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1.
In order to develop a catalyst with high activity for catalytic wet oxidation (CWO) process at room temperature and atmospheric pressure, Fe2O3-CeO2-TiO2/γ-Al2O3 catalyst was prepared by consecutive impregnation method and the prepared parameters were optimized. The structure of the catalyst was characterized by BET, XRF, SEM and XPS technologies, and the actual wastewater was used to investigate the catalytic activity of Fe2O3-CeO2-TiO2/γ-Al2O3 in CWO process. The experimental results showed that the prepared catalyst exhibited good catalytic activity when the doping amount of Ti was 1.0 wt% (the weight ratio of Ti to carriers), and the middle product, Fe2O3-CeO2-TiO2/γ-Al2O3, was calcined in 450℃ for 2 h. The CWO experiment for treating actual dye wastewater indicated that the COD, color and TOC of actual wastewater were decreased by 62.23%, 50.12% and 41.26% in 3 h, respectively, and the ratio of BOD5/COD was increased from 0.19 to 0.30.  相似文献   

2.
The massive amount of sludge generated by the classic Fenton process, which has often been hypothesized to consist of ferric hydroxide, remains a major obstacle to its large-scale application. Therefore, reutilization of Fenton sludge has recently gained more attention.Understanding the formation, transformation, and properties of Fenton sludge combined with the stages of the Fenton reaction is pivotal, but not well illustrated yet. In this study,SEM-EDS, FT-IR, XRD, and XPS were applied to study the morphology, crystallinity,elemental composition, and valence state of Fenton sludge. The authors report that schwertmannite and 2-line ferrihydrite were generated and transformed in the oxidation phase and the neutralization phase of the Fenton process. SO_4~(2-) in the solution decreased by8.7%–26.0% at different molar ratios of Fe(II) to H_2 O_2; meanwhile, iron ion precipitated completely at pH 3.70 with the formation of schwertmannite containing sulfate groups in the Fenton sludge. The structural sulfate(Fe-SO_4) in schwertmannite was released from the precipitate with the addition of OH-, and the production of Fenton sludge decreased with increasing pH when pH 3.70. Goethite was found to form when the final p H was adjusted to 12 or at a reaction temperature of 80°C. Moreover, the possible thermal transformation to goethite and hematite indicated that Fenton sludge can be reused as a raw material for synthesizing more stable iron(hydro)oxides. The results provide useful insights into the formation and transformation of Fenton sludge, with implications for regulating the crystal type of Fenton sludge for further reuse.  相似文献   

3.
The potentially hazardous iron-containing sludge from the Fenton process requires proper treatment and disposal, which often results in high treatment cost. In this study, a novel method for the reuse of Fenton sludge as an iron source for the synthesis of nickel ferrite particles(NiFe_2O_4) is proposed. Through a co-precipitation method followed by sintering at 800°C, magnetic NiFe_2O_4 particles were successfully synthesized, which was confirmed by powder X-ray diffraction(XRD), scanning electronic microscopy(SEM), energy dispersive spectroscopy(EDS), Fourier transform infrared spectroscopy(FT-IR) and Raman spectroscopy. The synthesized NiFe_2O_4 could be used as an efficient catalyst in the heterogeneous Fenton process. In phenol degradation with H_2O_2 or NiFe_2O_4 alone, the phenol removal efficiencies within the reaction time of 330 min were as low as 5.9% ± 0.1% and 13.5% ±0.4%, respectively. However, in the presence of both NiFe_2O_4 and H_2O_2, phenol removal efficiency as high as 95% ± 3.4% could be achieved, indicating the excellent catalytic performance of NiFe_2O_4 in the heterogeneous Fenton process. Notably, a rapid electron exchange between_Ni II and_Fe III ions in the NiFe_2O_4 structure could be beneficial for the Fenton reaction. In addition, the magnetic catalyst was relatively stable, highly active and recoverable, and has potential applications in the Fenton process for organic pollutant removal.  相似文献   

