In this study,the cobalt-nickel layered double hydroxides(CoNi LDH)were synthesized with a variety of Co/Ni mass ratio,as CoxNiyLDHs.In comparison,Co1Ni3LDH presented the best peroxymonosulfate(PMS)activation efficien...In this study,the cobalt-nickel layered double hydroxides(CoNi LDH)were synthesized with a variety of Co/Ni mass ratio,as CoxNiyLDHs.In comparison,Co1Ni3LDH presented the best peroxymonosulfate(PMS)activation efficiency for 2,4-dichlorophenol removal.Meanwhile,CoNi LDH@Nickel foam(CoNi LDH@NF)composite membrane was constructed for enhancing the stability of catalytic performance.Herein,CoNi LDH@NF-PMS system exerted high degradation efficiency of 99.22%within 90 min for 2,4-DCP when[PMS]_(0)=0.4 g/L,Co^(1)Ni^(3)LDH@NF=2 cm×2 cm(0.2 g/L),reaction temperature=298 K.For the surface morphology and structure of the catalyst,it was demonstrated that the CoNi LDH@NF composite membrane possessed abundant cavity structure,good specific surface area and sufficient active sites.Importantly,·OH,SO_(4)·^(-)and^(1)O_(2)played the primary role in the CoNi LDH@NF-PMS system for 2,4-DCP decomposition,which revealed the PMS activation mechanism in CoNi LDH@NF-PMS system.Hence,this study eliminated the stability and adaptability of CoNi LDH@NF composite membrane,proposing a new theoretical basis of PMS heterogeneous catalysts selection.展开更多
This study demonstrated interesting ultrafast activation of molecular O_(2) by copper oxide(CuO)particles and very rapid elimination of aqueous 2,4-dichlo rophenol(2,4-DCP)within reaction time of 30 s.Electron paramag...This study demonstrated interesting ultrafast activation of molecular O_(2) by copper oxide(CuO)particles and very rapid elimination of aqueous 2,4-dichlo rophenol(2,4-DCP)within reaction time of 30 s.Electron paramagnetic resonance(EPR)characterization indicated that·OH,Cu^(3+),^1 O_(2) and O_(2)^·-were generated in the CuO/O_(2) systems,wherein O_(2)^·-would be the main reactive species responsible for 2,4-DCP degradation.It was further found that the catalytic ability of CuO for O_(2) activation was highly size dependent and nano-CuO was far reactive than micro-CuO.H2 temperature-programmed reduction(H2-TPR),X-ray photoelectron spectroscopy(XPS)and vibrating sample magnetometer(VSM)analyses revealed that both the quantity and the reactivity of the surface reaction sites(surface Cu+and O_(2))could determine the catalytic ability of CuO affecting efficient Cu^(+)-based molecular oxygen activation.Moreover,the O_(2) activation ability of CuO would depend on not only the dimension,but also crystalline factors,for example,the exposed facets.展开更多
To understand the feasibility of its application to the in situ remediation of contaminated groundwater,the dechlori-nation of 2,4-dichlorophenol (2,4-DCP) by Ni/Fe nanoparticles in the presence of humic acid (HA) was...To understand the feasibility of its application to the in situ remediation of contaminated groundwater,the dechlori-nation of 2,4-dichlorophenol (2,4-DCP) by Ni/Fe nanoparticles in the presence of humic acid (HA) was investigated.We found that,as high performance liquid chromatography (HPLC) was used,the 2,4-DCP was first quickly reduced to o-chlorophenol (o-CP) and p-chlorophenol (p-CP),and then reduced to phenol as the final product.Our experimental results indicated that HA had an adverse effect on the dechlorination of 2,4-DCP by Ni/Fe nanoparticles,as the HA concentration increased,the removal rate decreased evidently.It also demonstrated that 2,4-DCP was reduced more easily to o-CP than to p-CP,and that the sequence of the tendency in dechlorination of intermediates was p-CP>o-CP.Transmission electron microscope (TEM) showed that HA could act as an adsorbate to compete reactive sites on the surface of Ni/Fe nanoparticles to decrease the dechlorination rate.Also we con-cluded that the dechlorination reaction of 2,4-DCP over Ni/Fe nanoparticles progressed through catalytic reductive dechlorination.展开更多
The adsorption capacity of activated carbon produced from oil palm empty fruit bunches through removal of 2,4-dichlorophenol from aqueous solution was carried out in the laboratory. The activated carbon was produced b...The adsorption capacity of activated carbon produced from oil palm empty fruit bunches through removal of 2,4-dichlorophenol from aqueous solution was carried out in the laboratory. The activated carbon was produced by thermal activation of activation time with 30 min at 800℃. The adsorption process conditions were determined with the statistical optimization followed by central composite design. A developed polynomial model for operating conditions of adsorption process indicated that the optimum conditions for maximum adsorption of phenolic compound were： agitation rate of 100 r/min, contact time of 8 h, initial adsorbate concentration of 250 mg/L and pH 4. Adsorption isotherms were conducted to evaluate biosorption process. Langmuir isotherm was more favorable （R^2=0.93） for removal of 2,4-dichlorophenol by the activated carbon rather than Freundlich isotherm （R^2=0.88）.展开更多
A hypercrosslinked adsorption resin （ZH-05） modified by N-acetylaniline in the post crosslinking process was prepared. The adsorption properties of ZH-05 toward 2,4-dichlorophenol in comparison with granular activat...A hypercrosslinked adsorption resin （ZH-05） modified by N-acetylaniline in the post crosslinking process was prepared. The adsorption properties of ZH-05 toward 2,4-dichlorophenol in comparison with granular activated carbon （GAC） and Amberlite XAD-4 were observed. The present study mainly focuses on the static equilibrium adsorption behaviors, desorption profiles and the proof of chemisorption. The results show that the Langmuir equation can give a perfect fitting to experimental data, and high temperature was favorable for adsorption of 2,4-dichlorophenol on ZH-05. A related equation was used to correlate the amount of chemisorption and the suppositionai chemisorption equilibrium concentration of adsorbate in aqueous solution. The adsorption capacities from different ranges of temperature and the static desorption experiment both reveal the same conclusion, i.e., the adsorption of 2,4-dichlorophenol from water on ZH-05 is a coexistent process of physical adsorption and chemical transition as on GAC.展开更多
