首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 31 毫秒
1.
Graphene electrodes (Ti/Gr) were prepared by depositing Gr sheets on Ti substrate, followed by an annealing process for enhancing the adhesion strength. Electrochemical impedance spectroscopies and X-ray dif- fraction patterns displayed that the electrochemical behavior of Ti/Gr electrodes can be improved due to the generation of TiO2 layer at Ti-Gr interface during the annealing process. The palladized Gr electrodes (Ti/Gr/Pd) were prepared by electrochemical depositing Pd nanoparticles on Gr sheets. The debromination ability of Ti/Gr/Pd electrodes was investigated using BDE-47 as a target pollutant with various bias potentials. The results indicated that the BDE-47 degradation rates on Ti/Gr/Pd electrodes increased with the negative bias potentials from 0V to -0.5 V (vs. SCE). Almost all of the BDE-47 was removed in the debromination reaction on the Ti/Gr/Pd electrode at - 0.5 V for 3 h, and the main product was diphenyl ethers, meaning it is promising to debrominate completely using the Ti/Gr/Pd electrode. Although the debromination rate was slightly slower at -0.3 V than that under -0.5 V, the current efficiency at -0.3 V was higher, because the electrical current acted mostly on BDE-47 rather than on water.  相似文献   

2.
• Bi doping in TiO2 enhanced the separation of photo-generated electron-hole. • The performance of photocatalytic degradation of MC-LR was improved. • Coexisting substances have no influence on algal removal performance. • The key reactive oxygen species were h+ and OH in the photocatalytic process. The increase in occurrence and severity of cyanobacteria blooms is causing increasing concern; moreover, human and animal health is affected by the toxic effects of Microcystin-LR released into the water. In this paper, a floating photocatalyst for the photocatalytic inactivation of the harmful algae Microcystis aeruginosa (M. aeruginosa) was prepared using a simple sol-gel method, i.e., coating g-C3N4 coupled with Bi-doped TiO2 on Al2O3-modified expanded perlite (CBTA for short). The impact of different molar ratios of Bi/Ti on CBTA was considered. The results indicated that Bi doping in TiO2 inhibited photogenerated electron-hole pair recombination. With 6 h of visible light illumination, 75.9% of M. aeruginosa (initial concentration= 2.7 × 106 cells/L) and 83.7% of Microcystin-LR (initial concentration= 100 μg/L) could be removed with the addition of 2 g/L CBTA-1% (i.e., Bi/Ti molar ratio= 1%). The key reactive oxygen species (ROSs) in the photocatalytic inactivation process are h+ and OH. The induction of the Bi4+/Bi3+ species by the incorporation of Bi could narrow the bandgap of TiO2, trap electrons, and enhance the stability of CBTA-1% in the solutions with coexisting environmental substances.  相似文献   

3.
GO/TiO2 membrane was prepared by assembling GO nanosheets and TiO2 nanotubes. The intercalation of TiO2 nanotubes enlarged the space of GO interlayers and modified the surface morphology. Hydrophilic/underwater superoleophobic property of GO/TiO2 membrane was obtained. Water permeability, hydrophilicity, oleophobicity and antifouling ability of GO-based membrane were all enhanced by intercalating TiO2 nontubes. Membrane technology for oil/water separation has received increasing attention in recent years. In this study, the hydrophilic/underwater superoleophobic membrane with enhanced water permeability and antifouling ability were fabricated by synergistically assembling graphene oxide(GO) nanosheets and titanium dioxide (TiO2) nanotubes for oil/water separation. GO/TiO2 membrane exhibits hydrophilic and underwater superoleophobic properties with water contact angle of 62° and under water oil contact angle of 162.8°. GO/TiO2 membrane shows greater water permeability with the water flux up to 531 L/(m2·h·bar), which was more than 5 times that of the pristine GO membrane. Moreover, GO/TiO2membrane had excellent oil/water separation efficiency and anti-oil-fouling capability, as oil residual in filtrate after separation was below 5 mg/L and flux recovery ratios were over 80%.The results indicate that the intercalation of TiO2 nanotubes into adjacent GO nanosheets enlarged the channel structure and modified surface topography of the obtained GO/TiO2 membranes, which improved the hydrophilicity, permeability and anti-oil-fouling ability of the membranes, enlightening the great prospects of GO/TiO2 membrane in oil-water treatment.  相似文献   

