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1.

The present work mainly deals with photocatalytic degradation of a herbicide, erioglaucine, in water in the presence of TiO2 nanoparticles (Degussa P-25) under ultraviolet (UV) light illumination (30 W). The degradation rate of erioglaucine was not so high when the photolysis was carried out in the absence of TiO2 and it was negligible in the absence of UV light. We have studied the influence of the basic photocatalytic parameters such as pH of the solution, amount of TiO2, irradiation time and initial concentration of erioglaucine on the photodegradation efficiency of erioglaucine. A kinetic model is applied for the photocatalytic oxidation by the UV/TiO2 system. Experimental results indicated that the photocatalytic degradation process could be explained in terms of the Langmuir–Hinshelwood kinetic model. The values of the adsorption equilibrium constant, K, and the second order kinetic rate constant, k, were 0.116 ppm? 1 and 0.984 ppm min? 1, respectively. In this work, we also compared the reactivity between the commercial TiO2 Degussa P-25 and a rutile TiO2. The photocatalytic activities of both photocatalysts were tested using the herbicide solution. We have noticed that photodegradation efficiency was different between both of them. The higher photoactivity of Degussa P-25 compared to that of rutile TiO2 for the photodegradation of erioglaucine may be due to higher hydroxyl content, higher surface area, nano-size and crystallinity of the Degussa P-25. Our results also showed that the UV/TiO2 process with Degussa P-25 as photocatalyst was appropriate as the effective treatment method for removal of erioglaucine from a real wastewater. The electrical energy consumption per order of magnitude for photocatalytic degradation of erioglaucine was lower with Degussa P-25 than in the presence of rutile TiO2.  相似文献   

2.
通过X-射线衍射仪(XRD)、扫描电镜(SEM)、透射电镜(TEM)和紫外可见光漫反射谱(UV-vis)对碳纳米管/二氧化钛/壳聚糖复合薄膜的晶体结构和形貌进行表征,以室内空气典型污染物气相苯为模型反应物,研究碳纳米管/二氧化钛/壳聚糖催化薄膜的光催化活性及其对苯的光降解机理。结果表明,制备的碳纳米管/二氧化钛/壳聚糖催化薄膜所具有的良好催化活性归功于碳纳米管、二氧化钛和壳聚糖三者的协调效应;气相苯光降解产生的主要中间产物是乙酸乙酯和十一烷,以及少量的丙烯醛、4-羰基-甲基-苯乙酮、十二烷烃、2,4,-二叔丁基苯酚、二十一烷烃。根据红外光谱分析与GC/MS分析结果,进一步提出了气相苯的降解机理过程。  相似文献   

3.
Abstract

The present work deals with photocatalytic degradation of an organophosphorus pesticide, phosalone, in water in the presence of TiO2 particles under UV light illumination (1000 W). The influence of the basic photocatalytic parameters such as pH of the solution, amount of TiO2, irradiation time, stirring rate, and distance from UV source, on the photodegradation efficiency of phosalone was investigated. The degradation rate of phosalone was not high when the photolysis was carried out in the absence of TiO2 and it was negligible in the absence of UV light. The half-life (DT50) of a 20 ppm aqueous solution of phosalone was 15 min in optimized conditions. The plot of lnC (phosalone) vs. time was linear, suggesting first order reaction (K = 0.0532 min?1). The half-life time of photomineralization in the concentration range of 7.5–20 ppm was 13.02 min. The efficiency of the method was also determined by measuring the reduction of Chemical Oxygen Demand (COD). During the mineralization under optimized conditions, COD decreased by more than 45% at irradiation time of 15 min. The photodegradation of phosalone was enhanced by addition of proper amount of hydrogen peroxide (150 ppm).  相似文献   

4.

