Radiation-induced degradation of methyl orange in aqueous solutions

Degradation of methyl orange under gamma-irradiation was investigated. The reactions followed pseudo first-order kinetics. Apparent degradation rate constant, estimated through linear regression analysis, increased with an increase of dose rate and a decrease of initial methyl orange concentration. Degradation of methyl orange was significantly accelerated under oxidative condition, but was slightly enhanced under reductive condition. However, the result of decoloration was better under reductive condition than oxidative one. An analysis on the intermediates using Fourier transform infrared and gas chromatography/mass spectrometry demonstrates that the radiolytic degradation of methyl orange was processed with different C-N cleavages under oxidative and reductive conditions.     

微波再生载苯酚活性炭过程中再生产物分析

研究了载氮气和无载气2种条件下,微波再生载苯酚活性炭过程中再生产物的成分和苯酚随再生过程的去向分布。结果表明,无载气时,微波功率越高,再生反应器内温度越高,吸附质的高温裂解反应越彻底,再生产物以挥发性气体为主,有机质种类很少;而当微波功率较低或载氮气再生时,反应器内温度相对较低,苯酚难以被彻底分解,再生产物中含多种复杂的链状或环状有机物。此外,载氮气时,经气提、挥发而去除的苯酚量约占总吸附量的一半,再生炭上无苯酚残留,活性炭吸附性能可完全恢复乃至优化;无载气时,经挥发而去除的苯酚量只有19.9%,其余大量苯酚则在微波作用下裂解或缩合为其他物质随尾气而去除,且再生炭上仍有少量苯酚未被解吸出来。因此,前者活性炭再生的效果优于后者。     

活性炭/聚丙烯腈纤维对溶液中的甲基橙染料吸附动力学研究

采用自制添加活性炭的聚丙烯腈纤维为吸附剂,吸附染料甲基橙溶液,考察了活性炭含量、温度及溶液pH值等因素对纤维吸附染料甲基橙吸附量和吸附速率的影响.结果表明,活性炭/聚丙烯腈纤维吸附甲基橙染料符合表观二级动力学方程.吸附过程的限速步骤为甲基橙染料向活性炭/聚丙烯腈纤维中活性炭颗粒内部微孔扩散,自制的活性炭/聚丙烯腈纤维对甲基橙染料具有较大的吸附容量和较快的吸附速率,可作为甲基橙等染料废水治理的理想材料.     

Photocatalytic oxidation of methyl orange in a three-phase fluidized bed reactor

The photocatalytic oxidation of methyl orange under weak illumination conditions was carried out in two different types of fluidized bed reactors. TiO2 powder was employed as the photocatalysts and a 15 W low pressure mercury lamp was used as the light source and the reactor volume was 2.5 l. The parametric study of photocatalytic oxidation of methyl orange in two different types of fluidized beds was investigated; effect of catalyst loadings, pH, air flow rate, initial concentration and oxygen concentration on the oxidation reaction rate. The experimental results were analyzed in conjunction with the characteristics of fluidized bed and the reactor geometry effect on the reaction rate was analyzed.     

铁炭微电解-Fe~（2＋）/K_2S_2O_8降解甲基橙

针对偶氮类有机物废水具有色度大,难降解的特点,以对二甲基氨基偶氮苯磺酸钠（甲基橙）为模拟研究对象,对水体系中铁炭微电解-Fe2＋/K2S2O8降解甲基橙的方法进行了研究。通过正交实验确定出该方法各因素的影响程度,进一步通过单因素影响实验确定该方法的最佳条件是：铁炭微电解填料、FeSO4和K2S2O8投加量分别为300 g/L、1.3mmol/L和0.7 mmol/L,初始pH值为7.0。在最佳条件下,甲基橙COD和色度去除率分别能达到64.7%和68.2%。     

多壁碳纳米管结构对复合光催化剂催化效果的影响

采用溶胶凝胶法制备了多壁碳纳米管负载纳米TiO₂的复合光催化剂（TiO₂/MWCNTs）,以偶氮类染料甲基橙为目标污染物,在自制的光催化反应器上进行了光催化降解反应实验。主要研究同一甲基橙初始浓度（C₀)下,多壁碳纳米管不同管长和管径对复合光催化剂催化效果的影响。结果表明：该降解反应可用一级反应动力学方程描述,反应速率常数k随着多壁碳纳米管管长和管径的增大而增大;与纯纳米TiO₂相比,复合光催化剂对甲基橙的降解率提高了6％～18％,反应速率常数为前者的1.19～2.11倍;采用复合光催化剂的甲基橙光降解溶液自行沉降分离效果较好,静止沉降60 min后达到沉降平衡,剩余浊度为8.5 NTU,下降了90.6％。     