4.
The catalyst of CuO_x/Al_2O_3 was prepared by the dipping-sedimentation method usingγ-Al_2O_3 as a supporter.CuO and Cu_2O were loaded on the surface of Al_2O_3,characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS).In the presence of CuO_x/Al_2O_3,the microwave-induced chlorine dioxide(ClO_2) catalytic oxidation process was conducted for the treatment of synthetic wastewater containing 100 mg/L phenol.The factors influencing phenol removal were investigated and the results showed that microwave-induced ClO_2-CuO_x/Al_2O_3 process could effectively degrade contaminants in a short reaction time with a low oxidant dosage,extensive pH range.Under a given condition(ClO_2 concentration 80 mg/L,microwave power 50 W,contact time 5 min,catalyst dosage 50 g/L,pH 9),phenol removal percentage approached 92.24%,corresponding to 79.13% of COD_(Cr) removal.The removal of phenol by microwave-induced ClO_2-CuO_x/Al_2O_3 catalytic oxidation process was a complicated non-homogeneous solid/water reaction, which fitted pseudo-first-order by kinetics.Compared with traditional ClO_2 oxidation,ClO_2 catalytic oxidation and microwave-induced ClO_2 oxidation,microwave-induced ClO_2 catalytic oxidation system could significantly enhance the degradation efficiency.It provides an effective technology for the removal of phenol wastewater.  相似文献   

5.
A novel joint method of bioleaching with Fenton oxidation was applied to condition sewage sludge. The specific resistance to filtration(SRF) and moisture of sludge cake(MSC) were adopted to evaluate the improvement of sludge dewaterability. After 2-day bioleaching, the sludge p H dropped to about 2.5 which satisfied the acidic condition for Fenton oxidation.Meanwhile, the SRF declined from 6.45 × 1010 to 2.07 × 1010s2/g, and MSC decreased from91.42% to 87.66%. The bioleached sludge was further conditioned with Fenton oxidation. From an economical point of view, the optimal dosages of H2O2 and Fe2+were 0.12 and 0.036 mol/L,respectively, and the optimal reaction time was 60 min. Under optimal conditions, SRF,volatile solids reduction, and MSC were 3.43 × 108s2/g, 36.93%, and 79.58%, respectively. The stability and settleability of sewage sludge were both improved significantly. Besides,the results indicated that bioleaching-Fenton oxidation was more efficient in dewatering the sewage sludge than traditional Fenton oxidation. The sludge conditioning mechanisms by bioleaching-Fenton oxidation might mainly include the flocculation effects and the releases of extracellular polymeric substances–bound water and intercellular water.  相似文献   

6.
The catalyst of CuOx/Al2O3 was prepared by the dipping-sedimentation method using γ-Al2O3 as a carrier. CuO and Cu2O were loaded on the surface of γ-Al2O3, characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). In the presence of CuOx/Al2O3, the microwave-induced chlorine dioxide (ClO2) catalytic oxidation process was conducted for the treatment of synthetic wastewater containing 100 mg/L phenol. The relationships between removal percentage and initial ClO2 concentration, catalyst dosage, microwave power, contact time, initial phenol concentration and pH were investigated and the results showed that microwave-induced ClO2-CuOx/Al2O3 process could effectively degrade contaminants in a short reaction time with a low oxidant dosage, extensive pH range. Under a given condition (ClO2 concentration 80 mg/L, microwave power 50 W, contact time 5 min, catalyst dosage 50 g/L, pH 9), phenol removal percentage approached 92.24%, corresponding to 79.13% of CODCr removal. The removal of phenol by microwave-induced ClO2-CuOx/Al2O3 catalytic oxidation process was a complicated non-homogeneous solid/water reaction, which fitted pseudo-first-order by kinetics. Compared with traditional ClO2 oxidation, ClO2 catalytic oxidation and microwave-induced ClO2 oxidation, microwave-induced ClO2 catalytic oxidation system could significantly enhance the degradation efficiency. It provides an effective technology for the removal of phenol wastewater.  相似文献   

