. Technol. 12, 1072-1080). The measured total peroxide (H2O2 + organic peroxide) values in a series of aim samples collected by the impinger bubbling method (0.06-3.7 ppb) were always higher than those obtained by the cold trap method (0.02-1.2 ppb). Laboratory experiments suggest that the difference in values between the two methods probably results from the aqueous phase generation of H2O2 and organic peroxide in the impinger solution by a reaction of atmospheric O3 with olefinic and aromatic compounds. If these O3-organic compound reactions which occur in the impinger also occur in aqueous droplets in the atmosphere, the process could be very important for aqueous phase generation of H2O2 in clouds and rainwater.  相似文献   

14.
BACKGROUND, AIMS AND SCOPE: Chromium enters into the aquatic environment as a result of effluent discharge from steel works, electroplating, leather tanning industries and chemical industries. As the Cr(VI) is very harmful to living organisms, it should be quickly removed from the environment when it happens to be contaminated. Therefore, the aim of this laboratory research was to develop a rapid, simple and adaptable solvent extraction system to quantitatively remove Cr(VI) from polluted waters. METHODS: Aqueous salt-solutions containing Cr(VI) as CrO4(2-) at ppm level (4-6 ppm) were prepared. Equal volumes (5 ml) of aqueous and organic (2-PrOH) phases were mixed in a 10 ml centrifuge tube for 15 min, centrifuged and separated. Concentrations of Cr(VI), in both the aqueous and organic phases, were determined by atomic absorption spectrometry. The effects of salt and acid concentrations, and phase-contact time on the extraction of Cr(VI) were investigated. In addition, the extraction of Cr(VI) was assessed in the presence of tetramethylammonium chloride (TMAC) in 2-PrOH phase. Effects of some other metals, (Cd(II), Co(II), Cu(II), Ni(II) and Zn(II)), on the extraction of Cr(VI) were also investigated. RESULTS AND DISCUSSION: The Cr(VI) at ppm level was extracted quantitatively by salting-out the homogeneous system of water and 2-propanol(2-PrOH) using chloride salts, namely CaCl2 or NaCl, under acidic chloride media. The extracted chemical species of Cr(VI) was confirmed to be the CrO3Cl-. The ion-pair complex extracted into the organic phase was rationalized as the solvated ion-pair complex of [2-PrOH2+, CrO3Cl-]. The complex was no longer stable. It implied the reaction between extracted species. Studies revealed that salts and acid directly participated in the formation of the above complex. Use of extracting agents (TMAC) didn't show any significant effect on the extraction of Cr(VI) under high salting-out conditions. There is no significant interference effect on the extraction of Cr(VI) by the presence of other metals. The Cr(VI) in the organic phase was back-extracted using an aqueous ammonia solution (1.6 mol dm(-3)) containing 3 mol dm(-3) NaCl. The extraction mechanism of Cr(VI) is also discussed. CONCLUSIONS: Salting-out of homogeneous mixed solvent of 2-propanol can be employed to extract Cr(VI) quantitatively, as an ion-pair of [2-PrOH2+ * CrO3Cl-] solvated by 2-PrOH molecules. Then, the complex becomes 'solvent-like' and is readily separated into the organic phase. The increase of Cl- ion concentration in the aqueous phase favors the extraction. The 2-PrOH, salts and acid play important roles in the extraction process. There is no need to use an extracting agent at a high salting-out condition. RECOMMENDATIONS AND PERSPECTIVES: Chromium(VI) must be quickly removed before it enters into the natural cycle. As the 2-PrOH is water-miscible in any proportion, ion-pairing between 2-PrOH2+ and CrO3Cl- becomes very fast. As a result, Cr(VI) can easily be extracted. Therefore, the method is recommended as a simple, rapid and adaptable method to quickly separate Cr(VI) from aqueous samples.  相似文献   

15.
通过溶胶-凝胶法制备了同时具有可见光(Vis)光催化和Fenton催化双重活性的Co-TiO2催化剂。通过对比Vis/Co-TiO2/KHSO5、Co-TiO2/KHSO5和Vis/Co-TiO23种体系对苯酚的降解效果,Vis/Co-TiO2/KHSO5表现出明显的Fenton-光催化协同作用。进一步研究pH值、KHSO5与苯酚摩尔比(nKHSO5∶nC6H6O)和Co-TiO2投加量(mCo-TiO2)对Fenton-光催化协同降解苯酚效果的影响。结果表明,pH=6.9、nKHSO5∶nC6H6O=10∶1、mCo-TiO2=1.0 g/L时,降解率达100%。最后,结合XRD、XPS和UV-DRS等手段和催化活性实验数据分析了Vis/Co-TiO2/KHSO5体系的催化机理。  相似文献   