微波改性活性炭的吸附性能

利用微波辐照技术代替传统的加热技术在N2 气中对煤质活性炭进行改性 ,以期提高活性炭的吸附性能。通过正交实验法 ,探讨了微波功率、辐照时间及样品粒径 3种因素对改性活性炭吸附效果的影响。结果表明 ,微波加热提高了活性炭的吸附能力 ,微波功率和辐照时间是决定改性活性炭吸附性能的关键因素 ,并通过对改性前后活性炭的孔隙结构和微结构变化进行分析 ,来讨论其改性机理。     

Adsorption of Cu2+ and methyl orange from aqueous solutions by activated carbons of corncob-derived char wastes

Corncob-derived char wastes (CCW) obtained from biomass conversion to syngas production through corncob steam gasification, which were often discarded, were utilized for preparation of activated carbon by calcination, and KOH and HNO₃ activation treatments, on the view of environment protection and waste recycling. Their adsorption performance in the removal of heavy metal ions and dye molecules from wastewater was evaluated by using Cu²⁺ and methyl orange (MO) as the model pollutant. The surface and structure characteristics of the CCW-based activated carbons (CACs) were investigated by N₂ adsorption, CO₂ adsorption, FT-IR, and He-TPD. The adsorption capacity varied with the activation methods of CACs and different initial solution concentrations, indicating that the adsorption behavior was influenced by not only the surface area and porosity but also the oxygen functional groups on the surface of the CACs. The equilibrium adsorption data were analyzed with the Langmuir, Freundlich, and Temkin isotherm models, and the adsorption kinetics was evaluated by the pseudo-first-order and pseudo-second-order models.     

黄麻纤维活性炭对亚甲基蓝和甲基橙吸附动力学

以黄麻纤维为原料,采用磷酸活化法制备活性炭。研究黄麻纤维活性炭对亚甲基蓝和甲基橙2种染料的吸附行为。结果表明,采用磷酸制备的活性炭,由于表面含有羧基和含磷官能团等酸性基团,能够促进活性炭对亚甲基蓝的吸附;黄麻纤维活性炭对2种染料的平衡吸附量、初始吸附速率均随着初始浓度的增加而升高;相同条件下,黄麻纤维活性炭对亚甲基蓝的平衡吸附量大于甲基橙;黄麻纤维活性炭对两种染料的吸附行为更符合准二级动力学模型。     

Degradation mechanism and the toxicity assessment in TiO2 photocatalysis and photolysis of parathion

The photocatalytic degradation of methyl parathion was carried out using a circulating TiO2/UV reactor. The experimental results showed that parathion was more effectively degraded in the photocatalytic condition than the photolysis and TiO2-only condition. With photocatalysis, 10mg/l parathion was completely degraded within 60 min with a TOC decrease exceeding 90% after 150 min. The main ionic byproducts during photocatalysis were measured. The nitrogen from parathion was recovered mainly as NO3-, NO2- and NH4+, 80% of the sulfur as SO4(2-), and less than 5% of the phosphorus as PO4(3-). The organic intermediates 4-nitrophenol and paraoxon were also identified, and these were further degraded. Two different bioassays (Vibrio fischeri and Daphnia magna) were used to test the acute toxicity of solutions treated by photocatalysis and photolysis. A Microtox test using V. fischeri showed that the toxicity, expressed as the relative toxicity (%), was reduced almost completely after 90 min under photocatalysis, whereas only an 83% reduction was achieved with photolysis alone. Another toxicity test using D. magna also showed that the relative toxicity disappeared after 90 min under photocatalysis, whereas there was a 65% reduction in relative toxicity with photolysis alone. The pattern of toxicity reduction parallels the decrease in parathion and TOC concentrations.     

铁炭微电解-Fe2+/K2S2O8降解甲基橙

针对偶氮类有机物废水具有色度大,难降解的特点,以对二甲基氨基偶氮苯磺酸钠(甲基橙)为模拟研究对象,对水体系中铁炭微电解-Fe2+/K2S2O8降解甲基橙的方法进行了研究。通过正交实验确定出该方法各因素的影响程度,进一步通过单因素影响实验确定该方法的最佳条件是:铁炭微电解填料、FeSO4和K2S2O8投加量分别为300 g/L、1.3mmol/L和0.7 mmol/L,初始pH值为7.0。在最佳条件下,甲基橙COD和色度去除率分别能达到64.7%和68.2%。     

