首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 109 毫秒
1.
Abstract

The traditional technologies for odor removal of thiol usually create either secondary pollution for scrubbing, adsorption, and absorption processes, or sulfur (S) poisoning for catalytic incineration. This study applied a laboratory-scale radio-frequency plasma reactor to destructive percentage-grade concentrations of odorous dimethyl sulfide (CH3SCH3, or DMS). Odor was diminished effectively via reforming DMS into mainly carbon disulfide (CS2) or sulfur dioxide (SO2). The removal efficiencies of DMS elevated significantly with a lower feeding concentration of DMS or a higher applied rf power. A greater inlet oxygen (O2)/DMS molar ratio slightly improved the removal efficiency. In an O2-free environment, DMS was converted primarily to CS2, methane (CH4), acetylene (C2H2), ethylene (C2H4), and hydrogen (H2), with traces of hydrogen sulfide (H2S), methyl mercaptan (CH3SH), and dimethyl disulfide. In an O2-containing environment, the species detected were SO2, CS2, carbonyl sulfide, carbon dioxide (CO2), CH4, C2H4, C2H2, H2, formal-dehyde, and methanol. Differences in yield of products were functions of the amounts of added O2 and the applied power. This study provided useful information for gaining insight into the reaction pathways for the DMS dissociation and the formation of products in the plasmolysis and conversion processes.  相似文献   

2.
The paper presents results of the studies photodegradation, photooxidation, and oxidation of phenylarsonic acid (PAA) in aquatic solution. The water solutions, which consist of 2.7 g dm?3 phenylarsonic acid, were subjected to advance oxidation process (AOP) in UV, UV/H2O2, UV/O3, H2O2, and O3 systems under two pH conditions. Kinetic rate constants and half-life of phenylarsonic acid decomposition reaction are presented. The results from the study indicate that at pH 2 and 7, PAA degradation processes takes place in accordance with the pseudo first order kinetic reaction. The highest rate constants (10.45?×?10?3 and 20.12?×?10?3) and degradation efficiencies at pH 2 and 7 were obtained at UV/O3 processes. In solution, after processes, benzene, phenol, acetophenone, o-hydroxybiphenyl, p-hydroxybiphenyl, benzoic acid, benzaldehyde, and biphenyl were identified.  相似文献   

3.
In the present study, selected advanced oxidation processes (AOPs)—namely, photo-Fenton (with Fe2+, Fe3+, and potassium ferrioxalate—FeOx—as iron sources), solar photo-Fenton, Fenton, and UV/H2O2—were investigated for degradation of the antineoplastic drug mitoxantrone (MTX), frequently used to treat metastatic breast cancer, skin cancer, and acute leukemia. The results showed that photo-Fenton processes employing Fe(III) and FeOx and the UV/H2O2 process were most efficient for mineralizing MTX, with 77, 82, and 90 % of total organic carbon removal, respectively. MTX probably forms a complex with Fe(III), as demonstrated by voltammetric and spectrophotometric measurements. Spectrophotometric titrations suggested that the complex has a 2:1 Fe3+:MTX stoichiometric ratio and a complexation constant (K) of 1.47 × 104 M–1, indicating high MTX affinity for Fe3+. Complexation partially inhibits the involvement of iron ions and hence the degradation of MTX during photo-Fenton. The UV/H2O2 process is usually slower than the photo-Fenton process, but, in this study, the UV/H2O2 process proved to be more efficient due to complexing of MTX with Fe(III). The drug exhibited no cytotoxicity against NIH/3T3 mouse embryonic fibroblast cells when oxidized by UV/H2O2 or by UV/H2O2/FeOx at the concentrations tested.  相似文献   

