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1.
Semiconductor photocatalysis is a solution to issues of environmental pollution and energy shortage because photocatalysis can use solar energy to degrade pollutants. The photocatalytic activity can be improved by using composites of ZnO and other semiconductors. Here, composites of ZnO and polymeric graphite-like C3N4 (g-C3N4) with high photocatalytic activities were prepared by microwave synthesis. Products were characterized by X-ray diffraction, transmission electron microscopy, ultraviolet–visible and Fourier transform infrared spectroscopy. The photocatalytic degradation of Rhodamine B was tested under irradiation from a Xe lamp. Results show that adding graphite-like C3N4 promotes the photocatalytic activity of ZnO. Composites with 1.0 wt% g-C3N4 showed the best photodegradation efficiency, and the reaction average energy was approximately 33.71 kJ mol?1.  相似文献   

2.
Photocatalytic oxidation using semiconductors is one of the advanced oxidation processes for degradation of organic pollutants in water and air. TiO2 is an excellent photocatalyst that can mineralize a large range of organic pollutants such as pesticides and dyes. The main challenge is to improve the efficiency of the TiO2 photocatalyst and to extend TiO2 light absorption spectra to the visible region. A potential solution is to couple TiO2 with a narrow band gap semiconductor possessing a higher conduction band such as bismuth oxide. Therefore, here we prepared Bi2O3/TiO2 heterojunctions by the impregnation method with different Bi/Ti ratio. The prepared composites have been characterized by UV–Vis diffused reflectance spectra and X-ray diffraction. The photocatalytic activity of the heterojunction has been determined from the degradation of orange II under visible and UV light. Results show that Bi2O3/TiO2 heterojunctions are more effective than pure TiO2-anatase under UV-A irradiation, with an optimum for the Bi/Ti ratio of 5 %, for the photocatalytic degradation of Orange II. However, the photocatalytic activity under irradiation at λ higher than 420 nm is not much improved. Under UV–visible radiation, the two semiconductors are activated. We propose a mechanism explaining why our products are more effective under UV–visible irradiation. In this case the charge separation is enhanced because a part of photogenerated electrons from the conduction band of TiO2 will go to the conduction band of bismuth oxide. In this composite, titanium dioxide is the main photocatalyst, while bismuth oxide acts as adsorbent photosensitizer under visible light.  相似文献   

3.
The explosive growth in anthropogenic energy consumption, coupled with the consequent environmental pollution, have been acknowledged as two impending challenges confronting humanity. Photocatalytic CO2 reduction to produce value-added hydrocarbon fuels, by using abundant solar energy and redundant atmospheric CO2, is an innovative way to satisfy global energy requirements whilst simultaneously reducing atmospheric CO2 levels. Although this notion is several decades old, it has unfortunately been lingering in a state of infancy due to inherently poor CO2-to-fuel conversion efficiencies, and the generation of low-value products (e.g., CO, HCHO). These pitfalls hamper this process from any potential commercial breakthrough and are primarily fuelled by the lack of progress in developing high-performance photocatalytic materials. Fortunately, the advent of nanotechnology has recently introduced many promising novel materials for this purpose. Here, we review photocatalysts with proven potential for converting CO2 into methanol, a high-value, energy-dense hydrocarbon fuel that is easily transported using existing pipeline infrastructure. Methanol possesses multifarious applications in the automobile, industrial and petrochemical sector. In addition, the development of direct methanol fuel cells (DMFCs) has introduced the tantalizing prospect of using methanol as a medium for storing solar energy that is easily converted to electricity via DMFCs. As such, methanol is an ideal fuel, with numerous advantages over its counterparts. This article reviews several photocatalysts that have been reported for this environmentally sustainable process of converting CO2 into methanol by photocatalysis. Specifically, the performance enhancement effected by adding dopant atoms, forming heterostructured composites and nanostructures, is investigated in terms of four key areas: (1) enhanced visible light sensitivity, (2) improved adsorption of reactants on the catalytic surface, (3) lowered electron–hole recombination and (4) increased CO2 reduction kinetics. The trends deduced therein are invaluable for researchers developing novel photocatalytic materials, which will utilize sunlight to convert CO2 into methanol with enhanced efficiency, thus ushering in the era of a green methanol-based economy.  相似文献   

