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1.
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   

2.
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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3.
In this study, FeVO4 was prepared and used as Fenton-like catalyst to degrade orange G (OG) dye. The removal of OG in an aqueous solution containing 0.5 g·L–1 FeVO4 and 15 mmol·L–1 hydrogen peroxide at pH 7.0 reached 93.2%. Similar rates were achieved at pH 5.7 (k = 0.0471 min–1), pH 7.0 (k = 0.0438 min–1), and pH 7.7 (k = 0.0434 min–1). The FeVO4 catalyst successfully overcomes the problem faced in the heterogeneous Fenton process, i.e., the narrow working pH range. The data for the removal of OG in FeVO4 systems containing H2O2 conform to the Langmuir–Hinshelwood model (R2 = 0.9988), indicating that adsorption and surface reaction are the two basic mechanisms for OG removal in the FeVO4–H2O2 system. Furthermore, the irradiation of FeVO4 by visible light significantly increases the degradation rate of OG, which is attributed to the enhanced rates of the iron cycles and vanadium cycles.
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4.
The transformation of the fungicide carbendazim (methyl-2 benzimidazole carbamate) induced by hydroxyl radical generated by the UV photolysis of H2O2 has been studied in dilute aqueous solution. The efficient reaction of hydroxyl radicals with carbendazim led to the rapid degradation of carbendazim. The study of reaction kinetics yielded a second order rate constant of 2.2±0.3 109 M−1 s−1 for HO· radicals with carbendazim. This value is in agreement with a high reactivity of HO· radicals with carbendazim. Most degradation products were identified by high performance liquid chromatography mass spectrometry (HPLC-MS). In the presence of hydrogenocarbonate and carbonate ions, hydroxyl radicals were quenched and in turn carbonate radicals CO3 ·− were formed. Carbonate radicals are indeed known to react efficiently with compounds containing electron-rich sites such as nitrogen or sulfur atoms. The use of a kinetic modelling software gave evidence for the occurrence of such reactions with carbendazim. The second order rate constant of carbonate radical with carbendazim was equal to 6±2 106 M−1 s−1. Electronic Publication  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.
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   

7.
Tetracycline (TC), one of the most common antibiotics, is often poorly bio-degraded in conventional wastewater treatment plants. In this study, the sonocatalytic degradation of TC was investigated using TiO2 nano-particles as catalyst. The effect of pH, initial TC concentrations, reaction times, and H2O2 concentrations were evaluated. The efficacy of ultrasonic irradiation alone in the removal of this pollutant was negligible but removal efficiency increased upon addition of TiO2 up to 250 mg L?1; increase of pH and initial TC concentration attenuated TC degradation. Addition of H2O2 raised the removal efficiency so that complete removal of TC was achieved within 75 min.  相似文献   

8.
Microwave-hydrothermal treatment of persistent and bioaccumulative perfluorooctanoic acid (PFOA) in water with persulfate (S2O 8 2? ) has been found effective. However, applications of this process to effectively remediate PFOA pollution require a better understanding on free-radical scavenging reactions that also take place. The objectives of this study were to investigate the effects of pH (pH = 2.5, 6.6, 8.8, and 10.5), chloride concentrations (0.01?C0.15 mol·L?1), and temperature (60°C, 90°C, and 130°C) on persulfate oxidation of PFOA under microwave irradiation. Maximum PFOA degradation occurred at pH 2.5, while little or no degradation at pH 10.5. Lowering system pH resulted in an increase in PFOA degradation rate. Both high pH and chloride concentrations would result in more scavenging of sulfate free radicals and slow down PFOA degradation. When chloride concentrations were less than 0.04 mol·L?1 at 90°C and 0.06 mol·L?1 at 60°C, presence of chloride ions had insignificant impacts on PFOA degradation. However, beyond these concentration levels, PFOA degradation rates reduced significantly with an increase in chloride concentrations, especially under the higher temperature.  相似文献   

9.
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   

10.
Antibiotic resistance is a serious public health risk that may spread via potable and reclaimed water. Effective disinfection is important for inactivation of antibiotic-resistant bacteria and disruption of antibiotic resistance genes. Ampicillin is a widely prescribed antibiotic but its effectiveness is increasingly undermined by resistance. In this study, changes in ampicillin resistance for Escherichia coli (E. coli) CGMCC 1.1595 were analyzed after exposure to different doses of ultraviolet (UV) or chlorine, and damage incurred by the plasmid encoding ampicillin resistance gene bla TEM-1 was assessed. We reported a greater stability in ampicillinresistant E. coli CGMCC 1.1595 after UV irradiation or chlorination when compared with previously published data for other E. coli strains. UV irradiation and chlorination led to a shift in the mortality frequency distributions of ampicillin-resistant E. coli when subsequently exposed to ampicillin. The ampicillin hemiinhibitory concentration (IC50) without disinfection was 3800 mg·L–1, and an increment was observed after UV irradiation or chlorination. The IC50 of ampicillin-resistant E. coli was 1.5-fold higher at a UV dose of 40 mJ·cm–2, and was 1.4-fold higher when exposed to 2.0 mg·L–1 chlorine. These results indicate that UV irradiation and chlorination can potentially increase the risk of selection for E. coli strains with high ampicillin resistance. There was no evident damage to bla TEM-1 after 1–10 mg Cl2·L–1 chlorination, while a UV dose of 80 mJ·cm–2 yielded a damage ratio for bla TEM-1 of approximately 1.2-log. Therefore, high UV doses are required for effective disruption of antibiotic resistance genes in bacteria.  相似文献   