4.
研究了1%和10%(V/V)模拟正丙醇废水在UV/TiO2体系、UV/H2O2体系、Fe2+/H2O2体系和UV/TiO2/Fe2+/H2O2体系等4种工艺条件下的降解动力学过程,对比了降解动力学特点及工艺参数对动力学常数的影响,优化工艺参数。结果表明,UV/TiO2体系和Fe2+/H2O2体系的降解过程可分为零级反应阶段和一级反应阶段,转折点分别在反应开始后2 h和氧化剂浓度为6.7 g/L,UV/H2O2体系和UV/TiO2/Fe2+/H2O2体系分别符合零级反应和一级反应规律;相同工艺参数条件下,6 h反应后,组合工艺UV/TiO2/Fe2+/H2O2体系在处理效率达85%,比前3个体系分别高52.0%、8.3%和32.0%,与UV/TiO2体系和Fe2+/H2O2体系的处理效率之和持平,其协同效应提高了速率常数,在目标物浓度降低时依然可维持较高降解速率。而目标物浓度提高10倍后,UV能量利用率提高35.5倍,氧化剂用量是Fe2+/H2O2体系的1/7.1。  相似文献   

5.
二氧化钛纳米管被用于光催化氧化水体中的百草枯,对光催化反应条件、常见Fe3+离子的干扰情况和百草枯光催化降解动力学规律进行了研究。结果表明,浓度为25 mg/L的百草枯溶液,在二氧化钛纳米管(TNT)1.0 g/L,H2O20.5 mL/50 mL,pH=5.0的最优光催化氧化条件下,经过30 min反应可以被100%从水体中去除,表现出非常高的光催化降解效率;动力学方程拟合表明,百草枯光催化氧化反应符合拟一级动力学规律,动力学方程为ln(C0/C)=1.0267t-0.1282,反应速率常数K为1.0267 h-1;双氧水存在时常见的Fe3+能够进一步提高百草枯光催化降解率;该光催化反应体系对低浓度百草枯废水有很好的处理效果,预示着光催化氧化技术适合地表或地下水体中百草枯的去除。  相似文献   

6.
In order to investigate the effects of humidity on the gas-phase oxidation of SO2 in polluted air and on the subsequent aerosol formation process, photoirradiation experiments were carried out by means of a 4-m3 chamber, in which mixtures containing SO2, NO and C3H6 with concentrations in the ppm range were exposed to simulated solar radiation in different relative humidity (r.h.) conditions. The total amount of oxidized SO2 was quantified from the SO42− yield determined by the chemical analysis of the aerosol product, and a part due to the oxidation by the OH radical was evaluated by estimating the OH concentration from the decay rate of C3H6. The remaining part was assigned to the oxidation by the Criegee intermediate, as it had a good correlation with the progress of the O3 + C3H6 reaction. The contributions of the two oxidizing species to the total conversion and the oxidation rate of SO2 were measured as functions of r.h. As a result, experimental evidence was obtained for the prediction of Calvert and Stockwell's (1983, Envir. Sci. Technol. 17, 428A–443A) simulation that the oxidation due to the Criegee intermediate was retarded by the increase in humidity. The OH contribution, on the other hand, was almost independent of r.h. It was observed consequently that the total oxidized amount of SO2 considerably decreased as r.h. was higher.The humidity effect on the aerosol formation process was found to be more complicated than the effect on the gas-phase chemistry. The maximum rate of increase in the particle number concentration rose linearly with increasing r.h., but the number concentration itself measured at its maximum or at the end of the irradiation reached a ceiling value around r.h. = 30% and went down for higher r.h. The average panicle size in the final stage of the reaction showed a minimum around the same r.h. at which the number concentration was maximum. The H2SO4 concentration in the mist particles, however, decreased monotonically as r.h. got higher. It was suggested that these different responses against the increase in humidity resulted from the cooperation of several processes such as the H2SO4 monomer formation, the H2O condensation, the particle coagulation, etc., which had different dependences on r.h.  相似文献   