4.
Multi-walled carbon nanotubes (MWCNTs)/TiO2 composite photocatalysts with high photoactivity were prepared by sol-gel process and further characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR), and UV-vis absorption spectra. Compared to pure TiO2, the combination of MWCNTs with titania could cause a significant absorption shift toward the visible region. The photocatalytic performances of the MWCNTs/TiO2 composite catalysts were evaluated for the decomposition of Reactive light yellow K-6G (K-6G) and Mordant black 7 (MB 7) azo dyes solution under solar light irradiation. The results showed that the addition of MWCNTs enhanced the adsorption and photocatalytic activity of TiO2 for the degradation of azo dyes K-6G and MB 7. The effect of MWCNTs content, catalyst dosage, pH, and initial dye concentration were examined as operational parameters. The kinetics of photocatalytic degradation of two dyes was found to follow a pseudo-first-order rate law. The photocatalyst was used for seven cycles with photocatalytic degradation efficiency still higher than 98%. A plausible mechanism is also proposed and discussed on the basis of experimental results.  相似文献   

5.
A solution of atrazine in a TiO2 suspension, an endocrine disruptor in natural water, was tentatively treated by microwave-assisted photocatalytic technique. The effects of mannitol, oxygen, humic acid, and hydrogen dioxide on the photodegradation rate were explored. The results could be deduced as follows: the photocatalytic degradation of atrazine fits the pseudo-first-order kinetic well with k = 0.0328 s?1, and ·OH was identified as the dominant reactant. Photodegradation of atrazine was hindered in the presence of humic acid, and the retardation effect increased as the concentration of humic acid increased. H2O2 displayed a significant negative influence on atrazine photocatalysis efficiency. Based on intermediates identified with gas chromatography-mass spectrometry (GC-MS) and Liquid chromatography-mass spectrometry (LC-MS/MS) techniques, the main degradation routes of atrazine are proposed.  相似文献   

6.
In this work, Er3+:YAlO3/TiO2 composite was synthesized by a ultrasonic dispersion and liquid boil method. The Er3+:YAlO3/TiO2 composite and pure TiO2 powder were characterized by XRD. The degradation of different organic dyes was used to evaluate the photocatalytic activity of the Er3+:YAlO3/TiO2 composite. It is found that the photocatalytic activity of Er3+:YAlO3/TiO2 composite is much higher than that for the similar system with only TiO2. Moreover, this Er3+:YAlO3/TiO2 composite provides a new way to take advantage of TiO2 in sewage treatment aspects using solar light.  相似文献   

7.
We have discovered that HNO3 and related species are released from the TiO2 surface into air in the TiO2 photocatalytic oxidation of NO2 (1 ppm) under continuous UV light illumination (1 mW cm−2) by dehumidifying the outlet gas of the reaction and analyzing the recovered condensate liquid by ion chromatography. The origin of the HNO3 recovered in the dehumidifier could not be explained by a simple desorption of HNO3 overproduced on the TiO2 surface. The produced HNO3 must be activated on the TiO2 surface and causing the unidentified reaction.  相似文献   

