The new biofilm-electrode method was used for the phenol degradation, because of its low current requirement. The biofilm-electrode reactor consisted of immobilized degrading bacteria on Ti electrode as cathode and Ti...The new biofilm-electrode method was used for the phenol degradation, because of its low current requirement. The biofilm-electrode reactor consisted of immobilized degrading bacteria on Ti electrode as cathode and Ti/PbO2 electrode as anode. With the biofilmelectrode reactor in a divided electrolytic cell, the phenol degradation rate could achieve 100% at 18 h which was higher than using traditional methods, such as biological or electrochemical methods. Chemical oxygen demand (COD) removal rate of the biofilmelectrode reactor was also greater than that using biological and electrochemical method, and could reach 80% at 16 h. The results suggested that the biofilm-electrode reactor system can be used to treat wastewater with phenol.展开更多
Sulfur doped anatase TiO2 nanoparticles (3 nm- 12 nm) were synthesized by the reaction of titanium tetrachloride, water and sulfuric acid with addition of 3 M NaOH at room temperature. The electro-optical and photoc...Sulfur doped anatase TiO2 nanoparticles (3 nm- 12 nm) were synthesized by the reaction of titanium tetrachloride, water and sulfuric acid with addition of 3 M NaOH at room temperature. The electro-optical and photocatalytic properties of the synthesized sulfur doped TiO2 nanoparticles were studied along with Degussa commercial TiO2 particles (24 nm). The results show that band gap of TiO2 particles decreases from 3.31 to 3.25 eV and for that of commercial TiO2 to 3.2 eV when the particle sizes increased from 3 nm to 12 nm with increase in sulfur doping. The results of the photocatalytic activity under UV and sun radiation show maximum phenol conversion at the particle size of 4 nm at 4.80% S-doping. Similar results are obtained using UV energy for both phenol conversion and conversion of CO2+H2O in which formation of methanol, ethanol and proponal is observed. Production of methanol is also achieved on samples with a particle size of 8 and 12 nm and sulfur doping of 4.80% and 5.26%. For TiO2 particle of 4 nm without S doping, the production of methanol, ethanol and proponal was lower as compared to the S-doped particles. This is attributed to the combined electronic effect and band gap change, S dopant, specific surface area and the light source used.展开更多
To promote the photocatalytic performance TiO2 and enlarge its application in visible region, carbon doped TiO2 (C/TiO2) composites were synthesized by wet impregnation method using sucrose as a precursor and used for...To promote the photocatalytic performance TiO2 and enlarge its application in visible region, carbon doped TiO2 (C/TiO2) composites were synthesized by wet impregnation method using sucrose as a precursor and used for phenol photocatalytic reaction. The synthesized products were characterized by Nitrogen adsorption-desorption isotherms (BET), X-ray diffraction (XRD), transmission electron microscopy (TEM) and UV-visible diffuse reflectance spectroscopy (UV-vis) techniques. The results showed that the obtained TiO2 was anatase phase in the C/TiO2 products, and its crystallite size was 11.7 nm, respectively. Carbon amount and calcined temperature of C/TiO2 can promote phenol removal. In this experiment, 5% carbon and 500 ℃ are the best choice for photocatalyst preparation. Under the UV light irradiation, 5%C/TiO2 (500 ℃, 2 h) exhibited the efficiency of 70.0% for phenol degradation within 150 min whereas TiO2 (500 ℃, 2 h) had 53.0% in the same duration of time. Also 5%C/TiO2 (500 ℃, 2 h) has higher photocatalytic performance under sunlight than pure TiO2. A combination of factors that include the smallest crystalline size, higher anatase percent, less band gap energy value and more oxygen vacant resulted in higher photocatalytic activities of 5%C/TiO2 (500 ℃, 2 h).展开更多
A synergistic photocatalysis combined pulsed diaphragm discharge(PDD)system with TiO_2 nanofilm deposited on the surface of quartz diaphragm is developed for the first time for phenol degradation in an aqueous solut...A synergistic photocatalysis combined pulsed diaphragm discharge(PDD)system with TiO_2 nanofilm deposited on the surface of quartz diaphragm is developed for the first time for phenol degradation in an aqueous solution.It is observed that the decomposition efficiency of phenol in the TiO_2 combined PDD system is higher than that of the single PDD system under the same conditions,indicating a successful collaboration between the photocatalysis and the plasma decomposition in the present system.Analysis of the solution's pH value confirms this collaboration and further reveals that the photocatalytic enhancement effect of phenol degradation is strong at a relatively low supplied voltage.The present TiO_2 combined PDD system exhibits improved efficiencies of pollutant degradation and energy utilization,suggesting a good candidate for wastewater treatment.展开更多
Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater treatment.Here,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coup...Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater treatment.Here,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coupled with the dispersion of magnetic Fe_(3)O_(4)/FeS(Fe/S)nanoparticles,was synthesized by simple impregnation precursor,followed by pyrolysis.The prepared Fe/S-biochar catalyst demonstrated outstanding phenol degradation efficiency across a wide pH range,with 98%of which eliminated even under neutral conditions(pH 7.0).The high catalytic activity was due to the multilevel porous structure of pollenderived biochar provided enough active sites and allowed for better electron transfer,then increases oxidation ability to promote the reaction.Moreover,the acid microenvironment formed by SO_(4)^(2-)group from Fe/S composite extended the pH range for Fenton reaction,and S^(2-)facilitated the conversion of≡Fe^(3+)to≡Fe^(2+),resulting in remarkable degradation efficiency.Further,biochar can effectively promote cycling stability by limiting Fe leaching.This work may provide a general strategy for designing 3D framework biochar-based Fe/S catalysts with excellent performance for heterogeneous Fenton reactions.展开更多