7.
Abstract

Sulfur hexafluoride (SF6) is an important gas for plasma etching processes in the semiconductor industry. SF6 intensely absorbs infrared radiation and, consequently, aggravates global warming. This study investigates SF6 abatement by nonthermal plasma technologies under atmospheric pressure. Two kinds of nonthermal plasma processes—dielectric barrier discharge (DBD) and combined plasma catalysis (CPC)—were employed and evaluated. Experimental results indicated that as much as 91% of SF6 was removed with DBDs at 20 kV of applied voltage and 150 Hz of discharge frequency for the gas stream containing 300 ppm SF6, 12% oxygen (O2), and 40% argon (Ar), with nitrogen (N2) as the carrier gas. Four additives, including Ar, O2, ethylene (C2H4), and H2O(g), are effective in enhancing SF6 abatement in the range of conditions studied. DBD achieves a higher SF6 removal efficiency than does CPC at the same operation condition. But CPC achieves a higher electrical energy utilization compared with DBD. However, poisoning of catalysts by sulfur (S)-containing species needs further investigation. SF6 is mainly converted to SOF2,SO2F4, sulfur dioxide (SO2), oxygen difluoride (OF2), and fluoride (F2). They do not cause global warming and can be captured by either wet scrubbing or adsorption. This study indicates that DBD and CPC are feasible control technologies for reducing SF6 emissions.  相似文献   

8.
Fenton氧化法同时脱硫脱硝的实验研究   总被引:1,自引:0,他引:1  
应用Fenton液相氧化吸收法进行同时脱硫脱硝实验。首先,利用单因素实验,分别考察了H2O2浓度、Fe2+投加量、初始pH值、UV照射和温度对脱硫脱硝的影响。结果表明,SO2和NO去除率随着H2O2浓度和Fe2+投加量的增大而提高;初始pH对SO2和NO的去除有较大影响;UV能促进SO2和NO的净化;温度对脱硫效率影响不大,但对NO的去除有显著作用,适当升温可以提高脱硝效率。随后,考察了SO2对NO去除率的影响。通过单独脱硝和同时脱硫脱硝的对比实验发现,SO2的加入对NO的去除有一定的促进作用,Fenton法可同时获得起始约80%的脱硝效率和98%以上的脱硫效率。  相似文献   

9.
The treatment of 1,4-dioxane solution by electrochemical oxidation on boron-doped diamond was studied using a central composite design and the response surface methodology to investigate the use of SO4 2? and HCO3 ? as supporting electrolytes considering the applied electric current, initial chemical oxygen demand (COD) value, and treatment time. Two industrial effluents containing bicarbonate alkalinity, one just carrying 1,4-dioxane (S1), and another one including 1,4-dioxane and 2-methyl-1,3-dioxolane (S2), were treated under optimized conditions and subsequently subjected to biodegradability assays with a Pseudomonas putida culture. Electrooxidation was compared with ozone oxidation (O3) and its combination with hydrogen peroxide (O3/H2O2). Regarding the experimental design, the optimal compromise for maximum COD removal at minimum energy consumption was shown at the maximum tested concentrations of SO4 2? and HCO3 ? (41.6 and 32.8 mEq L?1, respectively) and the maximum selected initial COD (750 mg L?1), applying a current density of 11.9 mA cm?2 for 3.8 h. Up to 98 % of the COD was removed in the electrooxidation treatment of S1 effluent using 114 kWh per kg of removed COD and about 91 % of the COD from S2 wastewater applying 49 kWh per kg of removed COD. The optimal biodegradability enhancement was achieved after 1 h of electrooxidation treatment. In comparison with O3 and O3/H2O2 alternatives, electrochemical oxidation achieved the fastest degradation rate per oxidant consumption unit, and it also resulted to be the most economical treatment in terms of energy consumption and price per unit of removed COD.  相似文献   

10.
In the last few years, several works dealing with Fenton oxidation of ionic liquids (ILs) have proved the capability of this technology for their degradation, achieving complete ILs removal and non-toxic effluents. Nevertheless, very little is known about the kinetics of this process, crucial for its potential application. In this work, the effect of several operating conditions, including reaction temperature (50–90 °C), catalyst load (10–50 mg L?1 Fe3+), initial IL concentration (100–2000 mg L?1), and hydrogen peroxide dose (10–200% of the stoichiometric amount for the complete IL mineralization) on 1-butyl-3-methylimidazolium chloride ([C4mim]Cl) oxidation has been investigated. Under the optimum operating conditions (T = 90 °C; [Fe3+]0 = 50 mg L?1; [H2O2]0 = 100% of the stoichiometric amount), the complete removal of [C4mim]Cl (1000 mg L?1) was achieved at 1.5-min reaction time. From the experimental results, a potential kinetic model capable to describe the removal of imidazolium-based ILs by Fenton oxidation has been developed. By fitting the proposed model to the experimental data, the orders of the reaction with respect to IL initial concentration, Fe3+ amount and H2O2 dose were found to be close to 1, with an apparent activation energy of 43.3 kJ mol?1. The model resulted in a reasonable fit within the wide range of operating conditions tested in this work.  相似文献   