Combined effect of microwave and activated carbon on the remediation of polychlorinated biphenyl-contaminated soil

The application of microwave and activated carbon for the treatment of polychlorinated biphenyl (PCB) contaminated soil was explored in this study with a model compound of 2,4,5-trichlorobiphenyl (PCB29). PCB-contaminated soil was treated in a quartz reactor by microwave irradiation at 2450MHz with the addition of granular activated carbon (GAC). In this procedure, GAC acted as microwave absorbent for reaching high temperature and reductant for dechlorination. A sheltered type-K thermocouple was applied to record the temperature rising courses. It was shown that the addition of GAC could effectively promote the temperature rising courses. The determination of PCB residues in soil by gas chromatography (GC) revealed that rates of PCB removal were highly dependent on microwave power, soil moisture content, and the amount of GAC added. GC with mass spectrum (MS) detector and ion chromatography were employed for the analysis of degradation intermediates and chlorine ions, respectively. It was suggested that microwave irradiation with the assistance of activated carbon might be a potential technology for the remediation of PCB-contaminated soil.     

The mechanism and kinetics of ultrasound-enhanced electrochemical oxidation of phenol on boron-doped diamond and Pt electrodes

The research on ultrasound (US) enhanced electrochemical oxidation of Phenol (Ph) on boron-doped diamond (BDD) and Pt electrodes is studied. The enhancement by US on BDD is much greater than for Pt. With the assistance of US, the degradation rate and current efficiency on BDD are increased by 301% and 100%, respectively, while those on Pt are 51% and 49%. The difference of the enhancement on these two electrodes is caused by the fact that mass transport, adsorption amount and electrode reaction affected by US on BDD are different from those of Pt. The kinetics investigation on intermediates formed during electrochemical degradation show that the variety of intermediates produced on BDD is less than for Pt. In the presence of US, on both electrodes, no change occurred to the amounts of the intermediate species. However, time for intermediates to reach the highest concentration is cut down. This effect for degradation of Ph on BDD is more obvious than for Pt. The present research indicates that BDD is suitable for degradation of Ph by US assisted electrochemical oxidation.     

Ultrasound enhanced activation of peroxydisulfate by activated carbon fiber for decolorization of azo dye

Activated carbon fiber (ACF) has become an emerging activator for peroxydisulfate (PDS) to generate sulfate radical (SO₄^??). However, the relative low activation efficiency and poor contaminant mineralization limited its widespread application. Herein, ultrasound (US) was introduced to the ACF activated PDS system, and the synergistic effect of US and ACF in PDS activation and the enhancement of contaminant mineralization were investigated. The synergistic effect of US and ACF was observed in the PDS activation to decolorize orange G (OG). The decolorization efficiency increased with increasing ACF loading and US power, and PDS/OG ratio from 1 to 40. The activation energy was determined to be 24.065 kJ/mol. The radical-induced decolorization of OG took place on the surface of ACF, and both SO₄^?? and hydroxyl radical (^?OH) contributed to OG decolorization. The azo bond and naphthalene ring on OG were destructed to other aromatic intermediates and finally mineralized to CO₂ and H₂O. The introduction of US in the ACF/PDS system significantly enhanced the mineralization of OG. The combination of US and PDS was highly efficient to activate PDS to decolorize azo dyes. Moreover, the introduction of US remarkably improved the contaminant mineralization.     

废活性炭微波再生新工艺的研究

提出用微波加热-二氧化碳活化法再生乙酸乙烯合成用触媒载体废活性炭工艺.采用条件实验法研究了活化时间、二氧化碳流量和微波功率对活性炭碘吸附值,亚甲基蓝吸附值和再生得率的影响,得到微波辐射加热二氧化碳活化再生乙酸乙烯用触媒载体废活性炭的最佳工艺条件为活化时间25 min,二氧化碳流量0.2 L/min,微波功率700 W.在此条件下制得的活性炭碘吸附值为1158.02 mg/g、亚甲基蓝吸附值为240 mg/g、得率为74.19%.并对活性炭进行了比表面积的测定和孔结构的分析,活性炭的比表面积为1308.13 m2/g,总孔容为0.76 mL/g.     