7.
The advanced treatment using integrated Fenton's reaction and coagulation process was investigated in this study. Before the advancement, the pharmaceutical wastewater containing lincomycin hydrochloride was pretreated by UASB (upflow anaerobic sludge bed) and a SBR (sequencing batch reactor) process. The residual recalcitrant compounds, measured by gas chromatographymass spectrometry (GC-MS), mainly consisted of alcohols, phenols, and nitrogenous and sulfur compounds. The experimental results indicated that when the Fenton's reaction was conducted at pH=3.0, H2O2CODOcr=0.27, H2O2/Fe^2+=3:1 and 30 min of reaction time, and the coagulation process operated at a sulfate aluminum concentration of 800 mg/L and pH value of 5.0, the color and COD in the wastewater decreased by 94% and 73%, respectively; with a finale COD concentration of 267 mg/L and color level of 40 units, meeting the secondary standard of GB8978-1996 for industrial wastewater.  相似文献   

8.
The microwave radiation oxidation process, Fenton as catalytic agent, was used to remove the thiocyanate from the industrial wastewater. The effects of microwave power, radiation time, pH and the feeding in ways of catalyst on the degradation rate of synthetic wastewater were investigated using the microwave radiation oxidation process by orthogonal experiment. The results show Fenton catalyst ratio was 1:20, the microwave radiation power was 900 W, the microwave radiation time was 7 min and the value of pH was 3. Under the optimum conditions, the removal of KSCN can reach over 90%. The apparent kinetics of removal was studied, which conformed to kinetics first-class reaction. In short, for the thiocyanate from the industrial wastewater, microwave-Fenton oxidation method is feasible and effective.  相似文献   

9.
Ordered mesoporous carbon supported iron catalysts(Fe/OMC) were prepared by the incipient wetness impregnation method and investigated in Fenton-like degradation of 4-chlorophenol(4CP) in this work. XRD and TEM characterization showed that the iron oxides were well dispersed on the OMC support and grew bigger with the increasing calcination temperature. The catalyst prepared with a lower calcination temperature showed higher decomposition efficiency towards 4CP and H2O2, but more metals were leached. The effect of different operational parameters such as initial pH, H2O2 dosage, and reaction temperature on the catalytic activity was evaluated. The results showed that 96.1% of 4CP and 47.4% of TOC was removed after 270 min at 30°C, initial pH of 3 and 6.6 mmol/L H2O2. 88% of 4CP removal efficiency was retained after three successive runs, indicating Fe/OMC a stable catalyst for Fenton reaction. 4CP was degraded predominately by the attack of hydroxyl radical formed on the catalyst surface and in the bulk solution due to iron leaching. Based on the degradation intermediates detected by high performance liquid chromatography, possible oxidation pathways were proposed during the 4CP degradation.  相似文献   

10.
Fe(II)/γ-Al2O3 powders synthesized using the dipping method were produced from a mixed aqueous solution containing aluminium oxide(γ-Al2O3) and iron(II)-precursor(FeSO4), and used for photoFenton degradation of phthalocyanine dyes(PCS) under ultraviolet(UV) irradiation in an up-flow fluidized bed. The catalysts were characterized by XRD, ESCA, BET, EDS and SEM. The results showed that Fe2+ion was compounded on the γ-Al2O3 carrier. The effects of different reaction parameters such as catalyst activity, dosage and solution pH on the decolorization of PCS were assessed. Results indicated that maximum decolorization(more than 95%) of PCS occurred with20 wt% Fe(II)/γ-Al2O3 catalyst(dosage of 60 g/L) using a combination of UV irradiation and heterogeneous Fenton system. The degradation efficiency of PCSincreases as pH decreases, exhibiting a maximum efficiency at pH 3.5. The recycled catalyst was capable of repeating three runs without a significant decrease in treatment efficiency, and this demonstrated the stability and reusability of catalyst.  相似文献   