Herein improved solar light–driven photocatalytic degradation and mineralization of two emerging pollutants as well as recalcitrant beta blockers propranolol (PR) and atenolol (AT) have been demonstrated by metal-free carbon dot/TiO2 (CDT) composite. Hydrothermally synthesized TiO2 has been decorated with electrochemically synthesized carbon dots (CDs) and was well characterized by various analytical techniques viz. XRD, FTIR, Raman, XPS, UV–visible DRS, FESEM, and TEM. The optimized CDT composite, 2CDT (2 mL carbon dot/TiO2), showed?~?3.45- and?~?1.75-fold enhancement in the photodegradation rate as compared to pristine TiO2 for PR and AT respectively in 1 hour of irradiation along with complete degradation of PR and AT after 3 hours of irradiation. 2CDT exhibited 76% and 80% mineralization of PR and AT in contrast with 62% and 47% observed by pristine TiO2. Further, the major reaction intermediates formed after degradation have been identified by HPLC/MS analysis, confirming more than 99% reduction of the parent compound for both PR and AT. Reusability of the optimized catalyst also showed successful degradation up to 3 cycles, showing reduction abilities of 97%, 95%, and 94% for 1st, 2nd, and 3rd cycle respectively. The enhanced degradation and mineralization efficiency of the 2CDT composite could be attributed to the excellent photosensitizer and electron reservoir properties of the CD along with upconverted photoluminescence behavior. The present study unlocks the possibility of using metal-free, facile CDT composite for effective degradation and mineralization of widely used beta blockers and other pharmaceuticals.

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5.
Roxarsone (3-nitro-4-hydroxyphenylarsonic acid) has been widely used as organic arsenic additive in animal industry. In this study, the adsorption of roxarsone on TiO2 under dark conditions, the photocatalytic decomposition of roxarsone under UV/TiO2, and the possible photocatalytic pathway were investigated. At the initial concentration of 5–35 mg/L, the adsorption of roxarsone fitted well with the pseudo-second-order kinetics. The isotherms analysis showed that the Langmuir model was better than the Freundlich and Dubinin–Radushkevich models for describing the adsorption process. After 7 h of photocatalytic decomposition, a complete disappearance of roxarsone was achieved. The pH value has a significant effect on both adsorption and photocatalytic decomposition of roxarsone. The results of high-performance liquid chromatography-hydride generation-atomic fluorescence spectrometry (HPLC-HG-AFS) and gas chromatography-mass spectrometry (GC/MS) analyses proved the cleavage of the As-C bond during the photocatalytic decomposition process by TiO2 and the intermediates of the decomposition. Based on the results, a possible photocatalytic decomposition pathway was proposed.  相似文献   

6.
Chu W  Rao YF 《Chemosphere》2012,86(11):1079-1086
A comprehensive study of the degradation of monuron, one of the phenylurea herbicides, was conducted by UV-Vis/WO3 process. It was found that hydroxyl radicals played a major role in the decay of monuron while other radicals (e.g. superoxide) and hole might also contribute to the decomposition of monuron. The oxidation path likely plays a major role in the generation of hydroxyl radicals. The effects of initial pH level, initial concentration of monuron, and inorganic oxidants on the performance of UV-Vis/WO3 process were also investigated and optimized. Comparison between monuron decay pathways by UV-Vis/WO3 and UV/TiO2 was conducted. The decay mechanisms, including N-terminus demethylation, dechlorination and direct hydroxylation on benzene ring, were observed to be involved in the oxidation of monuron in these two processes. Sixteen intermediates were identified during the photodegradation of monuron and degradation pathways were proposed accordingly.  相似文献   