Statistical experimental designs were used to optimize the process of phenol degradation by Candida tropicalis Z-04, isolated from phenol-degrading aerobic granules. The most important factors influencing phenol degra...Statistical experimental designs were used to optimize the process of phenol degradation by Candida tropicalis Z-04, isolated from phenol-degrading aerobic granules. The most important factors influencing phenol degradation (p 〈 0.05), as identified by a two-level Plackett-Burman design with 11 variables, were yeast extract, phenol, inoculum size, and temperature. Steepest ascent method was undertaken to determine the optimal regions of these four significant factors. Central composite design (CCD) and response surface analysis were adopted to further investigate the mutual interactions between these variables and to identify their optimal values that would generate maximum phenol degradation. The analysis results indicated that interactions between yeast extract and temperature, phenol and temperature, inocuhim size and temperature affected the response variable (phenol degradation) significantly. The predicted results showed that the maximum removal efficiency of phenol (99.10%) could be obtained under the optimum conditions of yeast extract 0.41 g/L, phenol 1.03 g/L, inoculum size 1.43% (V/V) and temperature 30.04℃. These predicted values were further verified by validation experiments. The excellent correlation between predicted and experimental values confirmed the validity and practicability of this statistical optimum strategy. This study indicated the excellent ability of C. tropicalis Z-04 in degrading high-strength phenol. Optimal conditions obtained in this experiment laid a solid foundation for further use of this microorganism in the treatment of highstrength phenol effluents.展开更多
The degradation of phenol was carried out using heterogeneous Fenton-type catalysts in the presence of H_2O_2 and UV. Catalysts were prepared by exchanging and immobilizing Fe 2+ in zeolite 13X, silica gel or Al_2O...The degradation of phenol was carried out using heterogeneous Fenton-type catalysts in the presence of H_2O_2 and UV. Catalysts were prepared by exchanging and immobilizing Fe 2+ in zeolite 13X, silica gel or Al_2O_3. The concentration of phenol solution was 100 mg/L. The amount of H_2O_2 added was the stoichiometric amount of H_2O_2 required for the total oxidation of phenol. Under the irradiation of medium pressure light (300 W) phenol was mineralized within 1 h in the presence of Fe 2+/zeolite 13X. The COD removal rate was enhanced in the presence of Fe 2+/zeolite 13X compared to that of Fe 2+/silica gel or Fe 2+/Al_2O_3. Analogous homogenous photo-Fenton reaction with equivalent Fe 2+ was also carried out to evaluate the catalysis efficiency of Fe 2+/zeolite 13X. Results showed that the COD removal rate was near to that of homogeneous Fenton, while heterogeneous Fe 2+/zeolite 13X catalyst could be recycled.展开更多
This study was conducted to evaluate the degradation of phenolic compounds by one strain isolated from coal gasification wastewater( CGW). 16S rRNA gene sequences homology and phylogenetic analysis showed that the iso...This study was conducted to evaluate the degradation of phenolic compounds by one strain isolated from coal gasification wastewater( CGW). 16S rRNA gene sequences homology and phylogenetic analysis showed that the isolate is belonged to the genus Klebsiella sp. The effect of different phenolic compounds on the isolate was investigated by determining OD600and phenoloxidase activity,of which the results showed that the isolate can utilize phenol,4-methyl phenol,3,5-dimethyl phenol and resorcinol as carbon resources. The biofilm reactor( formed by the isolate) can resist the influent concentration of phenolic compounds as high as750 mg /L when fed with synthetic CGW and incubated at optimum conditions. The capacity of improving the biodegradability of CGW through degrading phenolic compounds was testified with fed the biofilm reactor with real CGW. Thus,it might be an effective strain for bioaugmentation of CGW treatment.展开更多
Titania nanocrystals with different morphologies were prepared using the hydrothermal method via controlling the pH values of solution, the ratio of reactants, temperature, and time of the hydrothermal reaction. The e...Titania nanocrystals with different morphologies were prepared using the hydrothermal method via controlling the pH values of solution, the ratio of reactants, temperature, and time of the hydrothermal reaction. The experimental results showed that uniform rod-like titania particles with an average aspect ratio of 6:1 could be obtained under the conditions of pH=11, n(TBOT):n(TEA)=1:2, hydrothermal treatment at 150 °C for 24 h. When pH〈10, spherical titania nanocrystals could be obtained; with increasing the pH value, the diameter became smaller. Finally, the smallest size of the particles could reach 7 nm. Nanocrystals with uniformly well-dispersed and perfect crystallographic form were obtained via the above method. Phenol was used as the degradation model for testing the photocatalytical activity of the titania nanocrystals with different morphologies.展开更多
Under oxygen sparged, the synergetic effects of both anodic cathodic electrocatalysis(ACE) and ferrous ion catalyzed anodic cathodic electrocatalysis(FeACE) on phenol degradation were observed in an undivided cell c...Under oxygen sparged, the synergetic effects of both anodic cathodic electrocatalysis(ACE) and ferrous ion catalyzed anodic cathodic electrocatalysis(FeACE) on phenol degradation were observed in an undivided cell composed of a β PbO 2 anode modified with fluorine resin and a nickel chromium titanium alloy net cathode. Oxygen sparging rate, ferrous concentration, and current significantly affect phenol destruction. The phenol was removed by 10%-13% increasingly under FeACE vs . ACE, and by 12%-15% under ACE vs . anodic electrocatalysis(AE). The phenol destruction was due to the formation of hydroxyl oxidant on the surface of lead oxide at the anode and the reduction of oxygen at the cathode.展开更多
A novel electrocatalysis, ferrous ion catalyzed anodic-cathodic electrocatalysis (FACEC), was developed for organic pollutants degradation, which could promote the degradation by achieving synergetic effects of both a...A novel electrocatalysis, ferrous ion catalyzed anodic-cathodic electrocatalysis (FACEC), was developed for organic pollutants degradation, which could promote the degradation by achieving synergetic effects of both anodic oxidation and cathodic indirect oxidation. The degradation rate of model pollutants - phenol by FACEC could increase by nearly 30% comparing with that of anodic electrocatalysis, and the current efficiency could reach 67%.展开更多