11.
A key step in sludge treatment is sludge dewatering. However, activated sludge is generally very difficult to be dewatered. Sludge dewatering performance is largely affected by the sludge moisture distribution. Sludge disintegration can destroy the sludge structure and cell wall, so as change the sludge floc structure and moisture distribution, thus affecting the dewatering performance of sludge. In this article, the disintegration methods were ultrasound treatment, K2FeO4 oxidation and KMnO4 oxidation. The degree of disintegration (DDCOD), sludge moisture distribution and the final water content of sludge cake after centrifuging were measured. Results showed that three disintegration methods were all effective, and K2FeO4 oxidation was more efficient than KMnO4 oxidation. The content of free water increased obviously with K2FeO4 and KMnO4 oxidations, while it decreased with ultrasound treatment. The changes of free water and interstitial water were in the opposite trend. The content of bounding water decreased with K2FeO4 oxidation, and increased slightly with KMnO4 oxidation, while it increased obviously with ultrasound treatment. The water content of sludge cake after centrifuging decreased with K2FeO4 oxidation, and did not changed with KMnO4 oxidation, but increased obviously with ultrasound treatment. In summary, ultrasound treatment deteriorated the sludge dewaterability, while K2FeO4 and KMnO4 oxidation improved the sludge dewaterability.  相似文献   

12.
A key step in sludge treatment is sludge dewatering. However, activated sludge is generally very difficult to be dewatered. Sludge dewatering performance is largely affected by the sludge moisture distribution. Sludge disintegration can destroy the sludge structure and cell wall, so as change the sludge floc structure and moisture distribution, thus affecting the dewatering performance of sludge. In this article, the disintegration methods were ultrasound treatment, K2FeO4 oxidation and KMnO4 oxidation. The degree of disintegration (DDCOD), sludge moisture distribution and the final water content of sludge cake after centrifuging were measured. Results showed that three disintegration methods were all effective, and K2FeO4 oxidation was more efficient than KMnO4 oxidation. The content of free water increased obviously with K2FeO4 and KMnO4 oxidations, while it decreased with ultrasound treatment. The changes of free water and interstitial water were in the opposite trend. The content of bounding water decreased with K2FeO4 oxidation, and increased slightly with KMnO4 oxidation, while it increased obviously with ultrasound treatment. The water content of sludge cake after centrifuging decreased with K2FeO4 oxidation, and did not changed with KMnO4 oxidation, but increased obviously with ultrasound treatment. In summary, ultrasound treatment deteriorated the sludge dewaterability, while K2FeO4 and KMnO4 oxidation improved the sludge dewaterability.  相似文献   

13.
Fenton氧化/混凝协同处理焦化废水生物出水的研究   总被引:32,自引:5,他引:27  
左晨燕  何苗  张彭义  黄霞  赵文涛 《环境科学》2006,27(11):2201-2205
对Fenton氧化/混凝协同处理焦化废水生物出水的方法进行了研究,在综合考虑经济性和去除效果的前提下,提出了反应的最佳条件:H2O2投加量为220 mg/L,Fe2+投加量为180 mg/L,聚丙烯酰胺投加量为4.5 mg/L,反应时间为0.5h,pH=7.最终COD去除率可达44.5%,色度可以降为35倍,出水符合国家污水排放二级标准.同时,通过分析分子量分布和小分子有机物组成,揭示了Fenton氧化/混凝协同处理焦化废水生物出水的污染物变化规律.结果表明焦化废水经过Fenton氧化/混凝协同处理后,其出水可达到国家二级排放标准,并且处理成本相对较低,具有实际应用的前景.  相似文献   