4.
ZnO/TiO2 composites were synthesized by using the solvothermal method and ultrasonic precipitation followed by heat treatment in order to investigate their photocatalytic degradation of methyl orange (MO) in aqueous suspension under UV irradiation. The composition and surface structure of the catalyst were characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FE-SEM), and transmission electron microscopy (TEM). The degradation efficiencies of MO at various pH values were obtained. The highest degradation efficiencies were obtained before 30min and after 60min at pH 11.0 and pH 2.0, respectively. A sample analysis was conducted using liquid chromatography coupled with electrospray ionization ion-trap mass spectrometry. Six intermediates were found during the photocatalytic degradation process of quinonoid MO. The degradation pathway of quinonoid MO was also proposed.  相似文献   

5.
The aim of this study was to identify the intermediates in clofibric acid degradation under various advanced oxidation processes, namely ultraviolet (UV), UV/H2O2, vacuum ultraviolet (VUV), VUV/H2O2, and solar/TiO2 processes, as well as to assess the toxicity of these intermediates. Eleven intermediates have been detected by gas chromatography-mass spectrometer, most of which were reported for the first time to our best knowledge. Combining the evolution of the dissolved organic carbon, Cl- and specific ultraviolet absorption at 254 nm, it could be deduced that cleavage of aromatic ring followed by dechlorination was the mechanism in solar/TiO2 process, while dechlorination happened first and accumulation of aromatic intermediates occurred in the other processes. Different transformation pathways were proposed for UV-, VUV-assisted and solar/TiO2 processes, respectively. The acute toxicity was evaluated by means of Photobacterium phosphoreum T3 spp. bioassay. It was believed that aromatic intermediates increased the toxicity and the ring-opening pathway in solar/TiO2 process could relieve the toxicity.  相似文献   

6.
The effect of ion-doping on TiO2 nanotubes were investigated to obtain the optimal TiO2 nanotubes for the effective decomposition of humic acids (HA) through O3/UV/ion-doped TiO2 process. The experimental results show that changing the calcination temperature, which changed the weight fractions of the anatase phase, the average crystallite sizes, the Brunauer-Emmett-Teller surface area, and the energy band gap of the catalyst, affected the photocatalytic activity of the catalyst. The ionic radius, valence state, and configuration of the dopant also affected the photocatalytic activity. The photocatalytic activities of the catalysts on HA removal increased when Ag+, Al3+, Cu2+, Fe3+, V5+, and Zn2+ were doped into the TiO2 nanotubes, whereas such activities decreased as a result of Mn2+- and Ni2+-doping. In the presence of 1.0 at.% Fe3+-doped TiO2 nanotubes calcined at 550°C, the removal efficiency of HA was 80% with a pseudo-first-order rate constant of 0.158 min−1. Fe3+ in TiO2 could increase the generation of ·OH, which could remove HA. However, Fe3+ in water cannot function as a shallow trapping site for electrons or holes.  相似文献   