Binary oxide catalysts with various weight percentage V2O5 loadings were prepared by solid‐state dispersion and the nanocomposites were modified with surfactants. The catalysts were analyzed using X‐ray diffraction,...Binary oxide catalysts with various weight percentage V2O5 loadings were prepared by solid‐state dispersion and the nanocomposites were modified with surfactants. The catalysts were analyzed using X‐ray diffraction, diffuse‐reflectance spectroscopy, Fourier‐transform infrared spectroscopy, scanning electron microscopy, and N2 adsorption‐desorption. The photocatalytic activities of the catalysts were evaluated in the degradation of 2,4‐dichlorophenol under ultraviolet irradiation. The photocatalytic activity of 50 wt%V2O5‐TiO2 （50V2O5‐TiO2） was higher than those of pure V2O5, TiO2, and P25. Interactions between V2O5 and TiO2 affected the photocatalytic efficiencies of the binary oxide catalysts. Cetyltrimethylammonium bromide （CTAB） and hexadecyltrimethylammonium bromide （HTAB） significantly enhanced the efficiency of the 50V2O5‐TiO2 catalyst. The highest per‐centage of 2,4‐dichlorophenol degradation （100%） and highest reaction rate （2.22 mg/（L·min）） were obtained in 30 min with the （50V2O5‐TiO2）‐CTAB catalyst. It is concluded that the addition of a surfactant to the binary oxide significantly enhanced the photocatalytic activity by modifying the optical and electronic properties of V2O5 and TiO2.展开更多
Herein,with the exploitation of iron and nickel electrodes,the 2,4-dichlorophenol(2,4-DCP)dechlorinating processes at the anode and cathode,respectively,were separately studied via various electrochemical techniques(e...Herein,with the exploitation of iron and nickel electrodes,the 2,4-dichlorophenol(2,4-DCP)dechlorinating processes at the anode and cathode,respectively,were separately studied via various electrochemical techniques(e.g.,Tafel polarization,linear polarization,electrochemical impedance spectroscopy).With this in mind,Ni/Fe nanoparticles were prepared by chemical solution deposition,and utilized to test the dechlorination activities of 2,4-DCP over a bimetallic system.For the iron anode,the results showed that higher 2,4-DCP concentration and solution acidity aggravated the corrosion within the electrode.The charge transfer resistance(Rct)values of the iron electrode were 703,473,444,and 437Ω·cm2 for the initial 2,4-DCP concentrations of0,20,50,and 80 mg/L,respectively.When the bulk pH of the 2,4-DCP solution varied from 3.0,5.0to 7.0,the corresponding Rct values were 315,376,and 444Ω·cm2,respectively.For the nickel cathode,the reduction current densities on the electrode at-0.75 V(vs.saturated calomel electrode)were 80,106,and 111μA/cm2,for initial 2,4-DCP concentrations of 40,80,and125 mg/L.The dechlorination experiments demonstrated that when the initial pH of the solution was 7.0,5.0,and 3.0,the dechlorination percentage of 2,4-DCP by Ni/Fe nanoparticles was 62%,69%,and 74%,respectively,which was in line with the electrochemical experiments.10 wt.%Ni loading into Ni/Fe bimetal was affordable and gave a good dechlorination efficiency of 2,4-DCP,and fortunately the Ni/Fe nanoparticles remained comparatively stable in the dechlorination processes at pH 3.0.展开更多
In this study,the performance of 3,5-dimethyl-2,4-dichlorophenol（DCMX） degradation by a screened strain was investigated.18 S r DNA and the neighbor-joining method were used for identification of the isolated strain...In this study,the performance of 3,5-dimethyl-2,4-dichlorophenol（DCMX） degradation by a screened strain was investigated.18 S r DNA and the neighbor-joining method were used for identification of the isolated strain.The results of phylogenetic analysis and scanning electron micrographs showed that the most probable identity of the screened strain should be Penicillium sp.Growth characteristics of Penicillium sp.and degradation processes of DCMX were examined.Fourier transform infrared spectroscopy of the inoculated DCMX solution was recorded,which supported the capacity of DCMX degradation by the screened Penicillium sp.Under different salinity conditions,the highest growth rate and removal efficiency for DCMX were obtained at p H 6.0.The removal efficiency decreased from 100%to 66% when the DCMX concentration increased from 5 to 60 mg/L,respectively.Using a Box–Behnken design,the maximum DCMX removal efficiency was determined to be 98.4%.With acclimation to salinity,higher removal efficiency could be achieved.The results demonstrate that the screened Penicillium sp.has the capability for degradation of DCMX.展开更多
Adsorption isotherms of 2,4-dinitrophenol and 2,4-dichlorophenol on hexadecyltrimethylammonium (HDTMA) bromide modified red soil under different ionic strength, divalent cation Cu 2+ or different pH conditions were st...Adsorption isotherms of 2,4-dinitrophenol and 2,4-dichlorophenol on hexadecyltrimethylammonium (HDTMA) bromide modified red soil under different ionic strength, divalent cation Cu 2+ or different pH conditions were studied. All the adsorption isotherms were well fitted to the Freundlich equation. The adsorption capacities of 2,4-dinitrophenol or 2,4-dichlorophenol were dramatically enhanced by HDTMA treatment of red soil. The increase of ionic strength and the addition of divalent heavy metal cation Cu 2+ significantly enhanced the adsorption of 2,4-dinitrophenol or 2,4-dichlorophenol on the HDTMA-modified red soil. Adsorption capacities of HDTMA-modified red soil for 2,4-dinitrophenol and 2,4-dichlorophenol gradually increased with decreasing pH in the aqueous phase.展开更多
2,4-Dichlorophenol was removed from wasterwater using a new hydrophobic poly（phthalazinone ether sulfone ketone） （PPESK） hollow fiber membrane by vacuum membrane distillation （VMD）.