7.
1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane (or p,p′-DDT) is one of the most persistent pesticides. It is resistant to breakdown in nature and cause the water contamination problem. In this work, a major objective was to demonstrate the application of N-doped TiO2 in degradation and mineralization of the p,p′-DDT under UV and visible light in aqueous solution. The N-doped TiO2 nanopowders were prepared by a simple modified sol–gel procedure using diethanolamine (DEA) as a nitrogen source. The catalyst characteristics were investigated using XRD, SEM, TEM, and XPS. The adsorption and photocatalytic oxidation of p,p′-DDT using the synthesized N-doped TiO2 under UV and visible light were conducted in a batch photocatalytic experiment. The kinetics and p,p′-DDT degradation performance of the N-doped TiO2 were evaluated. Results show that the N-doped TiO2 can degrade p,p′-DDT effectively under both UV and visible lights. The rate constant of the p,p′-DDT degradation under UV light was only 0.0121 min?1, whereas the rate constant of the p,p′-DDT degradation under visible light was 0.1282 min?1. Under visible light, the 100% degradation of p,p′-DDT were obtained from N-doped TiO2 catalyst. The reaction rate of p,p′-DDT degradation using N-doped TiO2 under visible light was sixfold higher than that under UV light. According to Langmuir-Hinshelwood model, the adsorption equilibrium constant (K) for the N-doped TiO2 under visible light was 0.03078 L mg?1, and the apparent reaction rate constant (k) was 1.3941 mg L?1-min. Major intermediates detected during the p,p′-DDT degradation were p,p′-DDE, o,p′-DDE, p,p′-DDD and p,p′-DDD. Results from this work can be applied further for the breakdown of p,p′-DDT molecule in the real contaminated water using this technology.  相似文献   

8.
采用溶剂热合成法制备了一种新型的汉沙黄/TiO2复合物光催化剂,利用多种手段SEM、XRD、FT-IR对催化剂的样品形貌、结构进行表征。分别以罗丹明B、亚甲基蓝、中性红为目标降解物,考察了可见光下溶液pH值对催化剂的吸附性能和催化活性的影响。结果表明,敏化后的TiO2对光的响应由紫外区扩展到可见区,催化活性优于纯TiO2,对上述3种染料的吸附率分别为19.2%、29.2%和43.2%,降解率分别为98.6%、92.5%和97.8%。制备的汉沙黄/TiO2光催化剂稳定性好,重复使用率高,在印染废水处理中具有很好的应用前景。  相似文献   

9.
Background, aim, and scope  The pulp and paper industry is the sixth largest polluter discharging a variety of gaseous, liquid, and solid wastes into the environment. Effluents from bleached Kraft mill effluents (BKME) are polluting waters to a great extent These effluents cause considerable damage to the receiving waters if discharged untreated since they have high levels of biological oxygen demand (BOD), chemical oxygen demand (COD), chlorinated compounds (measured as AOX), suspended solids (mainly fibers), fatty acids, tannins, resin acids, lignin and its derivatives, sulfur and sulfur compounds, etc. This study aimed to remove adsorbed organic halogen (AOX), total nitrogen, and lignin-degrading products in the wastewater (4,500 m3/h) from the paper mill in the pulp and paper industry, which is discharged to sea from a plant located in western Turkey. Materials and methods  The photocatalytic degradation of AOX, total nitrogen, and chlorinated lignin in BKME have been investigated in different parameters, such as time, H2O2 and TiO2 concentration. In addition, for investigating the effect of chlorine on the removal of lignin, pure lignin solution was prepared in equal amounts to chlorinated lignin degradation products found in BKME. The same experiments were conducted for this solution. Experiments were carried out in photocatalytic reactor made of Pyrex glass. The mercury lamp was used as a radiation source. All irradiation was carried out under constant stirring. The existence of dissolved O2 is an important factor which increases the photocatalytic degradation. Hence, we used an air pump for the aeration of the wastewater solutions. The temperature of the wastewater was controlled and adjusted to 25°C by thermostat pump in conjunction with a cooler. At the end of all experiments, AOX, total nitrogen and lignin concentrations were analyzed according to standard methods. All experiments were performed in duplicate and average values were used. Results and discussion  When the effect of H2O2 and time were investigated, it was observed that the AOX concentration increased from 3.0 to 11.0 mg/L by only UV. However, when H2O2 was added, AOX concentration decreased from approximately 3.0 to 0.0 mg/L. The optimal conditions for the removal of AOX appear to be an initial H2O2 concentration of 20.0 mL/L and reaction time of 50 min. In addition, at the same experiment conditions, it was seen that the total nitrogen concentration decreased from 23.0 to 15.0 mg/L by only UV and by increasing H2O2 concentration, the concentration of 20.0 mL/L H2O2 appears to be optimal (9.0 mg/L). The AOX, total nitrogen and lignin degradation products and pure lignin go through a minimum when the concentration of H2O2 and TiO2 increases at constant pH and UV intensity. The kinetics for the degradation of AOX, total nitrogen and lignin degradation products followed a pseudo-first order law with respect to the products, and the degradation rates (min−1) for the UV/TiO2/H2O2 system were higher than that of the corresponding values for the UV/H2O2 system. Conclusions  The AOX, total nitrogen and lignin concentration go through a minimum when the concentration of H2O2 and TiO2 increases at constant pH and UV intensity. It was found that the UV/TiO2/H2O2 system has proved capable of the degradation of total nitrogen as well as chlorinated and degraded lignin in BKME. Recommendations and perspectives  The photocatalytic process can be considered a suitable alternative for the remove of some compounds from the BKME. Nevertheless, further studies should be carried out to confirm the practical feasibility of BKME. Another result obtained from the study is that pre-purification carried out with UV/TiO2/H2O2 photocatalytic process may constitute an important step for further purification processes such as adsorption, membrane processes, etc.  相似文献   