11.
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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12.
Abstract

A metal-organic framework of iron-doped copper 1,4-benzenedicarboxylate was synthesized and, for the first time, utilized as a heterogeneous photo-Fenton catalyst for degradation of methylene blue dye in aqueous solution under visible light irradiation. The synthesized materials were characterized by scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray diffraction and energy-dispersive X-ray spectroscopy. The influence factors, kinetics, and stability of the synthesized catalysts were investigated in detail. Iron-doped copper 1,4-benzenedicarboxylate showed higher degradation efficiency than pure copper 1,4-benzenedicarboxylate. An almost complete degradation was achieved within 70?min under visible light irradiation at a solution pH of 6, a catalyst loading of 1?g?L?1, a H2O2 dosage of 0.05?mol L?1 and methylene blue concentration of 50?mg?L?1. Recycling studies demonstrated that the iron-doped copper 1,4-benzenedicarboxylate is a promising heterogeneous photo-Fenton catalyst for long-term removal of methylene blue dye from industrial wastewater.  相似文献   

13.
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   

14.
Ammonia has emerged as a promising hydrogen carrier with applications as an energy source in recent years. However, in addition to being toxic, gaseous ammonia is a precursor of secondary inorganic aerosols. The concentration of ambient fine particulate matter (PM2.5) is intrinsically connected to public health. In this study, PM2.5-related health impacts of utilizing ammonia-hydrogen energy in Kanto Region, Japan, were investigated. It was assumed that 20% of the electricity consumption in Kanto Region, the most populated area in Japan, was supplied by ammonia-hydrogen energy. The PM2.5 resulted from incomplete ammonia decomposition was simulated by a chemical transport model: ADMER-PRO (modified version). Based on the incremental PM2.5 concentration, health impacts on the elderly (individuals over 65 years old) were quantitatively evaluated. The ammonia emission in this scenario increased PM2.5 by 11.7% (0.16 μg·m–3·y–1) in winter and 3.5% (0.08 μg ·m–3·y–1) in summer, resulting in 351 premature deaths per year. This study suggests that costeffective emissions control or treatment and appropriate land planning should be considered to reduce the associated health impacts of this type of energy generation. In addition, further in-depth research, including cost-benefit analysis and security standards, is needed.
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15.
A sampling campaign including summer, autumn and winter of 2014 and spring of 2015 was accomplished to obtain the characteristic of chemical components in PM2.5 at three sites of Kunming, a plateau city in South-west China. Nine kinds of water-soluble inorganic ions (WSI), organic and element carbon (OC and EC) in PM2.5 were analyzed by ion chromatography and thermal optical reflectance method, respectively. Results showed that the average concentrations of total WSI, OC and EC were 22.85±10.95 µg·m-3, 17.83±9.57 µg·m-3 and 5.11±4.29 µg·m-3, respectively. They totally accounted for 53.0% of PM2.5. Secondary organic and inorganic aerosols (SOA and SIA) were also assessed by the minimum ratio of OC/EC, nitrogen and sulfur oxidation ratios. The annual average concentrations of SOA and SIA totally accounted for 28.3% of the PM2.5 concentration. The low proportion suggested the primary emission was the main source of PM2.5 in Kunming. However, secondary pollution in the plateau city should also not be ignorable, due to the appropriate temperature and strong solar radiation, which can promote the atmospheric photochemical reactions.
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16.
Titanium dioxide is coated on the surface of MCM-41 wafer through the plasma enhanced chemical vapor deposition (PECVD) method using titanium isopropoxide (TTIP) as a precursor. Annealing temperature is a key factor affecting crystal phase of titanium dioxide. It will transform an amorphous structure to a polycrystalline structure by increasing temperature. The optimum anatase phase of TiO2 which can acquire the best methanol conversion under UV-light irradiation is obtained under an annealing temperature of 700°C for 2 h, substrate temperature of 500°C, 70 mL·min?1 of oxygen flow rate, and 100W of plasma power. In addition, the films are composed of an anatase-rutile mixed phase, and the ratio of anatase to rutile varies with substrate temperature and oxygen flow rate. The particle sizes of titanium dioxide are between 30.3 nm and 59.9 nm by the calculation of Scherrer equation. Under the reaction conditions of 116.8 mg·L-1 methanol, 2.9 mg·L?1 moisture, and 75°C of reaction temperature, the best conversion of methanol with UV-light is 48.2% by using the anatase-rutile (91.3/8.7) mixed phase TiO2 in a batch reactor for 60 min. While under fluorescent light irradiation, the best photoactivity appears by using the anatase-rutile (55.4/44.6) mixed phase TiO2 with a conversion of 40.0%.  相似文献   

