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1.
In the present study, photocatalytic reactions of nitrogen oxides (NOx = NO + NO2) were studied on commercial TiO2 doped facade paints in a flow tube photoreactor under simulated atmospheric conditions. Fast photocatalytic conversion of NO and NO2 was observed only for the photocatalytic paints and not for non-catalytic reference paints. Nitrous acid (HONO) was formed in the dark on all paints studied, however, it efficiently decomposes under irradiation only on the photocatalytic samples. Thus, it is concluded that photocatalytic paint surfaces do not represent a daytime source of HONO, in contrast to other recent studies on pure TiO2 surfaces. As main final product, the formation of adsorbed nitric acid/nitrate anion (HNO3/NO3?) was observed with near to unity yield. In addition, traces of H2O2 were observed in the gas phase only in the presence of O2. Formation of the greenhouse gas nitrous oxide (N2O) could be excluded. The uptake kinetics of NO, NO2 and HONO was very fast under atmospheric conditions (e.g. γ(NO + TiO2) > 10?5). Thus, the uptake on urban surfaces (painted houses, etc.) will be limited by transport. For a hypothetically painted street canyon, an average reduction of nitrogen oxide levels of ca. 5% is estimated. Since the harmful HNO3/NO3? is formed on the surface of the photoactive paints, whereas it is formed in the gas phase in the atmosphere, the use of photocatalytic paints may also help to reduce acid deposition, e.g. on plants, or nitric acid related health issues.  相似文献   

2.
Fe2O3 and CeO2 modified activated coke (AC) synthesized by the equivalent-volume impregnation were employed to remove elemental mercury (Hg0) from simulated flue gas at a low temperature. Effects of the mass ratio of Fe2O3 and CeO2, reaction temperature, and individual flue gas components including O2, NO, SO2, and H2O (g) on Hg0 removal efficiency of impregnated AC were investigated. The samples were characterized by Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). Results showed that with optimal mass percentage of 3 % Fe2O3 and 3 % CeO2 on Fe3Ce3/AC, the Hg0 removal efficiency could reach an average of 88.29 % at 110 °C. Besides, it was observed that O2 and NO exhibited a promotional effect on Hg0 removal, H2O (g) exerted a suppressive effect, and SO2 showed an insignificant inhibition without O2 to some extent. The analysis of XPS indicated that the main species of mercury on used Fe3Ce3/AC was HgO, which implied that adsorption and catalytic oxidation were both included in Hg0 removal. Furthermore, the lattice oxygen, chemisorbed oxygen, and/or weakly bonded oxygen species made a contribution to Hg0 oxidation.  相似文献   

3.
A thermal/optical carbon analyzer (TOA), normally used for quantification of organic carbon (OC) and elemental carbon (EC) in PM2.5 (fine particulate matter) speciation networks, was adapted to direct thermally evolved gases to an electron impact quadrupole mass spectrometer (QMS), creating a TOA-QMS. This approach produces spectra similar to those obtained by the Aerodyne aerosol mass spectrometer (AMS), but the ratios of the mass to charge (m/z) signals differ and must be remeasured using laboratory-generated standards. Linear relationships are found between TOA-QMS signals and ammonium (NH4+), nitrate (NO3?), and sulfate (SO42-) standards. For ambient samples, however, positive deviations are found for SO42-, compensated by negative deviations for NO3?, at higher concentrations. This indicates the utility of mixed-compound standards for calibration or separate calibration curves for low and high ion concentrations. The sum of the QMS signals across all m/z after removal of the NH4+, NO3?, and SO42- signals was highly correlated with the carbon content of oxalic acid (C?H?O?) standards. For ambient samples, the OC derived from the TOA-QMS method was the same as the OC derived from the standard IMPROVE_A TOA method. This method has the potential to reduce complexity and costs for speciation networks, especially for highly polluted urban areas such as those in Asia and Africa.

Implications: Ammonium, nitrate, and sulfate can be quantified by the same thermal evolution analysis applied to organic and elemental carbon. This holds the potential to replace multiple parallel filter samples and separate laboratory analyses with a single filter and a single analysis to account for a large portion of the PM2.5 mass concentration.  相似文献   