10.
This work aimed to investigate the effectiveness of ultraviolet (UV) radiation on the degradation of the antimicrobial triclocarban (TCC). We investigated the effects of several operational parameters, including solution pH, initial TCC concentration, photocatalyst TiO2 loading, presence of natural organic matter, and most common anions in surface waters (e.g., bicarbonate, nitrate, and sulfate). The results showed that UV radiation was very effective for TCC photodegradation and that the photolysis followed pseudo-first-order kinetics. The TCC photolysis rate was pH dependent and favored at high pH. A higher TCC photolysis rate was observed by direct photolysis than TiO2 photocatalysis. The presence of the inorganic ions bicarbonate, nitrate, and sulfate hindered TCC photolysis. Negative effects on TCC photolysis were also observed by the addition of humic acid due to competitive UV absorbance. The main degradation products of TCC were tentatively identified by gas chromatograph with mass spectrometer, and a possible degradation pathway of TCC was also proposed.  相似文献   

11.

Heterogeneous photocatalysis is highlighted to treat volatile organic compound (VOC) emission. Then, this work analysed the influence of palladium (Pd) content loaded in TiO2 on n-octane and iso-octane photodegradation. For this, TiO2 was loaded with Pd in different contents: 0.4%, 0.7%, and 1.0%. The samples were characterized, and the photodegradation experiments were conducted by Pd/TiO2/UV process. The characterization analyses showed that the metal presence did not change the catalyst structure or its surface area; however, it reduced the bandgap energy. The photocatalytic results proved that palladium improved n-octane degradation from 62% (pure TiO2) to 92.6% (0.4%Pd/TiO2) and, iso-octane degradation enhanced from 59% (pure TiO2) to 90.6% (0.7%Pd/TiO2); all results were obtained in the space time of 39 s. Therefore, 0.4%Pd/TiO2 and 0.7%Pd/TiO2 showed better oxidation results to degradation n-octane and iso-octane, respectively. The kinetic model of pseudo-first order showed a good fit for the data of both VOCs. Heterogeneous photocatalysis with Pd/TiO2 showed to be an adequate technique to reduce VOCs emission.

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12.
活性炭纤维负载TiO2光催化降解甲醛的影响因素   总被引:1,自引:0,他引:1  
利用自制光催化气体反应器体系,以活性炭纤维负载TiO2作催化剂,在紫外光照射下模拟降解室内污染气体甲醛,测试了活性炭纤维负载TiO2催化剂的催化活性,探讨了紫外光光强、催化剂的酸度、反应器内湿度及反应时间等控制反应的主要因素对甲醛降解率的影响。结果表明,活性炭纤维与TiO2的协同作用大大提高了对甲醛的降解效果;紫外光强增倍对甲醛降解率有一定提高,但提高幅度仅为11.71%;活性炭纤维用pH=5的TiO2溶胶浸泡做催化剂对甲醛的降解效果最好,60 min内降解率达到68.37%;反应器内的湿度为81%甲醛降解率最高,反应60 min后达82.2%;随着反应时间的延长,甲醛降解率的上升幅度不断减小,最高只能达到94.59%。  相似文献   