7.
● TiO2/ZSM-11 was prepared by a facile solid state dispersion method. ● Mechanism for photocatalytic degradation of dyes was investigated. ● Both experimental and MD simulations were conducted. ● Chemisorption instead of electrostatic interaction played a critical role. Photocatalytic degradation is a promising way to eliminate dye contaminants. In this work, a series of TiO2/ZSM-11 (TZ) nanocomposites were prepared using a facile solid state dispersion method. Methyl orange (MO), methylene blue (MB), and rhodamine B (RhB) were intentionally chosen as target substrates in the photocatalytic degradation reactions. Compared to pristine TiO2, negative effect was observed on MO degradation while promoted kinetics were collected on MB and RhB over TZ composites. Moreover, a much higher photocatalytic rate was interestingly achieved on RhB than MB, which indicated that a new factor has to be included other than the widely accepted electrostatic interaction mechanism to fully understand the selective photodegradation reactions. Systematic characterizations showed that TiO2 and ZSM-11 physically mixed and maintained both the whole framework and local structure without chemical interaction. The different trends observed in surface area and the photo-absorption ability of TZ composites with reaction performance further excluded both as the promotion mechanism. Instead, adsorption energies predicted by molecular dynamics simulations suggested that differences in the adsorption strength played a critical role. This work provided a deep mechanistic understanding of the selective photocatalytic degradation of dyes reactions, which helps to rationally design highly efficient photocatalysts.  相似文献   

8.
李明玉  曾凡银  房献宝  王君  宋琳 《生态环境》2010,19(10):2474-2478
用热氧化法制备了TiO2/Ti薄膜电极,并用XRD和AFM对TiO2/Ti薄膜电极的晶形和表面形貌进行了表征。结果表明:热氧化法制备的TiO2主要为锐钛型纳米颗粒,直径在40 nm左右。设计了一种新型双槽光电化学反应器,用于废水的处理。以热氧化法制备的TiO2/Ti薄膜电极为阳极进行光电催化反应,同时以石墨电极为阴极用于产生双氧水,并与紫外光组成UV/H2O2体系。考察了双槽反应器中活性艳红X-3B在不同条件下的降解效果。降解结果表明:在新型反应器的阴阳两极槽中,活性艳红不仅在TiO2/Ti阳极槽中被降解,而且在石墨阴极槽中也得到降解;活性艳红在酸性条件下的降解效果最好;相对于单纯的电化学氧化和光催化,光电化学协同作用对X-3B的降解效果最好。  相似文献   

9.
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   

10.
• PANI/Ti(OH)n(4n)+ exhibited excellent adsorption capacity and reusability. • Adsorption sites of Cr(VI) were hydroxyl, amino/imino group and benzene rings. • Sb(V) was adsorbed mainly through hydrogen bonds and Ti-O-Sb. • The formation of Cr-O-Sb in dual system demonstrated the synergistic adsorption. • PANI/TiO2 was a potential widely-applied adsorbent and worth further exploring. Removal of chromium (Cr) and antimony (Sb) from aquatic environments is crucial due to their bioaccumulation, high mobility and strong toxicity. In this work, a composite adsorbent consisting of Ti(OH)n(4n)+ and polyaniline (PANI) was designed and successfully synthesized by a simple and eco-friendly method for the uptake of Cr(VI) and Sb(V). The synthetic PANI/TiO2 composites exhibited excellent adsorption capacities for Cr(VI) and Sb(V) (394.43 mg/g for Cr(VI) and 48.54 mg/g for Sb(V)), wide pH applicability and remarkable reusability. The adsorption of Cr(VI) oxyanions mainly involved electrostatic attraction, hydrogen bonding and anion-π interactions. Based on X-ray photoelectron spectroscopy and FT-IR analysis, the adsorption sites were shown to be hydroxyl groups, amino/imino groups and benzene rings. Sb(V) was adsorbed mainly through hydrogen bonds and surface complexation to form Ti-O-Sb complexes. The formation of Cr-O-Sb in the dual system demonstrated the synergistic adsorption of Cr(VI) and Sb(V). More importantly, because of the different adsorption sites, the adsorption of Cr(VI) and Sb(V) occurred independently and was enhanced to some extent in the dual system. The results suggested that PANI/TiO2 is a promising prospect for practical wastewater treatment in the removal of Cr(VI) and Sb(V) from wastewater owing to its availability, wide applicability and great reusability.  相似文献   