A microbial community structure of granules harvested from an anaerobic sludge blanket reactor treating phenolic wastewater was investigated using fluorescence in situ hybridization(FISH)and clone library construction...A microbial community structure of granules harvested from an anaerobic sludge blanket reactor treating phenolic wastewater was investigated using fluorescence in situ hybridization(FISH)and clone library construction.Clones of Syntrophorhabdaceae and Cryptanaerobacter were observed to be responsible for phenol degradation.For accurate taxonomic assignment of Cryptanaerobacter clones,phylogenetic analysis using nearly full-length 16S ribosomal RNA(rRNA)gene sequences was necessary.Three oligonucleotide probes were designed to detect the following three taxonomic groups:Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus.FISH analysis of thin sections of anaerobic granules showed a random distribution of bacteria and archaea.However,a well-defined distribution of Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus was observed.Cryptanaerobacter and Syntrophus were found on the outer layer of the granules and were closely associated with each other,while Syntrophorhabdaceae was located in the deeper part of the granules.Such specific distribution of the bacteria is most likely due to their metabolic association and affinity for the substrate.Phenol degradation in the granular sludge was observed to be carried out in the following way.First,Cryptanaerobacter converts phenol to benzoate,which is then degraded by Syntrophus into acetate.This syntrophic degradation of phenol occurs near the surface of the granule,where the phenol concen-tration is high.In the deeper part of the granule,where the phenol concentration is lower,Syntrophorhabdaceae degrades phenol into acetate.We observed that Syntrophorhabdaceae is less likely to produce benzoate as an intermediate to feed the neighboring organisms,which contradicts the theo-ries presented by previous studies.展开更多
Phenol-containing wastewater is typical organic wastewater,and its treatment is arduous.An advanced method to treat this type of wastewater is persulfate activation.Environmentally friendly ceriummanganese composite o...Phenol-containing wastewater is typical organic wastewater,and its treatment is arduous.An advanced method to treat this type of wastewater is persulfate activation.Environmentally friendly ceriummanganese composite oxide materials were synthesized by hydrothermal method and applied to the phenol degradation process.Various ratios of cerium and manganese,as well as the amount of sodium hydroxide,were investigated.The solid solutions of cerium and manganese were formed and confirmed by X-ray diffraction(XRD) and transmission electron microscopy(TEM).H_(2)-temperature programmed reduction(H_(2)-TPR) and X-ray photoelectron spectroscopy(XPS) were utilized to analyze the synergistic effect of cerium and manganese.It is found that there is a transformation between Ce^(4+)/Ce^(3+) and Mn^(2+)/Mn^(3+),which makes the material more trivalent manganese and thereby increases the catalytic activity.The effect of materials in catalyzing phenol degradation by peroxodisulfate(PDS) under various preparation conditions is discussed and high-effciency removal of phenol can be achieved and the removal rate at 180 min is close to 100%.The kinetic of this process was investigated and activation energy of phenol degradation is 62,35 kJ/mol.The degradation pathway of phenol was studied and it is found that PDS can be activated by low metal ions and the OH and SO_(4·)^(-)radicals play crucial roles according to the quenching experiments.展开更多
Phenolic compounds,as well as other aromatic compounds,have been reported to be abundant in hadal trenches.Although high-throughput sequencing studies have hinted at the potential of hadal microbes to degrade these co...Phenolic compounds,as well as other aromatic compounds,have been reported to be abundant in hadal trenches.Although high-throughput sequencing studies have hinted at the potential of hadal microbes to degrade these compounds,direct microbiological,genetic and biochemical evidence under in situ pressures remain absent.Here,a microbial consortium and a pure culture of Pseudomonas,newly isolated from Mariana Trench sediments,efficiently degraded phenol under pressures up to 70 and 60 MPa,respectively,with concomitant increase in biomass.By analyzing a high-pressure(70 MPa)culture metatranscriptome,not only was the entire range of metabolic processes under high pressure generated,but also genes encod-ing complete phenol degradation via ortho-and meta-cleavage pathways were revealed.The isolate of Pseudomonas also contained genes encoding the complete degradation pathway.Six transcribed genes(dmpKLMNOP_(sed))were functionally identified to encode a multicomponent hydroxylase catalyzing the hydroxylation of phenol and its methylated derivatives by heterogeneous expression.In addition,key catabolic genes identified in the metatranscriptome of the high-pressure cultures and genomes of bacterial isolates were found to be all widely distributed in 22 published hadal microbial metagenomes.At microbiological,genetic,bioinformatics,and biochemical levels,this study found that microorganisms widely found in hadal trenches were able to effectively drive phenolic compound degradation under high hydrostatic pressures.This information will bridge a knowledge gap concerning the microbial aromatics degradation within hadal trenches.展开更多
Relative abundance and relationships between aniline, phenol and catechol degraders were investigated in unpolluted and polluted fresh waters in Osaka prefecture, Japan. Phenol and catechol degraders were found more f...Relative abundance and relationships between aniline, phenol and catechol degraders were investigated in unpolluted and polluted fresh waters in Osaka prefecture, Japan. Phenol and catechol degraders were found more frequently compared to aniline degraders. The results indicate that these degraders were more abundant in polluted waters than in unpolluted waters. Aniline degraders isolated from the Ina River water showed a higher capability of degrading catechol than phenol. Analysis on sequence homology among these three kinds of degraders indicated a possible relationship between aniline degraders and certain strains of both catechol and phenol degraders.展开更多
Wastewater from the thermochemical conversion of coal and biomass contains a significant amount of phenolic structures compounds.The degradation of these phenolic compounds to hydrogen-rich gasses can prevent envi-ron...Wastewater from the thermochemical conversion of coal and biomass contains a significant amount of phenolic structures compounds.The degradation of these phenolic compounds to hydrogen-rich gasses can prevent envi-ronmental pollution and save energy.Supercritical water(SCW)gasification of phenol is experimentally studied and a reactive force field molecular dynamics(ReaxFF-MD)simulation is conducted to investigate the catalytic mechanism of Ni/Al2 O3 in the phenol degradation.The experimental results indicate that Ni/Al2 O3 facilitates the conversion of phenol to 1-ethoxy butane via ring opening,which is a crucial step for complete gasification.The ReaxFF-MD simulation demonstrated that Ni facilitates the formation of H3 O free radicals and Ni-phenol inter-mediates.H3 O free radicals can be decomposed into H2 and OH free radicals.Both the generated OH free radical and Ni-phenol intermediate promote the ring-opening reaction of phenol.Ni promotes the direct decomposition of phenol into C1,C2,and C3 fragments,which is beneficial for further complete gasification.展开更多