4.
The influences of HCO3 ?, Cl?, and other components on the UV/TiO2 degradation of the antineoplastic agents ifosfamide (IFO) and cyclophosphamide (CP) were studied in this work. The results indicated that the presence of HCO3 ?, Cl?, NO3 ?, and SO4 2? in water bodies resulted in lower degradation efficiencies. The half-lives of IFO and CP were 1.2 and 1.1 min and increased 2.3–7.3 and 3.2–6.3 times, respectively, in the presence of the four anions (initial compound concentration = 100 μg/L, TiO2 loading =100 mg/L, anion concentration = 1000 mg/L, and pH = 8). Although the presence of HCO3 ? in the UV/TiO2/HCO3 ? system resulted in a lower degradation rate and less byproduct formation for IFO and CP, two newly identified byproducts, P11 (M.W. = 197) and P12 (M.W. = 101), were formed and detected, suggesting that additional pathways occurred during the reaction of ?CO3 ? in the system. The results also showed that ?CO3 ? likely induces a preferred ketonization pathway. Besides the inorganic anions HCO3 ?, Cl?, NO3 ?, and SO4 2?, the existence of dissolved organic matter in the water has a significant effect and inhibits CP degradation. Toxicity tests showed that higher toxicity occurred in the presence of HCO3 ? or Cl? during UV/TiO2 treatment and within 6 h of reaction time, implying that the effects of these two anions should not be ignored when photocatalytic treatment is applied to treat real wastewater.  相似文献   

5.
The study is aimed at evaluating the potential of immobilized TiO2-based zeolite composite for solar-driven photocatalytic water treatment. In that purpose, TiO2-iron-exchanged zeolite (FeZ) composite was prepared using commercial Aeroxide TiO2 P25 and iron-exchanged zeolite of ZSM5 type, FeZ. The activity of TiO2-FeZ, immobilized on glass support, was evaluated under solar irradiation for removal of diclofenac (DCF) in water. TiO2-FeZ immobilized in a form of thin film was characterized for its morphology, structure, and composition using scanning electron microscopy/energy-dispersive x-ray spectroscopy (SEM/EDX). Diffuse reflectance spectroscopy (DRS) was used to determine potential changes in band gaps of prepared TiO2-FeZ in comparison to pure TiO2. The influence of pH, concentration of hydrogen peroxide, FeZ wt% within the composite, and photocatalyst dosage on DCF removal and conversion efficiency by solar/TiO2-FeZ/H2O2 process was investigated. TiO2-FeZ demonstrated higher photocatalytic activity than pure TiO2 under solar irradiation in acidic conditions and presence of H2O2.  相似文献   

6.
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   

7.
采用电极一SBBR系统去除Cu^2+,考察了电流强度,IA竞争离子(阴离子SO4^2-、NO3^-、CL^-和阳离子Zn^2+、Ph^2+)、初始含Cu^2+量及溶液pH值对除铜效除果的影响。结果表明,当电流强度为40mA时Cu^2+去除率最高为98%。投加阴(SO4^2-、NO3^-、Cl^-)、阳(Zn^2+、Pb^2+)离子均会引起出水Cu^2+浓度的增加,且Cl^-和Ph^2+含量分别为45mg/L和30mg/L时对Cu^2+去除的影响更为显著。进水Cu^2+浓度为30mg/L时,Cu^2+去除率最高为98.48%,当进水Cu^2+≥70mg/L时,出水Cu^2+浓度不能达标。酸性(pH4.0~4.5)与碱性(pH9.0~10.0)条件均不利于Cu^2+的去除,且酸性条件的负面影响更显著.当pH为4.5~7.5时.Cu^2+去除率最高为97.78%。  相似文献   

8.
The photocatalytic reduction of CO2 with H2O was investigated using Cu/TiO2 photocatalysts in aqueous solution. For this purpose, Cu/TiO2 photocatalysts (with 0.2, 0.9, 2, 4, and 6 wt.% of Cu) have been synthesized via sol-gel method. The photocatalysts were extensively characterized by means of inductively coupled plasma optical emission spectrometry (ICP-OES), N2 physisorption (BET), XRD, UV-vis DRS, FT-IR, Raman spectroscopy, TEM-EDX, and photoelectrochemical measurements. The as-prepared photocatalysts contain anatase as a major crystalline phase with a crystallite size around 13 nm. By increasing the amount of Cu, specific surface area and band gap energy decreased in addition to the formation of large agglomeration of CuO. Results revealed that the photocatalytic reduction of CO2 decreased in the presence of Cu/TiO2 in comparison to pure TiO2, which might be associated to the formation of CuO phase acting as a recombination center of generated electron-hole pair. Decreasing of photoactivity can also be connected with a very low position of conduction band of photocatalysts with high Cu content, which makes H2 production necessary for CO2 reduction more difficult.  相似文献   