11.
Fe2O3-CeO2-Bi2O3/γ-Al2O3, an environmental friendly material, was investigated. The catalyst exhibited good catalytic performance in the CWAO of cationic red GTL. The apparent activation energy for the reaction was 79 kJ·mol−1. HO2· and O2· appeared as the main reactive species in the reaction. The Fe2O3-CeO2-Bi2O3/γ-Al2O3 catalyst, a novel environmental-friendly material, was used to investigate the catalytic wet air oxidation (CWAO) of cationic red GTL under mild operating conditions in a batch reactor. The catalyst was prepared by wet impregnation, and characterized by special surface area (BET measurement), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The Fe2O3-CeO2-Bi2O3/γ-Al2O3 catalyst exhibited good catalytic activity and stability in the CWAO under atmosphere pressure. The effect of the reaction conditions (catalyst loading, degradation temperature, solution concentration and initial solution pH value) was studied. The result showed that the decolorization efficiency of cationic red GTL was improved with increasing the initial solution pH value and the degradation temperature. The apparent activation energy for the reaction was 79 kJ·mol1. Hydroperoxy radicals (HO2·) and superoxide radicals (O2·) appeared as the main reactive species upon the CWAO of cationic red GTL.  相似文献   

12.
Polybrominated diphenyl ethers (PBDEs) have been widely used as fire-retardants. Due to their high production volume, widespread usage, and environmental persistence, PBDEs have become ubiquitous contaminants in various environments.Nanoscale zero-valent iron (ZVI) is an effective reductant for many halogenated organic compounds. To enhance the degradation efficiency, ZVI/Palladium bimetallic nanoparticles (nZVI/Pd) were synthesized in this study to degrade decabromodiphenyl ether (BDE209) in water. Approximately 90% of BDE209 was rapidly removed by nZVI/Pd within 80 min, whereas about 25% of BDE209 was removed by nZVI. Degradation of BDE209 by nZVI/Pd fits pseudo-first-order kinetics. An increase in pH led to sharply decrease the rate of BDE209 degradation. The degradation rate constant in the treatment with initial pH at 9.0 was more than 6.8 × higher than that under pH 5.0. The degradation intermediates of BDE209 by nZVI/Pd were identified and the degradation pathways were hypothesized. Results from this study suggest that nZVI/Pd may be an effective tool for treating polybrominated diphenyl ethers (PBDEs) in water.  相似文献   

13.
采用水热合成-浸渍法制备锌掺杂TiO2纳米管(Zn-TiO2纳米管),透射电镜照片显示Zn-TiO2纳米管为两端开口形貌均一的中空管状结构,管径约6~8 nm,壁厚约1 nm,长度约50~200 nm。研究了Zn-TiO2纳米管对甲基橙的光催化性能,结果表明:掺杂适量锌提高了TiO2纳米管对甲基橙的光催化降解性能,0.4%Zn-TiO2纳米管的光催化性能最佳。同时还探讨了Zn-TiO2纳米管用量和初始pH值等因素对光催化降解甲基橙的影响,结果显示Zn-TiO2纳米管能有效地降解甲基橙。随着光催化反应进行,CODCr去除率和脱色率变化规律不完全相同,可能是由于芳基和烷基降解速率不同所致。  相似文献   

14.
• A novel and multi-functional clay-based oil spill remediation system was constructed. • TiO2@PAL functions as a particulate dispersant to break oil slick into tiny droplets. • Effective dispersion leads to the direct contact of TiO2 with oil pollutes directly. • TiO2 loaded on PAL exhibits efficient photodegradation for oil pollutants. • TiO2@PAL shows a typical dispersion-photocatalysis synergistic remediation. Removing spilled oil from the water surface is critically important given that oil spill accidents are a common occurrence. In this study, TiO2@Palygorskite composite prepared by a simple coprecipitation method was used for oil spill remediation via a dispersion-photodegradation synergy. Diesel could be efficiently dispersed into small oil droplets by TiO2@Palygorskite. These dispersed droplets had an average diameter of 20–30 mm and exhibited good time stability. The tight adsorption of TiO2@Palygorskite on the surface of the droplets was observed in fluorescence and SEM images. As a particulate dispersant, the direct contact of TiO2@Palygorskite with oil pollutants effectively enhanced the photodegradation efficiency of TiO2 for oil. During the photodegradation process, •O2and •OH were detected by ESR and radical trapping experiments. The photodegradation efficiency of diesel by TiO2@Palygorskite was enhanced by about 5 times compared with pure TiO2 under simulated sunlight irradiation. The establishment of this new dispersion-photodegradation synergistic remediation system provides a new direction for the development of marine oil spill remediation.  相似文献   