16.
Cu/La共掺杂TiO2光催化氧化水中的氨氮   总被引:1,自引:0,他引:1  
采用水解-沉淀法制备了Cu/La共掺杂纳米TiO2催化剂,利用XRD、XPS和BET技术对其进行表征,并考察了在紫外灯下,共掺杂TiO2对氨氮的光催化氧化工艺条件。物相结构和比表面积测试结果表明,共掺杂催化剂具有较好的锐钛矿晶型,孔径分布为4~8 nm,Cu/La共掺杂TiO2La以La3+,Cu是以Cu2+、Cu+的形式掺杂进入TiO2的晶格。光催化实验表明:所得改性光催化剂对氨氮的去除及焦化废水的处理均具有较高的催化活性。  相似文献   

17.
Kumar A  Pandey AK  Singh SS  Shanker R  Dhawan A 《Chemosphere》2011,83(8):1124-1132
Extensive production and consumption of nanomaterials such as ZnO and TiO2 has increased their release and disposal into the environment. The accumulation of nanoparticles (NPs) in ecosystem is likely to pose threat to non-specific targets such as bacteria. The present study explored the effect of ZnO and TiO2 NPs in a model bacterium, Salmonella typhimurium. The uptake of ZnO and TiO2 bare NPs in nano range without agglomeration was observed in S. typhimurium. TEM analysis demonstrated the internalization and uniform distribution of NPs inside the cells. Flow cytometry data also demonstrates that both ZnO and TiO2 NPs were significantly internalized in the S. typhimurium cells in a concentration dependent manner. A significant increase in uptake was observed in the S. typhimurium treated even with 8 and 80 ng mL−1 of ZnO and TiO2 NPs with S9 after 60 min, possibly the formation of micelles or protein coat facilitated entry of NPs. These NPs exhibited weak mutagenic potential in S. typhimurium strains TA98, TA1537 and Escherichia coli (WP2uvrA) of Ames test underscoring the possible carcinogenic potential similar to certain mutagenic chemicals. Our study reiterates the need for re-evaluating environmental toxicity of ZnO and TiO2 NPs presumably considered safe in environment.  相似文献   

18.
An automated system for continuous measurement of N2O fluxes on an hourly basis was employed to study N2O emissions in an intensively managed low carbon calcareous soil under sub-humid temperate monsoon conditions. N2O emissions occurred mainly within two weeks of application of NH4+-based fertilizer and total N2O emissions in wheat (average 0.35 or 0.21 kg N ha−1 season−1) and maize (average 1.47 or 0.49 kg N ha−1 season−1) under conventional and optimum N fertilization (300 and 50-122 kg N ha−1, respectively) were lower than previously reported from low frequency measurements. Results from closed static chamber showed that N2O was produced mainly from nitrification of NH4+-based fertilizer, with little denitrification occurring due to limited readily oxidizable carbon and low soil moisture despite consistently high soil nitrate-N concentrations. Significant reductions in N2O emissions can be achieved by optimizing fertilizer N rates, using nitrification inhibitors, or changing from NH4+- to NO3ˉ-based fertilizers.  相似文献   

19.
Attempt has been made to study the accumulation behaviour of a common plant, Mung bean (Vigna radiata) towards Cr(III) and Cr(VI) to have an insight on the migration and bio-magnification of Cr. For this purpose healthy germinated Mung bean seeds were sown in the sand in the presence of Hoagland's nutrient solution containing measured amount of K(2)(51)Cr(2)O(7) and (51)Cr(NO(3))(3).9H(2)O. Growth rate was also studied in the presence and absence of phosphate salts in the medium. It has been found that the transfer of chromium from soil to plant is significantly low (maximum 5% for both Cr(III) and Cr(VI)). Maximum accumulation of Cr occurs in the root with respect to the total chromium accumulation by the plant. Other parts of the Mung bean plant, e.g. cotyledons, shoot and leaves, show negligible accumulation. Therefore, the chance of direct intake of Cr through food as well as through the grazing animals to human body is less.  相似文献   

20.
考察了3种不同硅铝比的ZSM-5沸石分子筛(25H、38H和50H,25、38和50为硅铝比)对水中Cu2+的吸附过程及其影响因素。结果表明,3种材料均能有效吸附去除水中Cu2+离子,动力学符合假二阶动力学模型,吸附等温线符合Langmuir吸附等温式。3种材料吸附速率及吸附容量顺序为:25H〉50H〉38H,其中,25H最大吸附容量达到12.83mg/g。投加量由0.8g/L增加至2.0g/L,材料对Cu2+吸附去除率由87.0%增加至97.5%。考察水中常见阳离子对吸附的干扰作用,结果表明,干扰离子的影响顺序为:Pb2+〉K+〉Na+〉Mg2+;随着干扰离子浓度的增大,材料对Cu2+的去除率显著下降。硅铝比及晶粒形貌均对沸石分子筛吸附Cu2+有较大影响,小的孔径不利于Cu2+的吸附,低硅铝比有利于Cu2+在分子筛上的吸附。  相似文献   

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