In the present study,a combination of pulsed discharge plasma and TiO2(plasma/TiO2)has been developed in order to study the activity of TiO2by varying the discharge conditions of pulsed voltage,discharge mode,air fl...In the present study,a combination of pulsed discharge plasma and TiO2(plasma/TiO2)has been developed in order to study the activity of TiO2by varying the discharge conditions of pulsed voltage,discharge mode,air flow rate and solution conductivity.Phenol was used as the chemical probe to characterize the activity of TiO2in a pulsed discharge system.The experimental results showed that the phenol removal efficiency could be improved by about 10%by increasing the applied voltage.The phenol removal efficiency for three discharge modes in the plasma-discharge-alone system was found to be highest in the spark mode,followed by the spark–streamer mode and finally the streamer mode.In the plasma/TiO2system,the highest catalytic effect of TiO2was observed in the spark–streamer discharge mode,which may be attributed to the favorable chemical and physical effects from the spark–streamer discharge mode,such as ultraviolet light,O3,H2O2,pyrolysis,shockwaves and high-energy electrons.Meanwhile,the optimal flow rate and conductivity were 0.05 m^3l^(-1)and 10μS cm^(-1),respectively.The main phenolic intermediates were hydroquinone,catechol,and p-benzoquinone during the discharge treatment process.A different phenol degradation pathway was observed in the plasma/TiO2system as compared to plasma alone.Analysis of the reaction intermediates demonstrated that p-benzoquinone reduction was selectively catalyzed on the TiO2surface.The effective decomposition of phenol constant(De)increased from 74.11%to 79.16%when TiO2was added,indicating that higher phenol mineralization was achieved in the plasma/TiO2system.展开更多
The connections between the building units of meta-stable lattice were generally considered to be easily disturbed during the doping process, causing serious hindrances blocking the development of functional doped mat...The connections between the building units of meta-stable lattice were generally considered to be easily disturbed during the doping process, causing serious hindrances blocking the development of functional doped materials. In this work, the synthesis of doped brookite, a typical meta-stable phase of TiO2, has been explored novelly by in-situ adding of cations of VIIIB and IB,IIB elements in the 3rd period(Fe, Co, Ni, Cu, Zn) during the urea-lactate aided low-basicity hydrothermal process. The results showed that only Cu-doped brookite could be successfully synthesized with trace amount of copper intensively internalized into the brookite lattice, while the other dopants lead to the formation of anatase TiO2. Extensive characterizations indicated a two-step doping process, where copper ions were firstly dispersed in an amorphous layer on the lattice surface and then they were internalized into brookite lattice. Cu-doped brookite exhibited significantly enhanced photocatalytic activity in the phenol degradation under visible light compared to bare brookite. The enhancement of catalytic performance was assigned to the impurity band gap and the reduction of charge carriers' recombination introduced by the internalization of Cu ions. The investigation reported herein contributes to the understanding of complex ion-doping effects on the structures of meta-stable materials, and provides hints for obtaining other functional doped materials.展开更多
The photocatalytic degradation of phenol and 4-chlorophenol (4-CP) in aqueous suspensions with the use of titanium dioxide (TiO2 ) under UV irradiation was examined. The effects of different supporting materials m...The photocatalytic degradation of phenol and 4-chlorophenol (4-CP) in aqueous suspensions with the use of titanium dioxide (TiO2 ) under UV irradiation was examined. The effects of different supporting materials mixed physically with TiO2 were studied to achieve maximum degradation efficiency. Among the three supports, namely activated carbon (AC), silica (SiO2 ) and zeolite (ZSM-5), all exhibited paramount efficiency for degradation of phenol and 4-CP and was better than TiO2 alone. The optimum concentration was found to be 50 mg for all supporting materials. The efficiency order of the three supports was as follows: AC 〉 ZSM-5 〉 SiO2 , respectively. Whilst, the degradation of phenol and 4-CP was improved from 70.6% to 87.6% and 80.6% to 89.7%, respectively, within 120 min photocatalysis in the presence of optimal amount of AC. The degradation was also comparatively enhanced in the presence of cheaper rice husk and the activity was closed to ZSM-5 and lower than AC.展开更多
Various compositions of cobalt and sulfur co-doped titania nano-photocatalyst are synthesized via sol–gel method. A number of techniques including X-ray diffraction(XRD), ultraviolet–visible(UV–Vis), Rutherford...Various compositions of cobalt and sulfur co-doped titania nano-photocatalyst are synthesized via sol–gel method. A number of techniques including X-ray diffraction(XRD), ultraviolet–visible(UV–Vis), Rutherford backscattering spectrometry(RBS), thermal gravimetric analysis(TGA)Raman, N2 sorption, electron microscopy are used to examine composition, crystalline phase, morphology, distribution of dopants, surface area and optical properties o synthesized materials. The synthesized materials consisted of quasispherical nanoparticles of anatase phase exhibiting a high surface area and homogeneous distribution o dopants. Cobalt and sulfur co-doped titania demonstrated remarkable structural and optical properties leading to an efficient photocatalytic activity for degradation of dyes and phenol under visible light irradiations. Moreover, the effect of dye concentration catalyst dose and p H on photodegradation behavior of environmental pollutants and recyclability of the catalyst is also examined to optimize the activity of nano-photocatalys and gain a better understanding of the process.展开更多
基金supported by the Hi-Tech Research and Development Program (863) of China (No. 2006AA06Z321)the National Natural Science Foundation of China(No.20843001)
文摘The new biofilm-electrode method was used for the phenol degradation, because of its low current requirement. The biofilm-electrode reactor consisted of immobilized degrading bacteria on Ti electrode as cathode and Ti/PbO2 electrode as anode. With the biofilmelectrode reactor in a divided electrolytic cell, the phenol degradation rate could achieve 100% at 18 h which was higher than using traditional methods, such as biological or electrochemical methods. Chemical oxygen demand (COD) removal rate of the biofilmelectrode reactor was also greater than that using biological and electrochemical method, and could reach 80% at 16 h. The results suggested that the biofilm-electrode reactor system can be used to treat wastewater with phenol.