8.
Fine particulate matter (PM2.5) levels, carbon dioxide (CO2) levels and particle-number concentrations (PNC) were monitored in train carriages on seven routes of the mass transit railway in Hong Kong between March and May 2014, using real-time monitoring instruments. The 8-h average PM2.5 levels in carriages on the seven routes ranged from 24.1 to 49.8 µg/m3, higher than levels in Finland and similar to those in New York, and in most cases exceeding the standard set by the World Health Organisation (25 µg/m3). The CO2 concentration ranged from 714 to 1801 ppm on four of the routes, generally exceeding indoor air quality guidelines (1000 ppm over 8 h) and reaching levels as high as those in Beijing. PNC ranged from 1506 to 11,570 particles/cm3, lower than readings in Sydney and higher than readings in Taipei. Correlation analysis indicated that the number of passengers in a given carriage did not affect the PM2.5 concentration or PNC in the carriage. However, a significant positive correlation (p < 0.001, R 2 = 0.834) was observed between passenger numbers and CO2 levels, with each passenger contributing approximately 7.7–9.8 ppm of CO2. The real-time measurements of PM2.5 and PNC varied considerably, rising when carriage doors opened on arrival at a station and when passengers inside the carriage were more active. This suggests that air pollutants outside the train and passenger movements may contribute to PM2.5 levels and PNC. Assessment of the risk associated with PM2.5 exposure revealed that children are most severely affected by PM2.5 pollution, followed in order by juveniles, adults and the elderly. In addition, females were found to be more vulnerable to PM2.5 pollution than males (p < 0.001), and different subway lines were associated with different levels of risk.  相似文献   

9.
In this study, a new water treatment system that couples (photo-) electrochemical catalysis (PEC or EC) in a microbial fuel cell (MFC) was configured using a stainless-steel (SS) cathode coated with Fe0/TiO2. We examined the destruction of methylene blue (MB) and tetracycline. Fe0/TiO2 was prepared using a chemical reduction-deposition method and coated onto an SS wire mesh (500 mesh) using a sol technique. The anode generates electricity using microbes (bio-anode). Connected via wire and ohmic resistance, the system requires a short reaction time and operates at a low cost by effectively removing 94% MB (initial concentration 20 mg?L–1) and 83% TOC/TOC0 under visible light illumination (50 W; 1.99 mW?cm–2 for 120 min, MFC-PEC). The removal was similar even without light irradiation (MFC-EC). The E Eo of the MFC-PEC system was approximately 0.675 kWh?m–3?order–1, whereas that of the MFC-EC system was zero. The system was able to remove 70% COD in tetracycline solution (initial tetracycline concentration 100 mg?L–1) after 120 min of visible light illumination; without light, the removal was 15% lower. The destruction of MB and tetracycline in both traditional photocatalysis and photoelectrocatalysis systems was notably low. The electron spinresonance spectroscopy (ESR) study demonstrated that ?OH was formed under visible light, and ?O 2 was formed without light. The bio-electricity-activated O2 and ROS (reactive oxidizing species) generation by Fe0/TiO2 effectively degraded the pollutants. This cathodic degradation improved the electricity generation by accepting and consuming more electrons from the bio-anode.
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10.
The concentrations and flux of CO2, 222Radon (Rn), and gaseous elemental mercury (Hg) in soil gas were investigated based on the field measurements in June 2010 at ten sites along the seismic rupture zones produced by the May 12, 2008, Wenchuan M s 8.0 earthquake in order to assess the environmental impact of degassing of CO2, Rn and Hg. Soil gas concentrations of 344 sampling points were obtained. Seventy measurements of CO2, Rn and Hg flux by the static accumulation chamber method were performed. The results of risk assessment of CO2, Rn and Hg concentration in soil gas showed that (1) the concentration of CO2 in the epicenter of Wenchuan M s 8.0 earthquake and north end of seismic ruptures had low risk of asphyxia; (2) the concentrations of Rn in the north segment of seismic ruptures had high levels of radon, Maximum was up to level 4, according to Chinese code (GB 50325-2001); (3) the average geoaccumulation index I geo of soil Hg denoted the lack of soil contamination, and maximum values classified the soil gas as moderately to strongly polluted in the epicenter. The investigation of soil gas CO2, Rn and Hg degassing rate indicated that (1) the CO2 in soil gas was characterized by a mean \(\updelta^{13}C_{CO2}\) of ?20.4 ‰ and by a mean CO2 flux of 88.1 g m?2 day?1, which were in the range of the typical values for biologic CO2 degassing. The maximum of soil CO2 flux reached values of 399 g m?2 day?1 in the epicenter; (2) the soil Rn had higher exhalation in the north segment of seismic ruptures, the maximum reached value of 1976 m Bq m?2 s?1; (3) the soil Hg flux was lower, ranging from ?2.5 to 18.7 n g m?2 h?1 and increased from south to north. The mean flux over the all profiles was 4.2 n g m?2 h?1. The total output of CO2 and Hg degassing estimated along seismic ruptures for a survey area of 18.17 km2 were approximately 0.57 Mt year?1 and 688.19 g year?1. It is recommended that land-use planners should incorporate soil gas and/or gas flux measurements in the environmental assessment of areas of possible risk. A survey of all houses along seismic ruptures is advised as structural measures to prevent the ingress of soil gases, including CO2 and Rn, were needed in some houses.  相似文献   