15.
We examined influence of phosphate on transport of TiO2 NPs in soil. Deposition was reduced at higher pH and by adsorption of phosphate in soil. Release was more for NPs initially deposited at higher pH. Release was more for NPs initially deposited in the presence of phosphate. Surface roughness and charge heterogeneity play a role in the deposition/ release. The widespread use of TiO2 nanoparticles (NPs) makes inevitable their release into the soil. Phosphate is also widespread within soil, and is likely copresent with TiO2 NPs. However, the influence of phosphate on deposition/release— and thereby on transport— of TiO2 NPs in soil is yet to be elucidated. In this study we conducted saturated column experiments to systematically examine the transport of TiO2 NPs in soil amended with phosphate at different ionic strengths (ISs) (1, 10, 100 mmol/L NaCl) and pHs (4 and 9). Results show that the deposition of TiO2 NPs decreased with decreasing IS, increasing pH, and when soil absorbed phosphate. These observations are qualitatively in agreement with Derjaguin-Landau-Verwey-Overbeek (DLVO) interaction energy calculations, because the repulsive energy barrier is larger and secondary minimum depth is smaller at a lower IS, higher pH, and in the presence of phosphate. Accordingly, both primary- and secondary-minimum deposition were inhibited. Interestingly, although the deposition was less at higher pH and in the presence of phosphate, the subsequent spontaneous detachment and detachment by reduction of solution IS in these cases were greater. In addition, the presence of phosphate in the solution can cause a small quantity of attached TiO2 NPs to detach, even without perturbations of physical and chemical conditions. Our study was the first to investigate the influence of phosphate on detachment of TiO2 NPs and the results have important implication for accurate prediction of fate and transport of TiO2 NPs in subsurface environments.  相似文献   

16.
● MnO x /Ti flow-through anode was coupled with the biofilm-attached cathode in ECBR. ● ECBR was able to enhance the azo dye removal and reduce the energy consumption. ● MnIV=O generated on the electrified MnO x /Ti anode catalyzed the azo dye oxidation. ● Aerobic heterotrophic bacteria on the cathode degraded azo dye intermediate products. ● Biodegradation of intermediate products was stimulated under the electric field. Dyeing wastewater treatment remains a challenge. Although effective, the in-series process using electrochemical oxidation as the pre- or post-treatment of biodegradation is long. This study proposes a compact dual-chamber electrocatalytic biofilm reactor (ECBR) to complete azo dye decolorization and mineralization in a single unit via anodic oxidation on a MnOx/Ti flow-through anode followed by cathodic biodegradation on carbon felts. Compared with the electrocatalytic reactor with a stainless-steel cathode (ECR-SS) and the biofilm reactor (BR), the ECBR increased the chemical oxygen demand (COD) removal efficiency by 24 % and 31 % (600 mg/L Acid Orange 7 as the feed, current of 6 mA), respectively. The COD removal efficiency of the ECBR was even higher than the sum of those of ECR-SS and BR. The ECBR also reduced the energy consumption (3.07 kWh/kg COD) by approximately half compared with ECR-SS. The advantages of the ECBR in azo dye removal were attributed to the synergistic effect of the MnOx/Ti flow-through anode and cathodic biofilms. Catalyzed by MnIV=O generated on the MnOx/Ti anode under a low applied current, azo dyes were oxidized and decolored. The intermediate products with improved biodegradability were further mineralized by the cathodic aerobic heterotrophic bacteria (non-electrochemically active) under the stimulation of the applied current. Taking advantage of the mutual interactions among the electricity, anode, and bacteria, this study provides a novel and compact process for the effective and energy-efficient treatment of azo dye wastewater.  相似文献   