文摘Sulfur doped anatase TiO2 nanoparticles (3 nm- 12 nm) were synthesized by the reaction of titanium tetrachloride, water and sulfuric acid with addition of 3 M NaOH at room temperature. The electro-optical and photocatalytic properties of the synthesized sulfur doped TiO2 nanoparticles were studied along with Degussa commercial TiO2 particles (24 nm). The results show that band gap of TiO2 particles decreases from 3.31 to 3.25 eV and for that of commercial TiO2 to 3.2 eV when the particle sizes increased from 3 nm to 12 nm with increase in sulfur doping. The results of the photocatalytic activity under UV and sun radiation show maximum phenol conversion at the particle size of 4 nm at 4.80% S-doping. Similar results are obtained using UV energy for both phenol conversion and conversion of CO2+H2O in which formation of methanol, ethanol and proponal is observed. Production of methanol is also achieved on samples with a particle size of 8 and 12 nm and sulfur doping of 4.80% and 5.26%. For TiO2 particle of 4 nm without S doping, the production of methanol, ethanol and proponal was lower as compared to the S-doped particles. This is attributed to the combined electronic effect and band gap change, S dopant, specific surface area and the light source used.
基金Funded by Yunnan Provincial Agricultural Joint Project (No.2018FG001-051)Yunnan Provincial Department of Education Research Fund (No. 2020Y0414)
文摘To promote the photocatalytic performance TiO2 and enlarge its application in visible region, carbon doped TiO2 (C/TiO2) composites were synthesized by wet impregnation method using sucrose as a precursor and used for phenol photocatalytic reaction. The synthesized products were characterized by Nitrogen adsorption-desorption isotherms (BET), X-ray diffraction (XRD), transmission electron microscopy (TEM) and UV-visible diffuse reflectance spectroscopy (UV-vis) techniques. The results showed that the obtained TiO2 was anatase phase in the C/TiO2 products, and its crystallite size was 11.7 nm, respectively. Carbon amount and calcined temperature of C/TiO2 can promote phenol removal. In this experiment, 5% carbon and 500 ℃ are the best choice for photocatalyst preparation. Under the UV light irradiation, 5%C/TiO2 (500 ℃, 2 h) exhibited the efficiency of 70.0% for phenol degradation within 150 min whereas TiO2 (500 ℃, 2 h) had 53.0% in the same duration of time. Also 5%C/TiO2 (500 ℃, 2 h) has higher photocatalytic performance under sunlight than pure TiO2. A combination of factors that include the smallest crystalline size, higher anatase percent, less band gap energy value and more oxygen vacant resulted in higher photocatalytic activities of 5%C/TiO2 (500 ℃, 2 h).
基金supported by National Natural Science Foundation of China(Nos.11205202,21203204 and 11175214)National Natural Science Foundation of Anhui Province(No.1308085QA09)
文摘A synergistic photocatalysis combined pulsed diaphragm discharge(PDD)system with TiO_2 nanofilm deposited on the surface of quartz diaphragm is developed for the first time for phenol degradation in an aqueous solution.It is observed that the decomposition efficiency of phenol in the TiO_2 combined PDD system is higher than that of the single PDD system under the same conditions,indicating a successful collaboration between the photocatalysis and the plasma decomposition in the present system.Analysis of the solution's pH value confirms this collaboration and further reveals that the photocatalytic enhancement effect of phenol degradation is strong at a relatively low supplied voltage.The present TiO_2 combined PDD system exhibits improved efficiencies of pollutant degradation and energy utilization,suggesting a good candidate for wastewater treatment.