A chemical system for facile and accurate detection of 2,4-dichlorophenol （DCP） via iron （Ⅱ） phthalocyanine （Fe（Ⅱ）Pc） catalyzed chromogenic reaction is reported for the first time. In this system, DCP could ...A chemical system for facile and accurate detection of 2,4-dichlorophenol （DCP） via iron （Ⅱ） phthalocyanine （Fe（Ⅱ）Pc） catalyzed chromogenic reaction is reported for the first time. In this system, DCP could be oxidized by dioxygen with the catalysis of Fe（Ⅱ）Pc and then coupled with 4-aminoantipyrine （4-AAP） to generate pink antipyrilquinoneimine dye. Control experiments showed that the addition of ethanol could obviously enhance the catalytic activity of heterogeneous Fe（Ⅱ）Pc catalysts because of the partial dissolution of Fe（II）Pc nanocubes, which was confirmed by the SEM analysis. On the basis of the detection results of DCP in the range from 2×10^-5 to 9×10^-4 mol/L, we obtained a regression equation （A = 0.187 5 ＋ 0.01 209C （R2=-0.995 6）） with the detection limit （3σ） of 3.26×10^-6 mol/L, which could be successfully used in detecting the real samples.展开更多
The remediation of groundwater which contains chlorinated organic compounds (COCs) by nanoscale bimetallic catalysts has received increasing interest in recent years. This report presents the dechlorination of 2,4-dic...The remediation of groundwater which contains chlorinated organic compounds (COCs) by nanoscale bimetallic catalysts has received increasing interest in recent years. This report presents the dechlorination of 2,4-dichlorophenol (2,4-DCP) by Pd-Fe bimetallic nanoparticles in the presence of humic acid (HA) to investigate the feasibility of using Pd-Fe for the in situ remediation of contaminated groundwater. Our experimental results indicated that HA had an adverse effect on the dechlorination of 2,4-DCP by Pd-Fe nanoparticles. The rate constant k values of 2,4-DCP dechlorination were 0.017, 0.013, 0.009, 0.006 and 0.004 min?1 for HA concentrations of 0, 5, 10, 15 and 20 mg/L, respectively. The relationship between HA dosage and k values can be described as a linear model.展开更多
A new fi ber optic sensor based on the oxidation of 2,4-dichlorophenol（DCP） catalyzed by iron（II） phthalocyanine（Fe（II）Pc） was developed for the determination of DCP. The optical oxygen sensing fi lm containin...A new fi ber optic sensor based on the oxidation of 2,4-dichlorophenol（DCP） catalyzed by iron（II） phthalocyanine（Fe（II）Pc） was developed for the determination of DCP. The optical oxygen sensing fi lm containing fl uorescence indicator Ru（bpy）3Cl2 was used to detect the consumption of oxygen in solution. Moreover, a lock-in amplifier was used to determine the lifetime of the sensor head by detecting its phase delay change. The results reveal that the sensor has a linear detection range of 1.0×10^-6- 9.0×10^-5 mol/L and a response time of 5 min. The sensor also has high selectivity, good repeatability and stability. It can be used effectively to determine DCP concentration in real samples.展开更多
Degradation of 2,4-dichlorophenol （2,4-DCP） was studied in a novel three-electrode photoelectrocatalytic （PEC） integrative oxidation process, and the factors influencing the degradation rate, such as applied curre...Degradation of 2,4-dichlorophenol （2,4-DCP） was studied in a novel three-electrode photoelectrocatalytic （PEC） integrative oxidation process, and the factors influencing the degradation rate, such as applied current, flow speed of O2, pH, adscititious voltage and initial 2,4-DCP concentration were investigated and optimized. H2O2 was produced nearby cathode and Fe^2＋ continuously generated from Fe anode in solution when current and O2 were applied, so, main reactions, H2O2-assisted TiO2 PEC oxidation and E-Fenton reaction, occurred during degradation of 2,4-DCP in this integrative system. The degradation ratio of 2,4-DCP was 93% in this integrative oxidation process, while it was only 31% in E-Fenton process and 46% in H2O2-assisted TiO2 PEC process. So, it revealed that the degradation of 2,4-DCP was improved greatly by photoelectrical cooperation effect. By the investigation of pH, it showed that this integrative process could work well in a wide pH range from pH 3 to pH 9.展开更多
A novel fiber optic sensor based on optical composite oxygen-sensitive film was developed for determination of 2,4-dichlorophenol(DCP).The optical composite oxygen-sensitive film consists of tris(2,2’-bipyridyl)dichl...A novel fiber optic sensor based on optical composite oxygen-sensitive film was developed for determination of 2,4-dichlorophenol(DCP).The optical composite oxygen-sensitive film consists of tris(2,2’-bipyridyl)dichloro ruthenium(II)hexahydrate(Ru(bpy)3Cl2)as the fluorescence indicator and iron(III)tetrasulfophthalocyanine(Fe(III)PcTs)as bionic enzyme.A lock-in amplifier was used for detecting the lifetime of the composite oxygen-sensitive film by measuring the phase delay of the sensor head.The different variables affecting the sensor performance were evaluated and optimized.Under the optimal conditions(i e,pH 6.0,25℃,Fe(III)PcTs concentration of 5.0×10^-5 mol/L),the linear detection range,detection limit and response time of the fiber optic sensor are 3.0×10^-7-9.0×10^-5 mol/L,4.8×10^-8 mol/L(S/N=3),and 220 s,respectively.The sensor displays high selectivity,good repeatability and stability,which have good potentials in analyzing DCP concentration in practical water samples.展开更多