17.
利用机械球磨法制备了零价镁/石墨(ZVMg/C)材料,并将其用于水溶液中三氯乙烯(TCE)的降解.研究通过SEM、BET和XRD等分析手段解析了ZVMg/C的表面形态结构和成分组成;采用正交实验方法优化了ZVMg/C的制备参数,比较了石墨含量对材料性能的影响;并考察了ZVMg/C投加量、溶液初始pH和地下水中常见阴(C...  相似文献   

18.
TiO2 supported on active carbon fiber (TiO2/ACF), an absorbable photocatalyst, is a new kind of material applied in air purification. In this paper, the influence of environmental temperature (T) and relative humidity (RH) on the gas-solid adsorption of toluene and the photocatalytic oxidation (PCO) efficiency of adsorbed toluene on TiO2/ACF were studied, and then, the purification capability of TiO2/ACF was estimated. PCO results showed that although the PCO efficiency increased under high RH and T levels, the amount of adsorption of toluene decreased. Moreover, quantitative analysis results of intermediates indicated that more environmental risk emerged when PCO of toluene was carried out at higher environmental T and RH levels because more toxic intermediates would be accumulated on the TiO2/ACF. So, it is significant to control the environmental T and RH conditions in the application of the PCO technique. T = 25°C and RH = 30% is the optimal condition for purifying toluene in our experimental system.  相似文献   

19.
CNT-TiO2 composite is used to activate PMS under UV-light assistance. Superior performance is due to the enhanced electron-transfer ability of CNT. SO4, •OH and 1O2 play key roles in the degradation of organic pollutants. In this work, a UV-light assisted peroxymonosulfate (PMS) activation system was constructed with the composite catalyst of multi-walled carbon nanotubes (CNT) - titanium dioxide (TiO2). Under the UV light irradiation, the photoinduced electrons generated from TiO2 could be continuously transferred to CNT for the activation of PMS to improve the catalytic performance of organic pollutant degradation. Meanwhile, the separation of photoinduced electron-hole pairs could enhance the photocatalysis efficiency. The electron spin resonance spectroscopy (EPR) and quenching experiments confirmed the generation of sulfate radical (SO4), hydroxyl radical (•OH) and singlet oxygen (1O2) in the UV/PMS/20%CNT-TiO2 system. Almost 100% phenol degradation was observed within 20 min UV-light irradiation. The kinetic reaction rate constant of the UV/PMS/20%CNT-TiO2 system (0.18 min1) was 23.7 times higher than that of the PMS/Co3O4 system (0.0076 min1). This higher catalytic performance was ascribed to the introduction of photoinduced electrons, which could enhance the activation of PMS by the transfer of electrons in the UV/PMS/CNT-TiO2 system.  相似文献   

20.
蒋焦  凌霄  何明磊  周明明 《环境化学》2021,40(2):653-661
以空气扩散阴极、纯铂阳极和紫外灯构建了阴阳极成对耦合紫外光辅助电催化的体系,并系统地研究了电流密度、阳极SO42-浓度以及毒死蜱初始浓度对毒死蜱降解效果的影响.结果表明,当阴极/阳极的电流密度为45/450 mA·cm-2,阳极SO42-浓度为1.0 mol·L-1,毒死蜱初始浓度为25 mg·L-1时,反应60 min后毒死蜱降解率可达99%.对阴极产物的红外分析结果表明,毒死蜱降解后结构中的吡啶环和PS被破坏,产生亚硝氮和正磷酸盐,毒性得到减弱.通过对比阴阳极成对耦合紫外光复合体系与阴极耦合紫外光复合体系、阳极耦合紫外光复合体系的电流效率,发现阴阳极成对耦合紫外光复合体系的电流效率是阴极耦合紫外光复合体系的2倍,是阳极耦合紫外光复合体系的4倍.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

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