基金financially supported by the National Natural Science Foundation of China (Nos.21876139 and 21922606)Yulin Science and Technology Project of China (No.CXY2021-134)。
文摘Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater treatment.Here,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coupled with the dispersion of magnetic Fe_(3)O_(4)/FeS(Fe/S)nanoparticles,was synthesized by simple impregnation precursor,followed by pyrolysis.The prepared Fe/S-biochar catalyst demonstrated outstanding phenol degradation efficiency across a wide pH range,with 98%of which eliminated even under neutral conditions(pH 7.0).The high catalytic activity was due to the multilevel porous structure of pollenderived biochar provided enough active sites and allowed for better electron transfer,then increases oxidation ability to promote the reaction.Moreover,the acid microenvironment formed by SO_(4)^(2-)group from Fe/S composite extended the pH range for Fenton reaction,and S^(2-)facilitated the conversion of≡Fe^(3+)to≡Fe^(2+),resulting in remarkable degradation efficiency.Further,biochar can effectively promote cycling stability by limiting Fe leaching.This work may provide a general strategy for designing 3D framework biochar-based Fe/S catalysts with excellent performance for heterogeneous Fenton reactions.
基金supported by the National Natural Science Foundation of China (No.50778110)
文摘Statistical experimental designs were used to optimize the process of phenol degradation by Candida tropicalis Z-04, isolated from phenol-degrading aerobic granules. The most important factors influencing phenol degradation (p 〈 0.05), as identified by a two-level Plackett-Burman design with 11 variables, were yeast extract, phenol, inoculum size, and temperature. Steepest ascent method was undertaken to determine the optimal regions of these four significant factors. Central composite design (CCD) and response surface analysis were adopted to further investigate the mutual interactions between these variables and to identify their optimal values that would generate maximum phenol degradation. The analysis results indicated that interactions between yeast extract and temperature, phenol and temperature, inocuhim size and temperature affected the response variable (phenol degradation) significantly. The predicted results showed that the maximum removal efficiency of phenol (99.10%) could be obtained under the optimum conditions of yeast extract 0.41 g/L, phenol 1.03 g/L, inoculum size 1.43% (V/V) and temperature 30.04℃. These predicted values were further verified by validation experiments. The excellent correlation between predicted and experimental values confirmed the validity and practicability of this statistical optimum strategy. This study indicated the excellent ability of C. tropicalis Z-04 in degrading high-strength phenol. Optimal conditions obtained in this experiment laid a solid foundation for further use of this microorganism in the treatment of highstrength phenol effluents.
基金TheNationalNaturalScienceFoundationofChina (No .2 0 1760 5 3 )
文摘The degradation of phenol was carried out using heterogeneous Fenton-type catalysts in the presence of H_2O_2 and UV. Catalysts were prepared by exchanging and immobilizing Fe 2+ in zeolite 13X, silica gel or Al_2O_3. The concentration of phenol solution was 100 mg/L. The amount of H_2O_2 added was the stoichiometric amount of H_2O_2 required for the total oxidation of phenol. Under the irradiation of medium pressure light (300 W) phenol was mineralized within 1 h in the presence of Fe 2+/zeolite 13X. The COD removal rate was enhanced in the presence of Fe 2+/zeolite 13X compared to that of Fe 2+/silica gel or Fe 2+/Al_2O_3. Analogous homogenous photo-Fenton reaction with equivalent Fe 2+ was also carried out to evaluate the catalysis efficiency of Fe 2+/zeolite 13X. Results showed that the COD removal rate was near to that of homogeneous Fenton, while heterogeneous Fe 2+/zeolite 13X catalyst could be recycled.
基金Sponsored by the Sino-Dutch Research Program(SDRP)(Grant No.2012-2016)the State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(Grant No.2013DX10)
文摘This study was conducted to evaluate the degradation of phenolic compounds by one strain isolated from coal gasification wastewater( CGW). 16S rRNA gene sequences homology and phylogenetic analysis showed that the isolate is belonged to the genus Klebsiella sp. The effect of different phenolic compounds on the isolate was investigated by determining OD600and phenoloxidase activity,of which the results showed that the isolate can utilize phenol,4-methyl phenol,3,5-dimethyl phenol and resorcinol as carbon resources. The biofilm reactor( formed by the isolate) can resist the influent concentration of phenolic compounds as high as750 mg /L when fed with synthetic CGW and incubated at optimum conditions. The capacity of improving the biodegradability of CGW through degrading phenolic compounds was testified with fed the biofilm reactor with real CGW. Thus,it might be an effective strain for bioaugmentation of CGW treatment.
基金the Foundation of the Ministry of Science and Technology of China(No.2006BA618A)
文摘Titania nanocrystals with different morphologies were prepared using the hydrothermal method via controlling the pH values of solution, the ratio of reactants, temperature, and time of the hydrothermal reaction. The experimental results showed that uniform rod-like titania particles with an average aspect ratio of 6:1 could be obtained under the conditions of pH=11, n(TBOT):n(TEA)=1:2, hydrothermal treatment at 150 °C for 24 h. When pH〈10, spherical titania nanocrystals could be obtained; with increasing the pH value, the diameter became smaller. Finally, the smallest size of the particles could reach 7 nm. Nanocrystals with uniformly well-dispersed and perfect crystallographic form were obtained via the above method. Phenol was used as the degradation model for testing the photocatalytical activity of the titania nanocrystals with different morphologies.
基金Supported by the Foundation of Educational Ministry of China(No.986 79) and Zhejiang Natural Science Foundation(No.2 0 0 0 4 3)
文摘Under oxygen sparged, the synergetic effects of both anodic cathodic electrocatalysis(ACE) and ferrous ion catalyzed anodic cathodic electrocatalysis(FeACE) on phenol degradation were observed in an undivided cell composed of a β PbO 2 anode modified with fluorine resin and a nickel chromium titanium alloy net cathode. Oxygen sparging rate, ferrous concentration, and current significantly affect phenol destruction. The phenol was removed by 10%-13% increasingly under FeACE vs . ACE, and by 12%-15% under ACE vs . anodic electrocatalysis(AE). The phenol destruction was due to the formation of hydroxyl oxidant on the surface of lead oxide at the anode and the reduction of oxygen at the cathode.