Bimetallic nanoparticles modified hollow-structured nanoporous carbons(NPCs) have been fabricated via a convenient one-step carbonizing strategy derived from covalent organic framework.The Pd/Fe/NPCs,Pt/Fe/NPCs and Rh...Bimetallic nanoparticles modified hollow-structured nanoporous carbons(NPCs) have been fabricated via a convenient one-step carbonizing strategy derived from covalent organic framework.The Pd/Fe/NPCs,Pt/Fe/NPCs and Rh/Fe/NPCs were obtained and can be used as Fenton-like catalysts with good stability and reusability.The catalytic activity was evaluated by the degradation of2,4-dichlorophenl(2,4-DCP).These fabricated bimetallic catalysts exhibited much higher catalytic activity than Fe/NPCs at room temperature.The enhancement of catalytic ability was benefited from synergetic catalytic effect of bimetallic nanoparticles and accelerated mass transfer of hollow structure.Additionally,the enhanced catalytic mechanism of bimetallic catalysts was studied in detail and the reasonable reaction pathway was proposed.Besides,the bimetallic catalysts were successfully used for degradation of 2,4-DCP in actual industrial wastewater and the removal efficiency could reach 74.3%within 120 min,which demonstrated the promising potential application of bimetallic catalysts in the removal of pollutants in environment.展开更多
Laccase possesses a good degradation effect on organic pollutants,but it is too long to achieve the desired effect.In order to improve the treatment effect of laccase on degradation of organic pollutants,2,4-dichlorop...Laccase possesses a good degradation effect on organic pollutants,but it is too long to achieve the desired effect.In order to improve the treatment effect of laccase on degradation of organic pollutants,2,4-dichlorophenol(2,4-DCP)was selected as a treatment target in the study.This study investigated a newtechnique for catalyzing the degradation of 2,4-DCP,that is,ultrasound-assisted laccase catalysis.The optimal experimental parameters such as p H,ultrasonic power,duty cycle and laccase concentration were determined under optimized experimental conditions.The results showed that the optimum conditions for degradation of 2,4-DCP were that pH=5.5,the input power was 105 W,the duty cycle was 50%and the laccase concentration was0.4 U/m L.The degradation rate of 2,4-DCP reached 77.5%under the optimum conditions at 4 h.When in ultrasonic environment,the enzymatic activity of laccase could be stimulated and improved.Compared with conventional methods,this technique significantly promoted the degradation rate of 2,4-DCP while reduced action time.Furthermore,no newpollutant was introduced into the degradation process.Therefore,ultrasound-assisted laccase catalysis is an environmentally friendly technique to degrade pollutants.展开更多
Electrochemicaldegradation of2,4-dichlorophenol （2,4-DCP） in aqueous solutionwas investigated over Ti/SnO2-Sb anode. The factors influencing thedegradation rate, such as applied currentdensity （2-40 mA/cm2 ）, pH ...Electrochemicaldegradation of2,4-dichlorophenol （2,4-DCP） in aqueous solutionwas investigated over Ti/SnO2-Sb anode. The factors influencing thedegradation rate, such as applied currentdensity （2-40 mA/cm2 ）, pH （3-11） and initial concentration （5-200 mg/L）were evaluated. Thedegradation of2,4-DCP followed apparent pseudo first-order kinetics. Thedegradation ratio on Ti/SnO2 -Sb anode attained 〉 99.9% after 20 min of electrolysis at initial 5-200 mg/L concentrations at a constant currentdensity of 30 mA/cm2 with a 10 mmol/L sodium sulphate （Na2SO4 ） supporting electrolyte solution. The results showed that 2,4-DCP （100 mg/L）degradation and total organic carbon （TOC） removal ratio achieved 99.9% and 92.8%, respectively, at the optimal conditions after 30 min electrolysis. Under this condition, thedegradation rate constant （k） and thedegradation half-life （t1/2 ）were 0.21 min1 and （2.8 ± 0.2） min, respectively. Mainly carboxylic acids （propanoic acid, maleic acid, propanedioic acid, acetic acid and oxalic acid） weredetected as intermediates. The energy efficiencies for2,4-DCPdegradation （5-200 mg/L）with Ti/SnO2-Sb anode ranged from 0.672 to 1.602 g/kWh. The Ti/SnO2-Sb anodewith a high activity to rapid organic oxidation could be employed todegrade chlorophenols, particularly2,4-DCP inwastewater.展开更多
The paper presents comparative kinetic characteristics of the decomposition of 2,4-dichlorophenol in a dielectric barrier discharge and a combined plasma-catalytic process. Vermiculite containing 5% zirconium was used...The paper presents comparative kinetic characteristics of the decomposition of 2,4-dichlorophenol in a dielectric barrier discharge and a combined plasma-catalytic process. Vermiculite containing 5% zirconium was used as a catalyst. The destruction processes of 2,4-DCP proceed efficiently, the degree of decomposition increases in the combined plasma-catalytic process by a factor of 1.33 and reaches 80%. The experimental results were processed according to the first-order kinetic law (R<sup>2</sup> > 0.97), according to which the effective constants (0.36 ± 0.04) and (0.51 ± 0.03) s<sup>-1</sup> and the decomposition rates of 2,4-DCP (106 and 123 μmol/l·s) when treating model solutions without a catalyst and with vermiculite + Zr 5%, respectively, and the energy costs are 0.012 and 0.017 molecules/100eV. The main decomposition products present in the solution have been determined to be carboxylic acids, aldehydes, the contribution of which does not exceed 2%, as well as chloride ions, and in the gas phase they are carbon dioxide and molecular chlorine (the share of which does not exceed 1.5% of total chlorine content in the system).展开更多