13.
This study investigated the photocatalytic degradation of acetaminophen (ACT) in synthetic titanium dioxide (TiO2) solution under a visible light (λ >440 nm). The TiO2 photocatalyst used in this study was synthesized via sol–gel method and doped with potassium aluminum sulfate (KAl(SO4)2) and sodium aluminate (NaAlO2). The influence of some parameters on the degradation of acetaminophen was examined, such as initial pH, photocatalyst dosage, and initial ACT concentration. The optimal operational conditions were also determined. Results showed that synthetic TiO2 catalysts presented mainly as anatase phase and no rutile phase was observed. The results of photocatalytic degradation showed that LED alone degraded negligible amount of ACT but with the presence of TiO2/KAl(SO4)2, 95 % removal of 0.10-mM acetaminophen in 540-min irradiation time was achieved. The synthetic TiO2/KAl(SO4)2 presented better photocatalytic degradation of acetaminophen than commercially available Degussa P-25. The weak crystallinity of synthesized TiO2/NaAlO2 photocatalyst showed low photocatalytic degradation than TiO2/KAl(SO4)2. The optimal operational conditions were obtained in pH 6.9 with a dose of 1.0 g/L TiO2/KAl(SO4)2 at 30 °C. Kinetic study illustrated that photocatalytic degradation of acetaminophen fits well in the pseudo-first order model. Competitive reactions from intermediates affected the degradation rate of ACT, and were more obvious as the initial ACT concentration increased.  相似文献   

14.
氮掺杂二氧化钛可见光催化降解曙红Y溶液   总被引:2,自引:1,他引:1  
采用溶胶凝胶法制备了氮掺杂二氧化钛光催化剂,用XRD、SEM、FTIR和粒度分析仪对催化剂进行了表征,并且在可见光作用下对曙红Y溶液进行了光催化降解实验。研究了催化剂的投加量、曙红Y的初始浓度、光照时间和pH对曙红Y溶液的光降解效果。结果表明,以可见光作光源,催化剂的投入量为0.4 g,曙红Y溶液的初始浓度为20 mg/L,光照时间为50 min,pH=4条件下,曙红Y溶液的降解率达98.87%。  相似文献   

15.
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   

16.
Photocatalytic process has shown recently a great potential as an environmental friendly and clean remediation technology for organic pollutants in wastewater. This work described the synthesis of silver-based bimetallic nanoparticles using colloid chemistry and the subsequent immobilization onto titania to form composite photocatalytic materials (titania-supported Ag–Pt nanoparticles). The photocatalysts were characterized by X-ray diffraction, electron microscopy, and nitrogen physisorption. The catalytic activity of the photocatalysts was evaluated by photocatalytic degradation of phenol and 2-chlorophenol (2-CP) in synthetic wastewater solutions. The photocatalytic processes were conducted in a batch photoreactor containing appropriate solutions of phenol and 2-CP with UV irradiation of 450 W. UV-visible spectrophotometer was used for analyzing the concentration of phenol and 2-CP in solutions. Parameters affecting the photocatalytic process such as the solution pH, phenol and 2-CP concentrations, and catalyst concentration were investigated. The results obtained revealed that TiO2-supported Ag/Pt nanoparticles showed a higher activity for UV-photocatalytic degradation of both phenol and 2-CP pollutants in the solution (as compared to the plain rutile TiO2). The photodegradation processes were optimized by the 0.5-g/L catalyst with a pollutant concentration of 50 mg/L for all the samples. Complete degradation for both phenol and 2-CP was achieved after 120 min.  相似文献   