文摘A novel electrocatalysis, ferrous ion catalyzed anodic-cathodic electrocatalysis (FACEC), was developed for organic pollutants degradation, which could promote the degradation by achieving synergetic effects of both anodic oxidation and cathodic indirect oxidation. The degradation rate of model pollutants - phenol by FACEC could increase by nearly 30% comparing with that of anodic electrocatalysis, and the current efficiency could reach 67%.
基金supported by Grant-in-Aids for Scientific Research(B)(JP18H01564)from the Japan Society for the Promotion of Science.
文摘A microbial community structure of granules harvested from an anaerobic sludge blanket reactor treating phenolic wastewater was investigated using fluorescence in situ hybridization(FISH)and clone library construction.Clones of Syntrophorhabdaceae and Cryptanaerobacter were observed to be responsible for phenol degradation.For accurate taxonomic assignment of Cryptanaerobacter clones,phylogenetic analysis using nearly full-length 16S ribosomal RNA(rRNA)gene sequences was necessary.Three oligonucleotide probes were designed to detect the following three taxonomic groups:Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus.FISH analysis of thin sections of anaerobic granules showed a random distribution of bacteria and archaea.However,a well-defined distribution of Syntrophorhabdaceae,Cryptanaerobacter,and Syntrophus was observed.Cryptanaerobacter and Syntrophus were found on the outer layer of the granules and were closely associated with each other,while Syntrophorhabdaceae was located in the deeper part of the granules.Such specific distribution of the bacteria is most likely due to their metabolic association and affinity for the substrate.Phenol degradation in the granular sludge was observed to be carried out in the following way.First,Cryptanaerobacter converts phenol to benzoate,which is then degraded by Syntrophus into acetate.This syntrophic degradation of phenol occurs near the surface of the granule,where the phenol concen-tration is high.In the deeper part of the granule,where the phenol concentration is lower,Syntrophorhabdaceae degrades phenol into acetate.We observed that Syntrophorhabdaceae is less likely to produce benzoate as an intermediate to feed the neighboring organisms,which contradicts the theo-ries presented by previous studies.
基金supported by the National Natural Science Foundation of China (21908132)。
文摘Phenol-containing wastewater is typical organic wastewater,and its treatment is arduous.An advanced method to treat this type of wastewater is persulfate activation.Environmentally friendly ceriummanganese composite oxide materials were synthesized by hydrothermal method and applied to the phenol degradation process.Various ratios of cerium and manganese,as well as the amount of sodium hydroxide,were investigated.The solid solutions of cerium and manganese were formed and confirmed by X-ray diffraction(XRD) and transmission electron microscopy(TEM).H_(2)-temperature programmed reduction(H_(2)-TPR) and X-ray photoelectron spectroscopy(XPS) were utilized to analyze the synergistic effect of cerium and manganese.It is found that there is a transformation between Ce^(4+)/Ce^(3+) and Mn^(2+)/Mn^(3+),which makes the material more trivalent manganese and thereby increases the catalytic activity.The effect of materials in catalyzing phenol degradation by peroxodisulfate(PDS) under various preparation conditions is discussed and high-effciency removal of phenol can be achieved and the removal rate at 180 min is close to 100%.The kinetic of this process was investigated and activation energy of phenol degradation is 62,35 kJ/mol.The degradation pathway of phenol was studied and it is found that PDS can be activated by low metal ions and the OH and SO_(4·)^(-)radicals play crucial roles according to the quenching experiments.
基金supported by the National Natural Science Foundation of China(Grants 91951106,92051104)。
文摘Phenolic compounds,as well as other aromatic compounds,have been reported to be abundant in hadal trenches.Although high-throughput sequencing studies have hinted at the potential of hadal microbes to degrade these compounds,direct microbiological,genetic and biochemical evidence under in situ pressures remain absent.Here,a microbial consortium and a pure culture of Pseudomonas,newly isolated from Mariana Trench sediments,efficiently degraded phenol under pressures up to 70 and 60 MPa,respectively,with concomitant increase in biomass.By analyzing a high-pressure(70 MPa)culture metatranscriptome,not only was the entire range of metabolic processes under high pressure generated,but also genes encod-ing complete phenol degradation via ortho-and meta-cleavage pathways were revealed.The isolate of Pseudomonas also contained genes encoding the complete degradation pathway.Six transcribed genes(dmpKLMNOP_(sed))were functionally identified to encode a multicomponent hydroxylase catalyzing the hydroxylation of phenol and its methylated derivatives by heterogeneous expression.In addition,key catabolic genes identified in the metatranscriptome of the high-pressure cultures and genomes of bacterial isolates were found to be all widely distributed in 22 published hadal microbial metagenomes.At microbiological,genetic,bioinformatics,and biochemical levels,this study found that microorganisms widely found in hadal trenches were able to effectively drive phenolic compound degradation under high hydrostatic pressures.This information will bridge a knowledge gap concerning the microbial aromatics degradation within hadal trenches.
文摘Relative abundance and relationships between aniline, phenol and catechol degraders were investigated in unpolluted and polluted fresh waters in Osaka prefecture, Japan. Phenol and catechol degraders were found more frequently compared to aniline degraders. The results indicate that these degraders were more abundant in polluted waters than in unpolluted waters. Aniline degraders isolated from the Ina River water showed a higher capability of degrading catechol than phenol. Analysis on sequence homology among these three kinds of degraders indicated a possible relationship between aniline degraders and certain strains of both catechol and phenol degraders.
基金supported by the National Natural Science Founda-tion of China(Grant Nos.:51976046 and 52006044)the Shenzhen Technology Project(Grant No.:RCJC20210609103755110).