9.
Lanthanum-modified TiO2 photocatalysts (0.2–1.5 wt% La) were investigated in the methanol decomposition in an aqueous solution. The photocatalysts were prepared by the common sol-gel method followed by calcination. The structural (X-ray diffraction, Raman, X-ray photoelectron spectroscopy), textural (N2 physisorption), and optical properties (diffuse reflectance spectroscopy, photoelectrochemical measurements) of all synthetized nanomaterials were correlated with photocatalytic activity. Both pure TiO2 and La-doped TiO2 photocatalysts proved higher yields of hydrogen in comparison to photolysis. The photocatalyst with optimal amount of lanthanum (0.2 wt% La) showed almost two times higher amount of hydrogen produced at the same time as in the presence of pure TiO2. The photocatalytic activity increased with both increasing photocurrent response and decreasing amount of lattice and surface O species. It has been shown that both direct and indirect mechanisms of methanol photocatalytic oxidation participate in the production of hydrogen. Both direct and indirect mechanisms take part in the formation of hydrogen.  相似文献   

10.

Introduction  

The kinetics of the transformation of ammonia and acid gases into components of PM2.5 has been examined. The interactions of existing aerosols and meteorology with the transformation mechanism have also been investigated. The specific objective was to discern the kinetics for the gas-to-particle conversion processes where the reactions of NH3 with H2SO4, HNO3, and HCl take place to form (NH4)2SO4, NH4NO3, and NH4Cl, respectively, in PM2.5.  相似文献   

11.
In the present study, an activated charcoal (AC) plate was prepared by physical activation method. Its surface was coated with TiO2 nanoparticles by electrophoretic deposition (EPD) method. The average crystallite size of TiO2 nanoparticles was determined approximately 28 nm. The nature of prepared electrode was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and Brunauer–Emmett–Teller (BET) surface area measurement before and after immobilization. The electrosorption and photocatalytic one-stage combined process was investigated in degradation of Lanasol Red 5B (LR5B), and the effect of dye concentration, electrolyte concentration, pH, voltage, and contact time was optimized and modeled using response surface methodology (RSM) approach. The dye concentration of 30 mg L?1, Na2SO4 concentration of 4.38 g L?1, pH of 4, voltage of 250 mV, and contact time of 120 min were determined as optimum conditions. Decolorization efficiency increased in combined process to 85.65 % at optimum conditions compared to 66.03 % in TiO2/AC photocatalytic, 20.09 % in TiO2/AC electrosorption, and 1.91 % in AC photocatalytic processes.  相似文献   

12.
There is global concern about the effects of decabromodiphenyl ether (BDE209) on environmental and public health. The molecular properties, biosorption, degradation, accumulation, and cellular metabolic effects of BDE209 were investigated in this study to identify the mechanisms involved in the aerobic biodegradation of BDE209. BDE209 is initially absorbed by wall teichoic acid and N-acetylglucosamine side chains in peptidoglycan, and then, BDE209 is transported and debrominated through three pathways, giving tri-, hepta-, octa-, and nona-bromodiphenyl ethers. The C–C bond energies decrease as the number of bromine atoms on the diphenyl decreases. Polybrominated diphenyl ethers (PBDEs) inhibit protein expression or accelerate protein degradation and increase membrane permeability and the release of Cl?, Na+, NH4 +, arabinose, proteins, acetic acid, and oxalic acid. However, PBDEs increase the amounts of K+, Mg2+, PO4 3?, SO4 2?, and NO3 ? assimilated. The biosorption, degradation, accumulation, and removal efficiencies when Brevibacillus brevis (1 g L?1) was exposed to BDE209 (0.5 mg L?1) for 7 days were 7.4, 69.5, 16.3, and 94.6 %, respectively.  相似文献   

13.
In this study, we present ∼1 yr (October 1998–September 1999) of 12-hour mean ammonia (NH3), ammonium (NH4+), hydrochloric acid (HCl), chloride (Cl), nitrate (NO3), nitric acid (HNO3), nitrous acid (HONO), sulfate (SO42−), and sulfur dioxide (SO2) concentrations measured at an agricultural site in North Carolina's Coastal Plain region. Mean gas concentrations were 0.46, 1.21, 0.54, 5.55, and 4.15 μg m−3 for HCl, HNO3, HONO, NH3, and SO2, respectively. Mean aerosol concentrations were 1.44, 1.23, 0.08, and 3.37 μg m−3 for NH4+, NO3, Cl, and SO42−, respectively. Ammonia, NH4+, HNO3, and SO42− exhibit higher concentrations during the summer, while higher SO2 concentrations occur during winter. A meteorology-based multivariate regression model using temperature, wind speed, and wind direction explains 76% of the variation in 12-hour mean NH3 concentrations (n=601). Ammonia concentration increases exponentially with temperature, which explains the majority of variation (54%) in 12-hour mean NH3 concentrations. Dependence of NH3 concentration on wind direction suggests a local source influence. Ammonia accounts for >70% of NHx (NHx=NH3+NH4+) during all seasons. Ammonium nitrate and sulfate aerosol formation does not appear to be NH3 limited. Sulfate is primarily associated ammonium sulfate, rather than bisulfate, except during the winter when the ratio of NO3–NH4+ is ∼0.66. The annual average NO3–NH4+ ratio is ∼0.25.  相似文献   