11.
Biochar has emerged as a universal sorbent for the removal of contaminants from water and soil. However, its efficiency is lower than that of commercially available sorbents. Engineering biochar by chemical modification may improve its sorption efficiency. In this study, conocarpus green waste was chemically modified with magnesium and iron oxides and then subjected to thermal pyrolysis to produce biochar. These chemically modified biochars were tested for NO3 removal efficiency from aqueous solutions in batch sorption isothermal and kinetic experiments. The results revealed that MgO-biochar outperformed other biochars with a maximum NO3 sorption capacity of 45.36 mmol kg?1 predicted by the Langmuir sorption model. The kinetics data were well described by the Type 1 pseudo-second-order model, indicating chemisorption as the dominating mechanism of NO3 sorption onto biochars. Greater efficiency of MgO-biochar was related to its high specific surface area (391.8 m2 g?1) and formation of strong ionic complexes with NO3. At an initial pH of 2, more than 89 % NO3 removal efficiency was observed for all of the biochars. We conclude that chemical modification can alter the surface chemistry of biochar, thereby leading to enhanced sorption capacity compared with simple biochar.  相似文献   

12.
Titanium dioxide photocatalysis for pharmaceutical wastewater treatment   总被引:1,自引:0,他引:1  
Heterogeneous photocatalysis using the semiconductor titanium dioxide (TiO2) has proven to be a promising treatment technology for water purification. The effectiveness of this oxidation technology for the destruction of pharmaceuticals has also been demonstrated in numerous studies. This review highlights recent research on TiO2 photocatalytic treatment applied to the removal of selected pharmaceuticals. The discussions are tailored based on the therapeutic drug classes as the kinetics and mechanistic aspects are compound dependent. These classes of pharmaceuticals were chosen because of their environmental prevalence and potential adverse effects. Optimal operational conditions and degradation pathways vary with different pharmaceutical compounds. The main conclusion is that the use of TiO2 photocatalysis can be considered a state-of-the-art pharmaceutical wastewater treatment methodology. Further studies are, however, required to optimize the operating conditions for maximum degradation of multiple pharmaceuticals in wastewater under realistic conditions and on an industrial scale.  相似文献   

13.
The photocatalytic degradation of a sulfonylurea herbicide, cinosulfuron, has been studied in TiO2 aqueous suspensions. A first order kinetic law was found. The influence of the initial concentration of cinosulfuron and of the initial radiant flux on the kinetics were evaluated. The identification of the intermediate products was based on high performance liquid chromatography coupled with mass spectrometry analyses (HPLC-MS). The mineralization of cinosulfuron was traced using ion chromatography and total organic carbon (TOC) measurements. These results indicate that the photocatalytic degradation of cinosulfuron leads to CO2, NO3 and SO4 2− as final products, and in addition cyanuric acid (C3H3O3N3), confirming previous results on triazinic ring-containing compounds. Electronic Publication  相似文献   