文摘Wastewater from the thermochemical conversion of coal and biomass contains a significant amount of phenolic structures compounds.The degradation of these phenolic compounds to hydrogen-rich gasses can prevent envi-ronmental pollution and save energy.Supercritical water(SCW)gasification of phenol is experimentally studied and a reactive force field molecular dynamics(ReaxFF-MD)simulation is conducted to investigate the catalytic mechanism of Ni/Al2 O3 in the phenol degradation.The experimental results indicate that Ni/Al2 O3 facilitates the conversion of phenol to 1-ethoxy butane via ring opening,which is a crucial step for complete gasification.The ReaxFF-MD simulation demonstrated that Ni facilitates the formation of H3 O free radicals and Ni-phenol inter-mediates.H3 O free radicals can be decomposed into H2 and OH free radicals.Both the generated OH free radical and Ni-phenol intermediate promote the ring-opening reaction of phenol.Ni promotes the direct decomposition of phenol into C1,C2,and C3 fragments,which is beneficial for further complete gasification.
基金funded by the Fundamental Research Funds for the Central Universities under Grant(DUT 15QY17)National Natural Science Foundation of China(Project Nos.51477025 and U1462105)
文摘In the present study,a combination of pulsed discharge plasma and TiO2(plasma/TiO2)has been developed in order to study the activity of TiO2by varying the discharge conditions of pulsed voltage,discharge mode,air flow rate and solution conductivity.Phenol was used as the chemical probe to characterize the activity of TiO2in a pulsed discharge system.The experimental results showed that the phenol removal efficiency could be improved by about 10%by increasing the applied voltage.The phenol removal efficiency for three discharge modes in the plasma-discharge-alone system was found to be highest in the spark mode,followed by the spark–streamer mode and finally the streamer mode.In the plasma/TiO2system,the highest catalytic effect of TiO2was observed in the spark–streamer discharge mode,which may be attributed to the favorable chemical and physical effects from the spark–streamer discharge mode,such as ultraviolet light,O3,H2O2,pyrolysis,shockwaves and high-energy electrons.Meanwhile,the optimal flow rate and conductivity were 0.05 m^3l^(-1)and 10μS cm^(-1),respectively.The main phenolic intermediates were hydroquinone,catechol,and p-benzoquinone during the discharge treatment process.A different phenol degradation pathway was observed in the plasma/TiO2system as compared to plasma alone.Analysis of the reaction intermediates demonstrated that p-benzoquinone reduction was selectively catalyzed on the TiO2surface.The effective decomposition of phenol constant(De)increased from 74.11%to 79.16%when TiO2was added,indicating that higher phenol mineralization was achieved in the plasma/TiO2system.
基金Financially supported by the Science and Technology Programs from Fujian Province(No.2013H0057)
文摘The connections between the building units of meta-stable lattice were generally considered to be easily disturbed during the doping process, causing serious hindrances blocking the development of functional doped materials. In this work, the synthesis of doped brookite, a typical meta-stable phase of TiO2, has been explored novelly by in-situ adding of cations of VIIIB and IB,IIB elements in the 3rd period(Fe, Co, Ni, Cu, Zn) during the urea-lactate aided low-basicity hydrothermal process. The results showed that only Cu-doped brookite could be successfully synthesized with trace amount of copper intensively internalized into the brookite lattice, while the other dopants lead to the formation of anatase TiO2. Extensive characterizations indicated a two-step doping process, where copper ions were firstly dispersed in an amorphous layer on the lattice surface and then they were internalized into brookite lattice. Cu-doped brookite exhibited significantly enhanced photocatalytic activity in the phenol degradation under visible light compared to bare brookite. The enhancement of catalytic performance was assigned to the impurity band gap and the reduction of charge carriers' recombination introduced by the internalization of Cu ions. The investigation reported herein contributes to the understanding of complex ion-doping effects on the structures of meta-stable materials, and provides hints for obtaining other functional doped materials.
文摘The photocatalytic degradation of phenol and 4-chlorophenol (4-CP) in aqueous suspensions with the use of titanium dioxide (TiO2 ) under UV irradiation was examined. The effects of different supporting materials mixed physically with TiO2 were studied to achieve maximum degradation efficiency. Among the three supports, namely activated carbon (AC), silica (SiO2 ) and zeolite (ZSM-5), all exhibited paramount efficiency for degradation of phenol and 4-CP and was better than TiO2 alone. The optimum concentration was found to be 50 mg for all supporting materials. The efficiency order of the three supports was as follows: AC 〉 ZSM-5 〉 SiO2 , respectively. Whilst, the degradation of phenol and 4-CP was improved from 70.6% to 87.6% and 80.6% to 89.7%, respectively, within 120 min photocatalysis in the presence of optimal amount of AC. The degradation was also comparatively enhanced in the presence of cheaper rice husk and the activity was closed to ZSM-5 and lower than AC.
文摘Various compositions of cobalt and sulfur co-doped titania nano-photocatalyst are synthesized via sol–gel method. A number of techniques including X-ray diffraction(XRD), ultraviolet–visible(UV–Vis), Rutherford backscattering spectrometry(RBS), thermal gravimetric analysis(TGA)Raman, N2 sorption, electron microscopy are used to examine composition, crystalline phase, morphology, distribution of dopants, surface area and optical properties o synthesized materials. The synthesized materials consisted of quasispherical nanoparticles of anatase phase exhibiting a high surface area and homogeneous distribution o dopants. Cobalt and sulfur co-doped titania demonstrated remarkable structural and optical properties leading to an efficient photocatalytic activity for degradation of dyes and phenol under visible light irradiations. Moreover, the effect of dye concentration catalyst dose and p H on photodegradation behavior of environmental pollutants and recyclability of the catalyst is also examined to optimize the activity of nano-photocatalys and gain a better understanding of the process.