The enhancement of photodegradation efficiency using Pt–TiO2 catalyst

This study investigates the mechanism of photosensitization and the recombination of excited electron–hole pairs affected by depositing platinum (Pt) on the surface of titanium dioxide (TiO₂). A new catalyst of Pt–TiO₂ was prepared by a photoreduction process. Being model reactions, the photocatalytic oxidation of methylene blue (MB) and methyl orange (MO) in aqueous solutions using the Pt–TiO₂ catalyst was carried out under either UV or visible light irradiation. The experimental results indicate that an optimal content of 0.75%Pt–TiO₂ achieves the best photocatalytic performance of MB and MO degradation and that the Pt–TiO₂ catalyst can be sensitized by visible light. The interaction of Pt and TiO₂ was investigated by means of UV–Vis absorption spectra, photoluminescence emission spectra, and X-ray photoelectron emission spectroscopy. The Pt⁰, Pt²⁺ and Pt⁴⁺ species existing on the surface of Pt–TiO₂, and the Ti³⁺ species existing in its lattice may form a defect energy level. The Pt impurities, including Pt, Pt(OH)₂, and PtO₂, and the defect energy level absorb visible light more efficiently in comparison with the pure TiO₂ and hinder the recombination rate of excited electron–hole pairs.     

In situ remediation of soils contaminated with toxic metal ions using microwave energy

Following onto our work on the in situ remediation of soils contaminated with PAH's, PCB's and other polychlorinated organic compounds using microwave energy, we now report a preliminary investigation on the in situ remediation of soils contaminated with toxic metal ions: Cd(II), Mn(II), Th(IV), Cr(III) and mainly Cr(VI). The soil is partially vitrified in the process, and extraction with hot (70 degrees C) 35% nitric acid for 4.5 h leads to the recovery of very small amounts of the metals which had been spiked into the clean soil: Cd, Mn, and Cr(III) are completely immobilized (unextractable), Th is mostly unextractable, and Cr(VI) partially extractable at very high levels of spiking, but almost completely unextractable using the US EPA Toxicity Characteristic Leaching Procedure. This suggests that contaminated soils which are not going to be used for agricultural purposes can be remediated safely to preset depths without fear of the toxic metal ions leaching out for a long time.     

微波促进含Cr(VI)-H2O2体系降解甲基橙溶液的研究

研究了微波辐射下Cr(VI)－H₂O₂催化降解甲基橙溶液的行为，探索了微波功率、微波辐射时间、pH值、H₂O₂浓度、Cr(VI)等对甲基橙溶液脱色率和COD去除率的影响。研究结果表明，Cr(VI)-H₂O₂能形成类Fenton体系；微波辐射可提高H₂O₂产生羟基自由基(·OH)的效率。1000 mg/L的甲基橙溶液，在Cr(VI)浓度为10.0 mmol/L、pH值为2.5、H₂O₂浓度为20.0 mmol/L、微波功率为700W下加热2 min，甲基橙溶液的脱色率为99.2%，COD去除率为82.8%。     

CuFe2O4/activated carbon composite: a novel magnetic adsorbent for the removal of acid orange II and catalytic regeneration

CuFe2O4/activated carbon magnetic adsorbents, which combined the adsorption features of activated carbon with the magnetic and the excellent catalytic properties of powdered CuFe2O4, were developed using a simple chemical coprecipitation procedure. The prepared magnetic composites can be used to adsorb acid orange II (AO7) in water and subsequently, easily be separated from the medium by a magnetic technique. CuFe2O4/activated carbon magnetic adsorbents with mass ratio of 1:1, 1:1.5 and 1:2 were prepared. Magnetization measurements, BET surface area measurements, powder XRD and SEM were used to characterize the prepared adsorbents. The results indicate that the magnetic phase present is spinel copper ferrite and the presence of CuFe2O4 did not significantly affect the surface area and pore structure of the activated carbon. The adsorption kinetics and adsorption isotherm of acid orange II (AO7) onto the composites at pH 5.2 also showed that the presence of CuFe2O4 did not affect the adsorption capacity of the activated carbon. The thermal decomposition of AO7 adsorbed on the activated carbon and the composite was investigated by in situ FTIR, respectively. The results suggest that the composite has much higher catalytic activity than that of activated carbon, attributed to the presence of CuFe2O4. The variation of the adsorption capacity of the composites after several adsorption-regeneration cycles has also been studied.     

磷钨酸光催化降解甲基橙溶液的研究

以磷钨酸为光催化剂,在紫外灯照射下,对模拟染料废水甲基橙溶液进行光催化降解,并研究了催化剂加入量、pH值、甲基橙初始浓度和外加氧化剂H2O2对光催化降解效果的影响.结果表明,磷钨酸光催化剂加入量为300 mg/100 mL,pH=2.5时,甲基橙溶液的降解率明显高于其他pH值的降解率;在较低浓度下,甲基橙溶液的光催化降解反应符合一级动力学方程;外加氧化剂H2O2可提高光催化反应速率.