14.
Based on available literature data of [NO2 ], steady-state [·OH], and ·OH generation rate upon nitrate photolysis in environmental aqueous samples under sunlight, the steady-state [·NO2], could be calculated. Interestingly, one to two orders of magnitude more ·NO2 would be formed in photochemical processes in atmospheric water droplets compared to transfer from the gas phase. The relative importance of nitrite oxidation compared to nitrate photolysis as an ·NO2 source would be higher in atmospheric than in surface waters. The calculated levels of ·NO2 could lead to substantial transformation of phenol into nitrophenols in both atmospheric and surface waters.  相似文献   

15.

Impacts of diazinon (O,O-diethyl O-2-isopropyl-6-methylpyrimidin-4-yl phosphorothioate), imidacloprid [1-(6-chloro-3-pyridylmethyl)-N-nitroimidazolidin-2-ylideneamine] and lindane (1,2,3,4,5.6-hexachlorocyclohexane) treatments on ammonium, nitrate, and nitrite nitrogen and nitrate reductase enzyme activities were determined in groundnut (Arachis hypogaea L.) field for three consecutive years (1997 to 1999). Diazinon was applied for both seed- and soil-treatments but imidacloprid and lindane were used for seed treatments only at recommended rates. Diazinon residues persisted for 60 days in both the cases. Average half-lives (t1/2) of diazinon were found 29.3 and 34.8 days respectively in seed and soil treatments. In diazinon seed treatment, NH4 +, NO3 ?, and NO2 ? nitrogen and nitrate reductase activity were not affected. Whereas, diazinon soil treatment indicated significant increase in NH4 +-N in a 1-day sample, which continued until 90 days. Some declines in NO3 ?N were found from 15 to 60 days. Along with this decline, significant increases in NO2 ?N and nitrate reductase activity were found between 1 and 30 days. Imidacloprid and lindane persisted for 90 and 120 days with average half-lives (t1/2) of 40.9 and 53.3 days, respectively. Within 90 days, imidacloprid residues lost by 73.17% to 82.49% while such losses for lindane residues were found 78.19% to 79.86 % within 120 days. In imidacloprid seed-treated field, stimulation of NO3 ?N and the decline in NH4 +NO2 ?-N and nitrate reductase enzyme activity were observed between 15 to 90 days. However, lindane seed treatment indicated significant increases in NH4 +-N, NO2 ?-N and nitrate reductase activity and some adverse effects on NO3 ?N between 15 and 90 days.  相似文献   

16.
Improvement of air quality models is required so that they can be utilized to design effective control strategies for fine particulate matter (PM2.5). The Community Multiscale Air Quality modeling system was applied to the Greater Tokyo Area of Japan in winter 2010 and summer 2011. The model results were compared with observed concentrations of PM2.5 sulfate (SO42-), nitrate (NO3?) and ammonium, and gaseous nitric acid (HNO3) and ammonia (NH3). The model approximately reproduced PM2.5 SO42? concentration, but clearly overestimated PM2.5 NO3? concentration, which was attributed to overestimation of production of ammonium nitrate (NH4NO3). This study conducted sensitivity analyses of factors associated with the model performance for PM2.5 NO3? concentration, including temperature and relative humidity, emission of nitrogen oxides, seasonal variation of NH3 emission, HNO3 and NH3 dry deposition velocities, and heterogeneous reaction probability of dinitrogen pentoxide. Change in NH3 emission directly affected NH3 concentration, and substantially affected NH4NO3 concentration. Higher dry deposition velocities of HNO3 and NH3 led to substantial reductions of concentrations of the gaseous species and NH4NO3. Because uncertainties in NH3 emission and dry deposition processes are probably large, these processes may be key factors for improvement of the model performance for PM2.5 NO3?.
Implications: The Community Multiscale Air Quality modeling system clearly overestimated the concentration of fine particulate nitrate in the Greater Tokyo Area of Japan, which was attributed to overestimation of production of ammonium nitrate. Sensitivity analyses were conducted for factors associated with the model performance for nitrate. Ammonia emission and dry deposition of nitric acid and ammonia may be key factors for improvement of the model performance.  相似文献   