基金supported by the Natural Science Foundation of Xinjiang Uygur Autonomous Region(No.2022D01C733)the Open Project of Key Disciplines of Physics(No.XJZDXKphy202309)the Research and Innovation Team Cultivation Program of Yili Normal University(No.CXZK2021004)。
文摘In this study,the cobalt-nickel layered double hydroxides(CoNi LDH)were synthesized with a variety of Co/Ni mass ratio,as CoxNiyLDHs.In comparison,Co1Ni3LDH presented the best peroxymonosulfate(PMS)activation efficiency for 2,4-dichlorophenol removal.Meanwhile,CoNi LDH@Nickel foam(CoNi LDH@NF)composite membrane was constructed for enhancing the stability of catalytic performance.Herein,CoNi LDH@NF-PMS system exerted high degradation efficiency of 99.22%within 90 min for 2,4-DCP when[PMS]_(0)=0.4 g/L,Co^(1)Ni^(3)LDH@NF=2 cm×2 cm(0.2 g/L),reaction temperature=298 K.For the surface morphology and structure of the catalyst,it was demonstrated that the CoNi LDH@NF composite membrane possessed abundant cavity structure,good specific surface area and sufficient active sites.Importantly,·OH,SO_(4)·^(-)and^(1)O_(2)played the primary role in the CoNi LDH@NF-PMS system for 2,4-DCP decomposition,which revealed the PMS activation mechanism in CoNi LDH@NF-PMS system.Hence,this study eliminated the stability and adaptability of CoNi LDH@NF composite membrane,proposing a new theoretical basis of PMS heterogeneous catalysts selection.
基金the National Natural Science Foundation of China(Nos.21677055 and 21407052)National Key Research and Development Program of China(2019YFC1805204)+1 种基金Project of Three Gorges Corporation(No.JDZC-FW-20-001)the Fundamental Research Funds for the Central Universities,HUST(Nos.2017KFXKJC004 and2016YXMS287)。
文摘This study demonstrated interesting ultrafast activation of molecular O_(2) by copper oxide(CuO)particles and very rapid elimination of aqueous 2,4-dichlo rophenol(2,4-DCP)within reaction time of 30 s.Electron paramagnetic resonance(EPR)characterization indicated that·OH,Cu^(3+),^1 O_(2) and O_(2)^·-were generated in the CuO/O_(2) systems,wherein O_(2)^·-would be the main reactive species responsible for 2,4-DCP degradation.It was further found that the catalytic ability of CuO for O_(2) activation was highly size dependent and nano-CuO was far reactive than micro-CuO.H2 temperature-programmed reduction(H2-TPR),X-ray photoelectron spectroscopy(XPS)and vibrating sample magnetometer(VSM)analyses revealed that both the quantity and the reactivity of the surface reaction sites(surface Cu+and O_(2))could determine the catalytic ability of CuO affecting efficient Cu^(+)-based molecular oxygen activation.Moreover,the O_(2) activation ability of CuO would depend on not only the dimension,but also crystalline factors,for example,the exposed facets.
基金Project supported by the National Natural Science Foundation of China(No.20407015)the Program for New Century Excellent Talents in University(No.NCET-06-0525),China
文摘To understand the feasibility of its application to the in situ remediation of contaminated groundwater,the dechlori-nation of 2,4-dichlorophenol (2,4-DCP) by Ni/Fe nanoparticles in the presence of humic acid (HA) was investigated.We found that,as high performance liquid chromatography (HPLC) was used,the 2,4-DCP was first quickly reduced to o-chlorophenol (o-CP) and p-chlorophenol (p-CP),and then reduced to phenol as the final product.Our experimental results indicated that HA had an adverse effect on the dechlorination of 2,4-DCP by Ni/Fe nanoparticles,as the HA concentration increased,the removal rate decreased evidently.It also demonstrated that 2,4-DCP was reduced more easily to o-CP than to p-CP,and that the sequence of the tendency in dechlorination of intermediates was p-CP>o-CP.Transmission electron microscope (TEM) showed that HA could act as an adsorbate to compete reactive sites on the surface of Ni/Fe nanoparticles to decrease the dechlorination rate.Also we con-cluded that the dechlorination reaction of 2,4-DCP over Ni/Fe nanoparticles progressed through catalytic reductive dechlorination.
文摘The adsorption capacity of activated carbon produced from oil palm empty fruit bunches through removal of 2,4-dichlorophenol from aqueous solution was carried out in the laboratory. The activated carbon was produced by thermal activation of activation time with 30 min at 800℃. The adsorption process conditions were determined with the statistical optimization followed by central composite design. A developed polynomial model for operating conditions of adsorption process indicated that the optimum conditions for maximum adsorption of phenolic compound were： agitation rate of 100 r/min, contact time of 8 h, initial adsorbate concentration of 250 mg/L and pH 4. Adsorption isotherms were conducted to evaluate biosorption process. Langmuir isotherm was more favorable （R^2=0.93） for removal of 2,4-dichlorophenol by the activated carbon rather than Freundlich isotherm （R^2=0.88）.