14.
Exposure to airborne particulate matter results in the deposition of millions of particle in the lung; consequently, there is need for monitoring them particularly in indoor environments. Case study was conducted in three different microenvironments, i.e., urban, rural and roadside to examine the elemental bioavailability in fine particulate matter and its potential health risk. The samples were collected on polytetrafluoroethylene filter paper with the help of fine particulate sampler during August–September, 2012. The average mass concentration of PM2.5 was 71.23 µg m?3 (rural), 45.33 µg m?3 (urban) and 36.71 µg m?3 (roadside). Elements in PM2.5 were analyzed by inductively coupled plasma atomic emission spectroscopy. Percentage bioavailability was determined to know the amount of soluble fraction that is actually taken across the cell membrane through inhalation pathway. Cadmium and lead were found to have cancer risk in a risk evaluation using an Integrated Risk Information system.  相似文献   

15.
Discharges of nutrients, urea, dissolved organic matter and heavy metals by a sewage underwater pipeline are analysed in comparison to environmental conditions in a shallow coastal zone. Variable thermo-haline stratifications of the water column and currents in upper (2.62–34.97 cm s?1) and deeper (0.83–10.91 cm s?1) layers drive vertical diffusion and lateral transport of wastewaters. Loads of reactive phosphorus (0.13 tons d?1) and ammonium (1.62 tons d?1) by the pipeline are not negligible compared to the major river loads in the gulf. High concentrations of urea (≤11.51 μmol N dm?3) were found in the area of wastewater release. Ammonium uptake (6.14–534 nmol N dm?3 h?1) strongly exceeded nitrate uptake (0.19–138 nmol N dm?3 h?1), indicating that discharges of ammonium by the pipeline are actively assimilated by plankton community even at low levels of light. Distribution of Zn (≤27.7 ppb), Cu (≤25.6 ppb), Cd (≤0.80 ppb) and Pb (≤13.5 ppb) in the water column and the measurement of their complex-forming capacity in seawater did not indicate a persistent perturbation of the pelagic environment due to heavy metals.  相似文献   

16.
Twenty trace elements in fine particulate matters (i.e., PM2.5) at urban Chengdu, a southwest megacity of China, were determined to study the characteristics, sources and human health risk of particulate toxic heavy metals. This work mainly focused on eight toxic heavy metal elements (As, Cd, Cr, Cu, Mn, Ni, Pb and Zn). The average concentration of PM2.5 was 165.1 ± 84.7 µg m?3 during the study period, significantly exceeding the National Ambient Air Quality Standard (35 µg m?3 in annual average). The particulate heavy metal pollution was very serious in which Cd and As concentrations in PM2.5 significantly surpassed the WHO standard. The enrichment factor values of heavy metals were typically higher than 10, suggesting that they were mainly influenced by anthropogenic sources. More specifically, the Cr, Mn and Ni were slightly enriched, Cu was highly enriched, while As, Cd, Pb and Zn were severely enriched. The results of correlation analysis showed that Cd may come from metallurgy and mechanical manufacturing emissions, and the other metals were predominately influenced by traffic emissions and coal combustion. The results of health risk assessment indicated that As, Mn and Cd would pose a significant non-carcinogenic health risk to both children and adults, while Cr would cause carcinogenic risk. Other toxic heavy metals were within a safe level.  相似文献   

17.
Three metallised azo dyes were investigated under TiO2‐photocatalytic and photosensitised conditions in aqueous buffering solutions. The degradation follows apparent first‐order kinetics. The size and strength of intramolecular conjugation determine the light‐fastness of the investigated dyes. Compared with 1O2 produced in photosensitised process, the more powerful *OH radicals in TiCO2 photocatalytic process are highly reactive towards the investigated azo dyes. And as a result, the TiO2‐photocatalysis makes little less distinction in the degradation kinetic data of the azo dyes compared with the photosensitised degradation of them.  相似文献   