11.
In this study, photocatalytic (photo-Fenton and H2O2/UV) and dark Fenton processes were used to remove ethylenethiourea (ETU) from water. The experiments were conducted in a photo-reactor with an 80 W mercury vapor lamp. The mineralization of ETU was determined by total organic carbon analysis, and ETU degradation was qualitatively monitored by the reduction of UV absorbance at 232 nm. A higher mineralization efficiency was obtained by using the photo-peroxidation process (UV/H2O2). Approximately 77% of ETU was mineralized within 120 min of the reaction using [H2O2]0 = 400 mg L?1. The photo-Fenton process mineralized 70% of the ETU with [H2O2]0 = 800 mg L?1 and [Fe2+] = 400 mg L?1, and there is evidence that hydrogen peroxide was the limiting reagent in the reaction because it was rapidly consumed. Moreover, increasing the concentration of H2O2 from 800 mg L?1 to 1200 mg L?1 did not enhance the degradation of ETU. Kinetics studies revealed that the pseudo-second-order model best fit the experimental conditions. The k values for the UV/H2O2 and photo-Fenton processes were determined to be 6.2 × 10?4 mg L?1 min?1 and 7.7 × 10?4 mg L?1 min?1, respectively. The mineralization of ETU in the absence of hydrogen peroxide has led to the conclusion that ETU transformation products are susceptible to photolysis by UV light. These are promising results for further research. The processes that were investigated can be used to remove pesticide metabolites from drinking water sources and wastewater in developing countries.  相似文献   

12.
The sensitivity of in-cloud oxidation of SO2 in corrective clouds to a number of chemical and physical parameters is examined. The parameterization of precipitation growth processes is based on the work of Scott (1978) and Hegg (1983). A chemical model predicts gas and aqueous phase distributions of soluble gases and in-cloud uncatalyzed oxidation of SO2 by O3 and H2O2. Sulfate aerosol and SO2, CO2, NH3, H2O2 and O3 gases and their aqueous phase dissociation products are treated.The results indicate that in-cloud conversion is an important removal mechanism for SO2 and accounts for a significant fraction of the precipitation sulfate. However, except at low SO2 concentrations, the precipitation sulfate concentration is insensitive to the initial SO2 concentration; the sulfate concentration is most sensitive to the initial H2O2 and NH3 concentrations. At low SO2 concentrations, the precipitation sulfate concentration is determined primarily by the initial sulfate aerosol concentration. The feedback between sulfate production and pH is important in limiting SO2 oxidation by O3. If gas phase H2O2 of order 1 ppb is the major source of aqueous phase H2O2 for S(IV) oxidation, it is likely that the oxidation reaction is oxidant limited. The sulfate concentration is a decreasing function of the precipitation rate. At low rainfall rates (< 1 mm h−1), ice phase growth decreases the sulfate concentration. However, the results are insensitive to an ice phase origin at moderate and high rainfall rates.  相似文献   

13.
The microstructure of 1/10 and 1/20 atmosphere, lean H2S—O2—N2 flames is developed using the mass-spectrometric flame-sampling technique. The flame mechanism developed is in agreement with that determined from an earlier study on 1-atm H2S flames. The formation of SO2 appears to be primarily related to the production of SH and the ensuing oxidation steps SH + O2 = SO + OH and SO + O2 = SO2 + O. While there is some question whether SO2 formation occurs via an SO or an S2O intermediate, the present study does not give direct support to the role of S2O in the oxidation mechanism. However, the presence of significant quantities of free sulfur in the pre-flame zone may be indicative of S2O formation via SO + S → S2O, and, possibly, via the disproportionation of SO, 3SO → S2O + SO2. Kinetic analyses of some of the pre-flame reactions indicate an apparent activation energy of 17,300 calories/mole for the decomposition of H2S. The actual initiation process in the flame mechanism requires further examination. The specific rate for the reaction step H2S + O = OH + SH is given by k 6 = 1.45 × 1015 exp ( – 6600/RT) cm3 mole–1 sec–1, and the specific rate for the oxidation of SO, SO + O2 = SO2 + O, is given by k 5 = 5.2 × 1014 exp (—19,300/RT) cm3 mole–1 sec–1.  相似文献   