基金This work was supported by the Educational Bureau (No.05KJD610250)the Science & Technology Bureau (No. BS2006032) of Jiangsu Province, China.
文摘A hypercrosslinked adsorption resin （ZH-05） modified by N-acetylaniline in the post crosslinking process was prepared. The adsorption properties of ZH-05 toward 2,4-dichlorophenol in comparison with granular activated carbon （GAC） and Amberlite XAD-4 were observed. The present study mainly focuses on the static equilibrium adsorption behaviors, desorption profiles and the proof of chemisorption. The results show that the Langmuir equation can give a perfect fitting to experimental data, and high temperature was favorable for adsorption of 2,4-dichlorophenol on ZH-05. A related equation was used to correlate the amount of chemisorption and the suppositionai chemisorption equilibrium concentration of adsorbate in aqueous solution. The adsorption capacities from different ranges of temperature and the static desorption experiment both reveal the same conclusion, i.e., the adsorption of 2,4-dichlorophenol from water on ZH-05 is a coexistent process of physical adsorption and chemical transition as on GAC.
基金supported by The Scientific and Technological Research Council of Turkey(TUBITAK)within the research project 111M210[2011-2013]~~
文摘Binary oxide catalysts with various weight percentage V2O5 loadings were prepared by solid‐state dispersion and the nanocomposites were modified with surfactants. The catalysts were analyzed using X‐ray diffraction, diffuse‐reflectance spectroscopy, Fourier‐transform infrared spectroscopy, scanning electron microscopy, and N2 adsorption‐desorption. The photocatalytic activities of the catalysts were evaluated in the degradation of 2,4‐dichlorophenol under ultraviolet irradiation. The photocatalytic activity of 50 wt%V2O5‐TiO2 （50V2O5‐TiO2） was higher than those of pure V2O5, TiO2, and P25. Interactions between V2O5 and TiO2 affected the photocatalytic efficiencies of the binary oxide catalysts. Cetyltrimethylammonium bromide （CTAB） and hexadecyltrimethylammonium bromide （HTAB） significantly enhanced the efficiency of the 50V2O5‐TiO2 catalyst. The highest per‐centage of 2,4‐dichlorophenol degradation （100%） and highest reaction rate （2.22 mg/（L·min）） were obtained in 30 min with the （50V2O5‐TiO2）‐CTAB catalyst. It is concluded that the addition of a surfactant to the binary oxide significantly enhanced the photocatalytic activity by modifying the optical and electronic properties of V2O5 and TiO2.
基金supported by the National Natural Science Foundation of China (No. 51325102)the Nature Science Foundation of Hubei Province of China (Team Project, No. 2015CFA017)
文摘Herein,with the exploitation of iron and nickel electrodes,the 2,4-dichlorophenol(2,4-DCP)dechlorinating processes at the anode and cathode,respectively,were separately studied via various electrochemical techniques(e.g.,Tafel polarization,linear polarization,electrochemical impedance spectroscopy).With this in mind,Ni/Fe nanoparticles were prepared by chemical solution deposition,and utilized to test the dechlorination activities of 2,4-DCP over a bimetallic system.For the iron anode,the results showed that higher 2,4-DCP concentration and solution acidity aggravated the corrosion within the electrode.The charge transfer resistance(Rct)values of the iron electrode were 703,473,444,and 437Ω·cm2 for the initial 2,4-DCP concentrations of0,20,50,and 80 mg/L,respectively.When the bulk pH of the 2,4-DCP solution varied from 3.0,5.0to 7.0,the corresponding Rct values were 315,376,and 444Ω·cm2,respectively.For the nickel cathode,the reduction current densities on the electrode at-0.75 V(vs.saturated calomel electrode)were 80,106,and 111μA/cm2,for initial 2,4-DCP concentrations of 40,80,and125 mg/L.The dechlorination experiments demonstrated that when the initial pH of the solution was 7.0,5.0,and 3.0,the dechlorination percentage of 2,4-DCP by Ni/Fe nanoparticles was 62%,69%,and 74%,respectively,which was in line with the electrochemical experiments.10 wt.%Ni loading into Ni/Fe bimetal was affordable and gave a good dechlorination efficiency of 2,4-DCP,and fortunately the Ni/Fe nanoparticles remained comparatively stable in the dechlorination processes at pH 3.0.
基金supported by the International S&T Cooperation Program of China(No.2015DFG92750)the National Natural Science Foundation of China(Nos.51478172 and 51278464)the Natural Science Foundation of Zhejiang Province of China(No.LY17E080002)
文摘In this study,the performance of 3,5-dimethyl-2,4-dichlorophenol（DCMX） degradation by a screened strain was investigated.18 S r DNA and the neighbor-joining method were used for identification of the isolated strain.The results of phylogenetic analysis and scanning electron micrographs showed that the most probable identity of the screened strain should be Penicillium sp.Growth characteristics of Penicillium sp.and degradation processes of DCMX were examined.Fourier transform infrared spectroscopy of the inoculated DCMX solution was recorded,which supported the capacity of DCMX degradation by the screened Penicillium sp.Under different salinity conditions,the highest growth rate and removal efficiency for DCMX were obtained at p H 6.0.The removal efficiency decreased from 100%to 66% when the DCMX concentration increased from 5 to 60 mg/L,respectively.Using a Box–Behnken design,the maximum DCMX removal efficiency was determined to be 98.4%.With acclimation to salinity,higher removal efficiency could be achieved.The results demonstrate that the screened Penicillium sp.has the capability for degradation of DCMX.