14.
The effect of phosphate on adsorption and oxidation of catechol, 1,2-dihydroxybenzene, in a heterogeneous Fenton system was investigated. In situ attenuated total reflectance infrared spectroscopy (ATR-FTIR) was used to monitor the surface speciation at the nano-Fe3O4 catalyst surface. The presence of phosphate decreased the removal rate of catechol and the abatement of dissolved organic compounds, as well as the decomposition of H2O2. This effect of phosphate was mainly due to its strong reaction with surface sites on the iron oxide catalyst. At neutral and acid pH, phosphate could displace the adsorbed catechol from the surface of catalyst and also could compete for surface sites with H2O2. In situ IR spectra indicated the formation of iron phosphate precipitation at the catalyst surface. The iron phosphate surface species may affect the amount of iron atoms taking part in the catalytic decomposition of H2O2 and formation of hydroxyl radicals, and inhibit the catalytic ability of Fe3O4 catalyst. Therefore, phosphate ions worked as stabilizer and inhibitor in a heterogeneous Fenton reaction at the same time, in effect leading to an increase in oxidation efficiency in this study. However, before use of phosphate as pH buffer or H2O2 stabilizer in a heterogeneous Fenton system, the possible inhibitory effect of phosphate on the actual removal of organic pollutants should be fully considered.  相似文献   

15.
Characteristics of toluene decomposition and formation of nitrogen oxide (NOx) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al2O3/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO2 selectivity. In addition, NOx was suppressed with the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NOx suppression. The MnOx catalyst exhibited the lowest concentration of O3 and highest CO2 selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.  相似文献   

16.
以城市污水厂二沉池污泥为原料,考察了不同H_2O_2投加量下污泥预氧化对铁负载污泥形成前驱体及其热解后制得炭基催化剂性能的影响,研究了污泥预氧化对强化铁负载制备均一分散型污泥炭基催化剂的机理.结果表明,污泥预氧化促进了污泥细胞破解,降低了絮体颗粒粒径和表面Zeta电位,使铁负载量增加、铁活性位点在污泥载体上的分散性明显增强,形成炭基催化剂保持着高催化活性,其稳定性显著增加.对模拟含铬黑T染料废水的多相芬顿降解试验说明,当污泥预氧化H_2O_2投加量为2.25%时制备的炭基催化剂,其反应120 min后铬黑T的降解率为91%,略低于未预氧化时污泥炭基催化剂的降解效率(96%);但未预氧化炭基催化剂其反应后溶液中铁离子的溶出量(18.9%)远高于预氧化后形成的催化剂(2.5%),且后者循环3次对铬黑T的降解率仍可达到86%,表现出较强的稳定性.  相似文献   

17.
为了有效提高污泥水解效率、缩短厌氧消化时间,以K2FeO4为氧化剂破解剩余污泥,考察K2FeO4投加量(50~500 g/kg,以干质量计)对污泥破解率的影响,分析水解液各项特征指标并对其可生化性能进行预测,探究该方法作为污泥厌氧预处理的可行性.结果表明:污泥水解效率随着K2FeO4投加量的增加而升高,当搅拌速率为500 r/min、反应时间为2 h、K2FeO4投加量为500 g/kg的条件下,可实现最高的污泥破解率(34.6%).污泥水解液中有机物以多糖、蛋白质为主,并有少量挥发性有机酸;污泥破解过程也伴随着P和NH4+-N的释放,上清液中ρ(TP)最高可达496 mg/L,且以正磷酸盐为主(约310 mg/L),可对其进行回收.采用三维荧光体积积分的方法对污泥水解液的可生化性能进行预测,发现污泥经K2FeO4预处理后,水解液中RB(易降解有机质)和PB(难降解有机质)荧光强度均明显增加,当K2FeO4投加量为50 g/kg时,Fdigestion(生物可降解性指数)达到最大值(4.75),预测此时污泥的可生化性能最佳.以K2FeO4为氧化剂预处理污泥可有效提升污泥水解效率,但若作为厌氧消化预处理,应综合考虑污泥破解率和可生化性能.研究显示,搅拌速率为500 r/min、反应时间为2 h、K2FeO4投加量为50 g/kg预处理条件下污泥的可生化性能最佳.   相似文献   