14.
The photodegradation of two common and very stable azo-dyes, i.e. methyl-orange (C14H14N3SO3Na) and orange II (C16H11N2SO4Na), is reported. The photocatalytic oxidation was carried out in aqueous suspensions of polycrystalline TiO2 irradiated by sunlight. Compound parabolic collectors, installed at the “Plataforma Solar de Almería” (PSA, Spain) were used as the photoreactors and two identical reacting systems allowed to perform photoreactivity runs for the two dyes at the same time and under the same irradiation conditions. The disappearance of colour and substrates together with the abatement of total organic carbon content was monitored. The main sulfonate-containing intermediates were found to be in lower number in respect to those obtained under artificial irradiation. In particular there were no more evidence of the presence of hydroxylated transients. The dependence of dye photooxidation rate on: (i) substrate concentration; (ii) catalyst amount; and (iii) initial pH was investigated. The influence of the presence of strong oxidant species (H2O2, S2O82−) and some ions (Cl, SO42−) on the process was also studied.  相似文献   

15.
Chen HW  Chen CY  Wang GS 《Chemosphere》2011,85(4):591-597
The presence of various organic contaminants in water sources is of concern due to their direct threats to human health and potential to react with disinfectants to form carcinogenic byproducts including trihalomethanes, haloacetic acids and nitrosamines in finished water. This study applied both medium-pressure and low-pressure ultraviolet light coupled with hydrogen peroxide (UV/H2O2) to evaluate its efficacy for degradation of selected nitrogenous organic compounds and corresponding disinfection byproduct (DBP) formation. Six organic compounds were chosen as target precursors based on their nitrogen contents and molecular structures. The results showed that higher oxidation capacity resulted in better reduction of organic matters and DBP formation potentials (DBPFPs). However, insufficient contact time and oxidant doses could lead to a rise of DBPFPs in the early stages of UV/H2O2 reactions. A greater percentage removal was achieved for organic carbon than organic nitrogen after UV/H2O2 treatment, especially for compounds with complicated structure such as diltiazem. During the UV/H2O2 treatment, the intermediate products include tertiary amine, dimethyl amine (DMA) or DMA-like structures, which are N-nitrosodimethylamine (NDMA) precursors after chlorination or chloramination. Furthermore, it was observed that using dissolved organic nitrogen and DMA to predict NDMAFP could lead to biased conclusions because of the complex nature of nitrogenous matters in aqueous environments.  相似文献   

16.
Photochemical degradation of fluoroquinolone ciprofloxacin (CIP) in water by UV and UV/H2O2 were investigated. The degradation rate of CIP was affected by pH, H2O2 dosage, as well as the presence of other inorganic components. The optimized pH value and H2O2 concentration were 7.0 and 5 mM. Carbonate and nitrate both impeded CIP degradation. According to liquid chromatography–tandem mass spectrometry analysis, four and 16 products were identified in UV and UV/H2O2 system, respectively. Proposed degradation pathways suggest that reactions including the piperazinyl substituent, quinolone moiety, and cyclopropyl group lead to the photochemical degradation of CIP. Toxicity of products assessed by Vibrio qinghaiensis demonstrated that UV/H2O2 process was more capable on controlling the toxicity of intermediates in CIP degradation than UV process.  相似文献   

17.