文摘Adsorption isotherms of 2,4-dinitrophenol and 2,4-dichlorophenol on hexadecyltrimethylammonium (HDTMA) bromide modified red soil under different ionic strength, divalent cation Cu 2+ or different pH conditions were studied. All the adsorption isotherms were well fitted to the Freundlich equation. The adsorption capacities of 2,4-dinitrophenol or 2,4-dichlorophenol were dramatically enhanced by HDTMA treatment of red soil. The increase of ionic strength and the addition of divalent heavy metal cation Cu 2+ significantly enhanced the adsorption of 2,4-dinitrophenol or 2,4-dichlorophenol on the HDTMA-modified red soil. Adsorption capacities of HDTMA-modified red soil for 2,4-dinitrophenol and 2,4-dichlorophenol gradually increased with decreasing pH in the aqueous phase.
文摘2,4-Dichlorophenol was removed from wasterwater using a new hydrophobic poly（phthalazinone ether sulfone ketone） （PPESK） hollow fiber membrane by vacuum membrane distillation （VMD）.
基金Funded by the National Natural Science Foundation of China(No.61377092)
文摘A chemical system for facile and accurate detection of 2,4-dichlorophenol （DCP） via iron （Ⅱ） phthalocyanine （Fe（Ⅱ）Pc） catalyzed chromogenic reaction is reported for the first time. In this system, DCP could be oxidized by dioxygen with the catalysis of Fe（Ⅱ）Pc and then coupled with 4-aminoantipyrine （4-AAP） to generate pink antipyrilquinoneimine dye. Control experiments showed that the addition of ethanol could obviously enhance the catalytic activity of heterogeneous Fe（Ⅱ）Pc catalysts because of the partial dissolution of Fe（II）Pc nanocubes, which was confirmed by the SEM analysis. On the basis of the detection results of DCP in the range from 2×10^-5 to 9×10^-4 mol/L, we obtained a regression equation （A = 0.187 5 ＋ 0.01 209C （R2=-0.995 6）） with the detection limit （3σ） of 3.26×10^-6 mol/L, which could be successfully used in detecting the real samples.
基金Project supported by the National Natural Science Foundation of China (No. 20407015)the Program for the New Century Excel-lent Talents in University (No. NCET-06-0525), China
文摘The remediation of groundwater which contains chlorinated organic compounds (COCs) by nanoscale bimetallic catalysts has received increasing interest in recent years. This report presents the dechlorination of 2,4-dichlorophenol (2,4-DCP) by Pd-Fe bimetallic nanoparticles in the presence of humic acid (HA) to investigate the feasibility of using Pd-Fe for the in situ remediation of contaminated groundwater. Our experimental results indicated that HA had an adverse effect on the dechlorination of 2,4-DCP by Pd-Fe nanoparticles. The rate constant k values of 2,4-DCP dechlorination were 0.017, 0.013, 0.009, 0.006 and 0.004 min?1 for HA concentrations of 0, 5, 10, 15 and 20 mg/L, respectively. The relationship between HA dosage and k values can be described as a linear model.
基金Funded by the National Natural Science Foundation of China(Nos.61377092 and 51303115)
文摘A new fi ber optic sensor based on the oxidation of 2,4-dichlorophenol（DCP） catalyzed by iron（II） phthalocyanine（Fe（II）Pc） was developed for the determination of DCP. The optical oxygen sensing fi lm containing fl uorescence indicator Ru（bpy）3Cl2 was used to detect the consumption of oxygen in solution. Moreover, a lock-in amplifier was used to determine the lifetime of the sensor head by detecting its phase delay change. The results reveal that the sensor has a linear detection range of 1.0×10^-6- 9.0×10^-5 mol/L and a response time of 5 min. The sensor also has high selectivity, good repeatability and stability. It can be used effectively to determine DCP concentration in real samples.
基金Project supported by the Hong Kong Government Research Grant Committee(RGC No.PolyU5148/03E).
文摘Degradation of 2,4-dichlorophenol （2,4-DCP） was studied in a novel three-electrode photoelectrocatalytic （PEC） integrative oxidation process, and the factors influencing the degradation rate, such as applied current, flow speed of O2, pH, adscititious voltage and initial 2,4-DCP concentration were investigated and optimized. H2O2 was produced nearby cathode and Fe^2＋ continuously generated from Fe anode in solution when current and O2 were applied, so, main reactions, H2O2-assisted TiO2 PEC oxidation and E-Fenton reaction, occurred during degradation of 2,4-DCP in this integrative system. The degradation ratio of 2,4-DCP was 93% in this integrative oxidation process, while it was only 31% in E-Fenton process and 46% in H2O2-assisted TiO2 PEC process. So, it revealed that the degradation of 2,4-DCP was improved greatly by photoelectrical cooperation effect. By the investigation of pH, it showed that this integrative process could work well in a wide pH range from pH 3 to pH 9.
基金Funded by the National Natural Science Foundation of China(No.61205062)the Scientific Research Foundation for Doctor of University(No.2019Y02)。
文摘A novel fiber optic sensor based on optical composite oxygen-sensitive film was developed for determination of 2,4-dichlorophenol(DCP).The optical composite oxygen-sensitive film consists of tris(2,2’-bipyridyl)dichloro ruthenium(II)hexahydrate(Ru(bpy)3Cl2)as the fluorescence indicator and iron(III)tetrasulfophthalocyanine(Fe(III)PcTs)as bionic enzyme.A lock-in amplifier was used for detecting the lifetime of the composite oxygen-sensitive film by measuring the phase delay of the sensor head.The different variables affecting the sensor performance were evaluated and optimized.Under the optimal conditions(i e,pH 6.0,25℃,Fe(III)PcTs concentration of 5.0×10^-5 mol/L),the linear detection range,detection limit and response time of the fiber optic sensor are 3.0×10^-7-9.0×10^-5 mol/L,4.8×10^-8 mol/L(S/N=3),and 220 s,respectively.The sensor displays high selectivity,good repeatability and stability,which have good potentials in analyzing DCP concentration in practical water samples.