18.
A series of Sr-doped BiFeO3 perovskites (Bi1-xSrxFeO3, BSFO) fabricated via sol-gel method was applied as peroxydisulfate (PDS) activator for ciprofloxacin (CIP) degradation. Various technologies were used to characterize the morphology and physicochemical features of prepared BSFO samples and the results indicated that Sr was successfully inserted into the perovskites lattice. The catalytic performance of BiFeO3 was significantly boosted by strontium doping. Specifically, Bi0.9Sr0.1FeO3 (0.1BSFO) exhibited the highest catalytic performance for PDS activation to remove CIP, where 95% of CIP (10 mg/L) could be degraded with the addition of 1 g/L 0.1BSFO and 1 mmol/L PDS within 60 min. Moreover, 0.1BSFO displayed high reusability and stability with lower metal leaching. Weak acidic condition was preferred to neutral and alkaline conditions in 0.1BSFO/PDS system. The boosted catalytic performance can be interpreted as the lower oxidation state of Fe and the existence of affluent oxygen vacancies generated by Sr doping, that induced the formation of singlet oxygen (1O2) which was confirmed as the dominant reactive species by radical scavenging studies and electron spin resonance (ESR) tests. The catalytic oxidation mechanism related to major 1O2 and minor free radicals was proposed. Current study opens a new avenue to develop effective A-site modified perovskite and expands their application for PDS activation in wastewater remediation.  相似文献   

19.
本研究首先分析了铁负载污泥炭的物理化学性质,评估了铁负载污泥炭与有机高分子(聚丙烯酰胺,PAM)联合调理改善高级厌氧消化污泥脱水性的效能,研究了联合调理过程中污泥絮体特性与胞外聚合物(EPS)的变化特征.结果表明,单独投加污泥炭可以通过铁的电中和作用降低污泥颗粒间的静电排斥力,同时充当骨架材料改善污泥的脱水性能.此外,铁负载污泥炭可以有效去除污泥体系中大分子溶解性有机物,从而改善污泥的过滤性能.污泥炭和有机絮凝剂在污泥调理过程中表现出明显的协同作用,污泥碳和PAM的最佳投加量分别为250 mg·g-1(以TSS计)和8 mg·g-1(以TSS计).激光共聚焦显微镜分析表明,PAM主要与污泥絮体中的蛋白质分子作用,从而促使污泥颗粒凝聚.  相似文献   

20.
芬顿/絮凝组合工艺在处理难降解有机物废水时会产生大量的芬顿污泥,会提高废水处理成本,同时也会对环境构成威胁,迫切需要开发一种绿色可持续的方法实现芬顿污泥资源化利用.该研究通过将处理PNP(对硝基苯酚)废水产生的芬顿污泥和污水厂生化污泥共热解,原位制备具有高催化活性的MBC(磁性生物炭),并作为多相芬顿催化剂用于去除PNP,实现“以废治废”.结果表明:当芬顿污泥和生化污泥质量比为1∶1、热解温度为800℃时,制备得到的MBC-800-3催化性能最佳;合适的混合比例可有效避免颗粒聚集,高温形成缺陷结构和多种铁相,为MBC-800-3提供了丰富的反应活性位点;当废水初始pH为3、H2O2浓度为60 mmol/L、MBC-800-3投加量为0.4 g/L时,PNP和TOC(总有机碳)的去除率均最高,在催化反应100 min时分别达到98%和62%;酸性条件下,MBC活化H2O2产生·OH和·O2-催化降解废水的有机物,其中,·OH作为主要活性物种,其来源包括均相芬顿反应和非均芬顿相反应...  相似文献   

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