A theoretical and experimental study of bisphenol A (BPA) degradation by the UV/H2O2 process in water is presented. The effects of the H2O2 concentration and the specific rate of photon emission (EP,0) on BPA degradation were investigated. A kinetic model derived from a reaction sequence was employed to predict BPA and hydrogen peroxide concentrations over time using an annular photochemical reactor in batch recirculation mode. The local volumetric rate of photon absorption (LVRPA) inside the photoreactor was computed using a Line Source with Parallel Plane emission model (LSPP). From the proposed kinetic model and the experimental data, the second order rate constants of the reactions between hydroxyl radicals and the main reacting species (H2O2 and BPA) were estimated applying a nonlinear regression method. A good agreement between the kinetic model and experimental data, for a wide range of operating conditions, was obtained. For BPA, H2O2, and TOC concentrations, the calculated root means square errors (RMSE) were 2.3?×?10??2, 9.8?×?10??1, and 9.0?×?10??2 mmol L??1, respectively. The simplified kinetic model presented in this work can be directly applied to scaling-up and reactor design, since the estimated kinetic constants are independent of the reactor size, shape, and configuration. Further experiments were made by employing low BPA initial concentration (100 μg L??1) in water and real wastewater. A lower degradation rate of BPA was observed in the real wastewater, although the UV/H2O2 process has also been able to completely degrade the target pollutant in less than 1 h.

  相似文献   

18.

The vacuum ultraviolet (VUV) process, which can directly produce hydroxyl radical from water, is considered to be a promising oxidation process in degrading contaminants of emerging concern, because of no need for extra reagents. In this study, the influencing factors and mechanism for degradation of diethyl phthalate (DEP) by the VUV process were investigated. The effects of irradiation intensity, inorganic anions, natural organic matter (NOM), and H2O2 dosage on the performance of VUV process were evaluated. The results showed that DEP could be more efficiently degraded by the VUV process compared with ultraviolet (UV)-254-nm irradiation. The presence of HCO3?, NO3? and NOM in the aqueous solutions inhibited the degradation of DEP to a different degree, mainly by competing hydroxyl radicals (HO?) with DEP. Degradation rate and removal efficiency of DEP by VUV process significantly enhanced with the addition of H2O2, while excess H2O2 dosage could inhibit the DEP degradation. Moreover, based on the identified seven oxidation byproducts and their time-dependent evolution profiles, a possible pathway for DEP degradation during the VUV process was proposed. Finally, the ecotoxicity of DEP and its oxidation byproducts reduced overall according to the calculated results from Ecological Structure Activity Relationships (ECOSAR) program. The electrical energy per order (EE/O) was also assessed to analysis the energy cost of the DEP degradation in the VUV process. Our work showed the VUV process could be an alternative and environmental friendly technology for removing contaminants in water.

  相似文献   

19.
G Matafonova  V Batoev 《Chemosphere》2012,89(6):637-647
Excilamps as modern mercury-free sources of narrow-band UV radiation represent an attractive alternative in environmental applications. This review focuses on recent studies on the water and surface decontamination with excilamps by means of direct photolysis and advanced oxidation processes. To date, direct photolysis and advanced oxidation processes (AOPs) such as UV/H2O2, UV/Fenton and UV/O3 have been applied for degradation of organic compounds (mainly, phenols, dyes and herbicides) in model aqueous solutions. Special emphasis is placed on studies combining UV irradiation (as a pre-treatment or post-treatment step) with biological treatment. In this review, the efficiencies of direct UV, UV/H2O2 and UV/TiO2 processes for inactivation of a variety of pathogenic microorganisms in water and on surfaces are discussed. The analysis of the literature shows that more works need to be done on scaling up the processes, degradation/mineralization of target pollutant(s) in real effluents and evaluation of energy requirements.  相似文献   

20.
A chemiluminescent method for measuring hydrogen peroxide was developed using hemin as a catalyst for luminol-based H2O2 oxidation, which gave a detection limit below 0.1 μg ∝−1 in the solution. It was shown that most atmospheric species did not give serious interference, and that negative interference of SO2; could be eliminated if pH of the collecting solution was above 10 whereas O3, gave significant positive interference. The Henry's law constant of H2O2 was experimentally determined to be 1.42 × 105 M atm−1 at 20°C at ambient concentration levels of H2O2. This method was also applied to the measurements of H2O2 concentration in rainwater in Tokyo, Japan, which was in the range of 5–1065μg ∝−1.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号