17.
Abstract

Sewage sludge and yard waste compost were used as biofilter materials and tested with respect to their capacity for removing ammonia from air at different water contents. Ammonia removal was measured in biofilters containing compost wetted to different moisture contents ranging from air dry to field capacity (maximum water holding capacity). Filters were operated for 15 days and subsequently analyzed for NH3/NH4 +, NO2 -, and NO3 -. The measured nitrogen species concentration profiles inside the filters were used to calculate ammonia removal rates. The results showed that ammonia removal is strongly dependent on the water content in the filter material. At gravimetric water contents below 0.25 g H2O g solids-1 for the yard waste compost and 0.5 g H2O g solids-1 ammonia removal rates were very low but increased rapidly above these values. The sewage sludge compost filters yielded more than twice the ammonia removal rate observed for yard waste compost likely because of a high initial concentration of nitrifying bacteria originating from the wastewater treatment process and a high air-water interphase surface area that facilitates effective ammonia dissolution and transport to the biofilm.  相似文献   

18.

A process combining catalyzed Fe(0)-carbon microelectrolysis (IC-ME) with activated carbon (AC) adsorption was developed for advanced reclaimed water treatment. Simultaneous nitrate reduction and chemical oxygen demand (COD) removal were achieved, and the effects of composite catalyst (CC) addition, AC addition, and initial pH were investigated. The reaction kinetics and reaction mechanisms were calculated and analyzed. The results showed that CC addition could enhance the reduction rate of nitrate and effectively inhibit the production of ammonia. Moreover, AC addition increased the adsorption capacity of biorefractory organic compounds (BROs) and enhanced the degradation of BRO. The reduction of NO3?–N at different pH values was consistently greater than 96.9%, and NH4+–N was suppressed by high pH. The presence of CC ensured the reaction rate of IC-ME at high pH. The reaction kinetics orders and constants were calculated. Catalyzed iron scrap (IS)-AC showed much better nitrate reduction and BRO degradation performances than IS-AC and AC. The IC-ME showed great potential for application to nitrate and BRO reduction in reclaimed water.

  相似文献   

19.

Pseudomonas sp. Y-5, a strain with simultaneous nitrification and denitrification (SND) capacity, was isolated from the Wuhan Municipal Sewage Treatment Plant. This strain could rapidly remove high concentrations of inorganic nitrogen. Specifically, Pseudomonas sp. Y-5 removed 103 mg/L of NH4+-N in 24 h without nitrate or nitrite accumulation when NH4+-N was its sole nitrogen source. The NH4+-N removal efficiency (RE) was 97.26%, and the average removal rate (RR) was 4.30 mg/L/h. Strain Y-5 also removed NO3?-N and NO2?-N even in aerobic conditions, with average RRs of 4.39 and 4.23 mg/L/h, respectively, and REs of up to 99.34% and 95.81% within 24 h. When cultured in SND medium (SNDM-1), strain Y-5 achieved an NH4+-N RE of up to 97.80% and a total nitrogen (TN) RE of 93.01%, whereas NO3?-N was fully depleted in 48 h. Interestingly, high nitrite concentrations did not inhibit the nitrification capacity of Y-5 when grown in SNDM-2, the RE of NH4+-N and TN reached 96.29% and 94.26%, respectively, and nitrite was consumed completely. Strain Y-5 also adapted well to high concentrations of ammonia (~401.68 mg NH4+-N/L) or organic nitrogen (~315.12 mg TN/L). Our results suggested that Pseudomonas sp. Y-5 achieved efficient simultaneous nitrification and denitrification, thus demonstrating its potential applicability in the treatment of nitrogen-polluted wastewater.

  相似文献   

20.
土壤渗滤介质系统去除雨水径流污染物   总被引:2,自引:0,他引:2  
刘芳  侯立柱 《环境工程学报》2012,6(12):4294-4298
利用昆明当地的土壤在室内填装一个土柱渗滤系统,使用配水浓度模拟昆明市区雨水径流污染物浓度,进行去除雨水径流污染物的实验研究,考察系统对COD、TN、NH4+、NO3^-、NO2^-和TP的去除效果。实验结果表明,该土壤渗滤系统对COD平均去除率为82.04%,对TN的平均去除率为22.64%,对NH;平均去除率为94.26%,但是对NO3^-、NO2^-去除效果较差,对TP平均去除率为96.95%;另外,系统长期运行导致下渗速度降低,出水效果反而变好。  相似文献   

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