基金supported by the National Natural Science Foundation of China (Nos.21675178,21775167 and 21976213)the National Key Research and Development Program of China(No.2019YFC1606101)the Research and Development Plan for Key Areas of Food Safety in Guangdong Province of China (No.2019B020211001),respectively。
文摘Bimetallic nanoparticles modified hollow-structured nanoporous carbons(NPCs) have been fabricated via a convenient one-step carbonizing strategy derived from covalent organic framework.The Pd/Fe/NPCs,Pt/Fe/NPCs and Rh/Fe/NPCs were obtained and can be used as Fenton-like catalysts with good stability and reusability.The catalytic activity was evaluated by the degradation of2,4-dichlorophenl(2,4-DCP).These fabricated bimetallic catalysts exhibited much higher catalytic activity than Fe/NPCs at room temperature.The enhancement of catalytic ability was benefited from synergetic catalytic effect of bimetallic nanoparticles and accelerated mass transfer of hollow structure.Additionally,the enhanced catalytic mechanism of bimetallic catalysts was studied in detail and the reasonable reaction pathway was proposed.Besides,the bimetallic catalysts were successfully used for degradation of 2,4-DCP in actual industrial wastewater and the removal efficiency could reach 74.3%within 120 min,which demonstrated the promising potential application of bimetallic catalysts in the removal of pollutants in environment.
基金National Natural Science Foundation of China(No.41571306)the Project of Excellent Fund in Hubei Province,China(No.2018CFA067)Hubei Key Laboratory for Efficient Utilization and Agglomeration of Metallurgic Mineral Resources,China(No.2017zy003)
文摘Laccase possesses a good degradation effect on organic pollutants,but it is too long to achieve the desired effect.In order to improve the treatment effect of laccase on degradation of organic pollutants,2,4-dichlorophenol(2,4-DCP)was selected as a treatment target in the study.This study investigated a newtechnique for catalyzing the degradation of 2,4-DCP,that is,ultrasound-assisted laccase catalysis.The optimal experimental parameters such as p H,ultrasonic power,duty cycle and laccase concentration were determined under optimized experimental conditions.The results showed that the optimum conditions for degradation of 2,4-DCP were that pH=5.5,the input power was 105 W,the duty cycle was 50%and the laccase concentration was0.4 U/m L.The degradation rate of 2,4-DCP reached 77.5%under the optimum conditions at 4 h.When in ultrasonic environment,the enzymatic activity of laccase could be stimulated and improved.Compared with conventional methods,this technique significantly promoted the degradation rate of 2,4-DCP while reduced action time.Furthermore,no newpollutant was introduced into the degradation process.Therefore,ultrasound-assisted laccase catalysis is an environmentally friendly technique to degrade pollutants.
基金supported by the National Science Foundation for Innovative Research Group of China(No.51121003)the Specialized Research Fund for the Doctoral Program of Higher Education of China(No.20110003110023)the special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control of China
文摘Electrochemicaldegradation of2,4-dichlorophenol （2,4-DCP） in aqueous solutionwas investigated over Ti/SnO2-Sb anode. The factors influencing thedegradation rate, such as applied currentdensity （2-40 mA/cm2 ）, pH （3-11） and initial concentration （5-200 mg/L）were evaluated. Thedegradation of2,4-DCP followed apparent pseudo first-order kinetics. Thedegradation ratio on Ti/SnO2 -Sb anode attained 〉 99.9% after 20 min of electrolysis at initial 5-200 mg/L concentrations at a constant currentdensity of 30 mA/cm2 with a 10 mmol/L sodium sulphate （Na2SO4 ） supporting electrolyte solution. The results showed that 2,4-DCP （100 mg/L）degradation and total organic carbon （TOC） removal ratio achieved 99.9% and 92.8%, respectively, at the optimal conditions after 30 min electrolysis. Under this condition, thedegradation rate constant （k） and thedegradation half-life （t1/2 ）were 0.21 min1 and （2.8 ± 0.2） min, respectively. Mainly carboxylic acids （propanoic acid, maleic acid, propanedioic acid, acetic acid and oxalic acid） weredetected as intermediates. The energy efficiencies for2,4-DCPdegradation （5-200 mg/L）with Ti/SnO2-Sb anode ranged from 0.672 to 1.602 g/kWh. The Ti/SnO2-Sb anodewith a high activity to rapid organic oxidation could be employed todegrade chlorophenols, particularly2,4-DCP inwastewater.
文摘The paper presents comparative kinetic characteristics of the decomposition of 2,4-dichlorophenol in a dielectric barrier discharge and a combined plasma-catalytic process. Vermiculite containing 5% zirconium was used as a catalyst. The destruction processes of 2,4-DCP proceed efficiently, the degree of decomposition increases in the combined plasma-catalytic process by a factor of 1.33 and reaches 80%. The experimental results were processed according to the first-order kinetic law (R<sup>2</sup> > 0.97), according to which the effective constants (0.36 ± 0.04) and (0.51 ± 0.03) s<sup>-1</sup> and the decomposition rates of 2,4-DCP (106 and 123 μmol/l·s) when treating model solutions without a catalyst and with vermiculite + Zr 5%, respectively, and the energy costs are 0.012 and 0.017 molecules/100eV. The main decomposition products present in the solution have been determined to be carboxylic acids, aldehydes, the contribution of which does not exceed 2%, as well as chloride ions, and in the gas phase they are carbon dioxide and molecular chlorine (the share of which does not exceed 1.5% of total chlorine content in the system).