17.
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   

18.
DN322p, an offspring of Aeromonas hydrophila DN322, has the capacity to adsorb and decolorize triphenylmethane dyes in wastewater simultaneously. As a common triphenylmethane dye, crystal violet (CV) was chosen to test the decolorization characteristics of DN322p. Within 0.5 h, the strain DN322p adsorbed a large amount of CV, producing a deep-colored cell pellet and colorless supernatant. The colors of the cell pellet and supernatant lightened over time. The supernatant and dichloromethane extract of the cell pellet both showed conspicuous CV and leuco CV (LCV) characteristic absorbance peaks at 590 nm and 260 nm, respectively, in the UV-vis spectral analysis. This finding indicated that the DN322p cells can adsorb the two dyes. A 99% (w/w) decolorization rate was achieved within 2.5 h with shaking at 30°C for 50 mg CV·L?1. High Performance Liquid Chromatography (HPLC) analysis of the dichloromethane extract of the supernatant and cell pellet confirmed that CV was mainly converted into its leuco form. Dead cells had a similar adsorption capacity with living cells. About 90% of CV in the dye solution (50 mg·L?1) was removed by autoclaved cells with an optical delnsity at 600 nm (OD600) above 1.0.  相似文献   

19.
Oxidation of aldehydes to carboxylic acids is a major reaction. Conventionally, this reaction is carried out with oxidants and metal catalysts, thus producing unwanted metal waste. Recently, aqueous media have been used as an alternative for toxic organic solvents. Here, we tested the clathrate-structured, neutral hydrogen peroxide adduct 4Na2SO4·2H2O2·NaCl for the oxidation of aldehydes to acids in aqueous solution. We found that various aromatic, heteroaromatic and aliphatic aldehydes were selectively oxidized to corresponding acids in 70–98% yields. This simple acid–base treatment allows to separate easily the acid product in high purity without any organic solvent. Moreover, the adduct is produced using 25% H2O2, with inexpensive sodium sulphate, Na2SO4, and sodium chloride, NaCl. The adduct is a non-toxic white crystalline solid, readily soluble in water, and easy to handle.  相似文献   

20.
A pot experiment was conducted to examine the influence of potassium (K) fertilizer (K2SO4) application on the phytoavailability and speciation distribution of cadmium (Cd) and lead (Pb) in soil. Spring wheat (Triticum aestivum L.) was selected as the test plant. There were seven treatments including single and combined contamination of Cd and Pb. CdCl2·2.5 H2O and Pb(NO3)2 were added to the soil at the following dosages: Cd + Pb = 0.00 + 0.00, 5.00 + 0.00, 25.0 + 0.00, 0.00 + 500, 0.00 + 1000, 5.00 + 500 and 25.0 + 1000 mg kg−1, denoted by CK, T1, T2, T3, T4, T5 and T6, respectively. The K fertilizer had five levels: 0.00, 50.0, 100, 200 and 400 mg K2O kg−1 soil, denoted by K0, K1, K2, K3 and K4, respectively. The results showed that the K fertilizer promoted the dry weight (DW) of wheat in all treatments and alleviated the contamination by Cd and Pb. The application of K2SO4 reduced the uptake of Cd in different parts including roots, haulms and grains of wheat; the optimum dosage was the K2 level. K supply resulted in a significant (P < 0.05) decrease in the soluble plus exchangeable (SE) fraction of Cd and there was a negative correlation (not significant, P > 0.05) between the levels of K and the SE fraction of Cd in soil. The application of the K fertilizer could obviously restrain the uptake of Pb by wheat and there were significant (P < 0.05) negative correlations between the concentrations of Pb in grains and the levels of K in soil. K supply resulted in a decrease in the SE fraction of Pb (except the K1 level) from the K0 to K4 levels. At the same time, the application of the K fertilizer induced a significant (P < 0.05) decrease in the weakly specifically adsorbed (WSA) fraction of Pb and a significant (P < 0.05) increase in the bound to Fe–Mn oxides (OX) fraction of Pb. At different K levels, the concentration of Pb in the roots, haulms and grains had a positive correlation with the SE (not significant, P > 0.05) and WSA (significant, P < 0.05) fractions of Pb in the soil. All the K application levels in this experiment reduced the phytoavailability of Cd and Pb. Thus, it is feasible to apply K fertilizer (K2SO4) to alleviate contamination by Cd and/or Pb in soil. Moreover, the level of K application should be considered to obtain an optimal effect with the minimum dosage.  相似文献   

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