17.
Carbofuran (CBF) removal in a continuous-flow photocatalytic reactor with granular activated carbon supported titanium dioxide (GAC-TiO2) catalyst was investigated. The effects of feed flow rate, TiO2 concentration and addition of supplementary oxidants on CBF removal were investigated. The central composite design (CCD) was used to design the experiments and to estimate the effects of feed flow rate and TiO2 concentration on CBF removal. The outcome of CCD experiments demonstrated that reactor performance was influenced mainly by feed flow rate compared to TiO2 concentration. A second-order polynomial model developed based on CCD experiments fitted the experimental data with good correlation (R2 ~ 0.964). The addition of 1 mL min?1 hydrogen peroxide has shown complete CBF degradation and 76% chemical oxygen demand removal under the following operating conditions of CBF ~50 mg L?1, TiO2 ~5 mg L?1 and feed flow rate ~82.5 mL min?1. Rate constant of the photodegradation process was also calculated by applying the kinetic data in pseudo-first-order kinetics. Four major degradation intermediates of CBF were identified using GC-MS analysis. As a whole, the reactor system and GAC-TiO2 catalyst used could be constructive in cost-effective CBF removal with no impact to receiving environment through getaway of photocatalyst.  相似文献   

18.
针对实际水处理中对催化剂性能的要求,以光催化降解苯酚溶液作为探针反应,考察了玻璃纤维网上负载的TiO2膜催化剂长期使用条件下的稳定性,研究了催化剂在自来水中使用失活后的再生方法。结果表明,经过50次使用之后,膜催化剂120 min反应对苯酚的降解率从100%下降至83%,总体上看,所制催化剂还是具有相当好的稳定性;在反应器中用蒸馏水浸泡配合光催化反应对TiO2膜催化剂进行原位再生是一种可行的再生途径。  相似文献   

19.
Liu H  Liu G  Fan J  Zhou Q  Zhou H  Zhang N  Hou Z  Zhang M  He Z 《Chemosphere》2011,82(1):43-47
Polybrominated biphenyls have been widely used as flameretardants in textile and electronic industries, and additives in plastics. Over the past few decades, much attention has been given to polybrominated biphenyls in the environment and their effects on humans. In this paper, we studied on the degradation of 4,4′-dibromobiphenyl, a typical one of polybrominated biphenyls, through photoelectrocatalytic process with TiO2, Zr/TiO2 and Zr, N/TiO2 nanotube arrays. The results showed that the photoelectrocatalytic process was more efficient than photocatalytic and electrolytic process alone. The results exhibited that the photoelectrocatalytic efficiency was significantly affected by the properties of the catalysts and bias potential, and the highest photoelectrocatalytic degradation rate was achieved with Zr, N/TiO2 at 1 V and the order was Zr, N/TiO2 > Zr/TiO2 > TiO2. The mechanism was also discussed by detecting the changes of pH value, bromine anion, total organic carbon and intermediates during the process.  相似文献   

20.
Fate of pharmaceuticals--photodegradation by simulated solar UV-light   总被引:6,自引:0,他引:6  
Doll TE  Frimmel FH 《Chemosphere》2003,52(10):1757-1769
The fate of pharmaceuticals in surface waters under solar irradiation was investigated. Photodegradation of pharmaceuticals caused by sun irradiation may be of major significance in the natural elimination process. Based on a data compilation from the literature, the lipid lowering agent metabolite clofibric acid, the iodinated X-ray contrast media iomeprol, which contribute to the adsorbable organic halogen compounds, and the antiepileptic drug carbamazepine were selected. The irradiation experiments were carried out in batch experiments with simulated UV–sunlight. The photodegradation of the pharmaceuticals showed a pseudo-first-order kinetics. The objective of this investigation was to demonstrate that the extent of photoinduced degradation of pharmaceuticals can vary significantly for the different pharmaceuticals and it strongly depends on the water constituents present in solution. The influences of different initial pharmaceutical concentrations, the presence of other pharmaceuticals like carbamazepine or clofibric acid and the presence of natural organic matter on the photochemical degradation rate of pharmaceuticals in aqueous solutions were investigated. Analyses of the pharmaceuticals and their photodegradation products were carried out by high performance liquid chromatography with diode-array and fluorescence detection.  相似文献   

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