18.
PM2.5 has become an important environmental issue in Taiwan during the past few years. Moreover, electricity increased significantly during the summertime and TTPP generated by coal burning base is the main electricity provider in central Taiwan. Therefore, summer season has become the main research target in this study. The ambient air concentrations of particulate matter PM2.5 and PM10 collected by using VAPS at a mixed characteristic sampling site were studied in central Taiwan. The results indicated that the average daytime PM2.5 and PM10 particulate concentrations were occurred in May and they were 44.75 and 57.77 µg/m3 in this study. The results also indicated that the average nighttime PM2.5 and PM10 particulate concentrations were occurred in June and they were 38.19 and 45.79 µg/m3 in this study. The average PM2.5/PM10 ratios were 0.7 for daytime, nighttime and 24-h sampling periods in the summer for this study. This value was ranked as the lowest ratios when compared to the other seasons in previous study. Noteworthy, the results further indicated that the metallic element Pb has the mean highest concentrations for 24-h, daytime and nighttime sampling periods when compared to those of the other metallic elements (Ni, Cu, Zn and Cd). The average mean highest metallic Pb concentrations in PM10 were 110.7, 203.0 and 207.2 ng/m3 for 24-h, daytime and nighttime sampling periods in this study. And there were 59.53, 105.2 and 106.6 ng/m3 for Pb in PM2.5 for 24-h, daytime and nighttime sampling periods, respectively. Moreover, the results further indicated that mean metallic element Pb concentrations on PM2.5 and PM10 were all higher than those of the other elements for 24 h, day and nighttime.  相似文献   

19.
Visible light is a major fraction of the solar spectrum; however, information on visible light radiation of macrophyte detritus is lacking. In this study, we conducted a microcosm experiment to assess the effects of visible light radiation on degradation of two litter species: Potamogeton malaianus (P. malaianus) and Phragmites australis (Ph. australis). This research represents an investigation of mass loss, microbial activity and nutrients released over a period of 168 days. Overall, we found that visible light radiation had significant effects on litter decomposition, but it did not affect the microbial activities which degrade cellulose and lignin. The decomposition rate order of the three components in P. malaianus and Ph. australis in treatments was: cellulose?>?hemicellulose?>?lignin. The visible light radiation mainly affected the degradation of lignin, which is the primary compound in litter susceptible to photodegradation. The exposure to visible light radiation up to 17.6?Wm?2 stimulated the dissolved organic carbon release and reduced the molecular weight to less reactive. Meanwhile, no obvious difference in nutrient contents (TP, TN, NO3–N, NO2–N, and NH3–N) was observed among different visible light intensities. The results of this study contribute to better understanding of the photochemical behaviour of macrophyte litter in shallow lakes.  相似文献   

20.
Heterogeneous Fenton-like reaction has been extensively investigated to eliminate refractory organic contaminants in wastewater, but it usually shows low catalytic performance due to difficulty in reduction from Fe(III) to Fe(II). In this study, enhanced catalytic efficiency was obtained by employing Cu-doped BiFeO3 as heterogeneous Fenton-like catalysts, which exhibited higher catalytic performance toward the activation of H2O2 for phenol degradation than un-doped BiFeO3. BiFe0.8Cu0.2O3 displayed the best performance, which yielded 91% removal of phenol (10 mg L–1) in 120 min. The pseudo first-order kinetic rate constant of phenol degradation in BiFe0.8Cu0.2O3 catalyzed heterogeneous Fenton-like reaction was 5 times higher than those of traditional heterogeneous Fenton-like catalysts, such as Fe3O4 and goethite. The phenol degradation efficiency could still reach 83% after 4 cycles, which implied the good stability of BiFe0.8Cu0.2O3. The high catalytic activity of BiFe0.8Cu0.2O3 was attributed to the fact that the doping Cu into BiFeO3 could promote the generation of Fe(II) in the catalyst and then facilitate the activation of H2O2 to degrade the organic pollutants.
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