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1.
非均相钴活化过氧乙酸(PAA)是一种有前景的杂环类药物去除技术,然而目前报道的钴基催化剂通常为粉末状,难以回收,因此,构建可循环利用的非均相钴基催化剂及其活化PAA体系具有重要意义.通过浸渍煅烧法制备负载型钴基催化剂(载钴陶粒),系统研究了不同影响因素下载钴陶粒活化PAA体系降解水中典型杂环类药物(磺胺甲恶唑(SMX)、磺胺嘧啶(SDZ)、卡马西平(CBZ)和甲氧苄啶(TMP))的性能.结果表明,其最优反应条件为:载钴陶粒投加体积比(载钴陶粒/反应溶液)为1∶20 (V/V),PAA浓度为150 mg·L-1.当杂环类药物初始浓度为20mg·L-1时,反应30 min后SMX、SDZ、CBZ、TMP的降解率分别为96.42%、99.63%、96.74%和89.93%.溶液中的共存离子对杂环类药物的降解存在抑制作用,其影响为:HCO3->NO3-≈SO42-≈Cl-.反应结束后钴溶出浓度均低于1 mg·L-1,符合我国地表水环境质量标准规定,但溶液发光细菌急性毒性均升高.经5次循环使用后,载钴陶粒/PAA体系对除TM...  相似文献   

2.
采用溶胶-凝胶法以十六烷基三甲基溴化铵(CTAB)为模板剂,正硅酸乙酯(TEOS)为硅源,制备以纳米零价铁(nZVI)为核,SiO2为壳层的nZVI@SiO2核壳复合材料,通过SEM、TEM、XRD和BET对材料进行表征,并对nZVI@SiO2活化过硫酸盐(PDS)去除氯苯(MCB)性能进行研究.结果表明,nZVI@SiO2-1材料为均匀的核壳结构;比表面积达到了212.67 m2·g-1,壳层厚度为7 nm左右,Fe含量达到了38.92%.在MCB初始浓度为20 mg·L-1、温度(20±2)℃、nZVI@SiO2-1投加量为0.5 g·L-1、PDS投加量为3 mmol·L-1条件下MCB去除率为83.81%.低浓度HA和Cl-对nZVI@SiO2-1/PDS体系去除MCB呈促进作用.而HCO3  相似文献   

3.
张晓  胡春  张丽丽  石宝友 《环境科学学报》2020,40(11):3895-3904
采用醇助水热法制备了新型生物质炭修饰的α-FeOOH类芬顿催化剂(BC-FeOOH),并通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)对催化剂进行了表征,证明生物质炭(BC)成功引入到α-FeOOH中.以罗丹明B(RhB)为目标污染物,考察了BC修饰量、催化剂及H2O2投加量对其催化效率的影响.结果表明,BC的引入可以极大地提高FeOOH的类芬顿催化性能.在pH中性、催化剂投加量0.6 g·L-1、H2O2初始浓度10 mmol·L-1的条件下,BC-FeOOH(22.2%BC)对RhB的降解率可达到90%,重复利用5次活性仍可保持在80%左右,且铁离子溶出浓度仅为0.08 mg·L-1.进一步通过ESR在不同体系中的测试结果表明,BC的引入不仅可促进H2O2有效还原分解产生更多的羟基自由基(·OH),而且增强了催化剂与污染物Rh...  相似文献   

4.
王渊源  阎鑫  艾涛  李卓  牛艳辉 《环境科学》2022,43(4):2039-2046
Co3O4具有优良的活化过硫酸盐的性能而受到人们的重视,但Co3O4粉体易团聚、使用过程中难以分离、易流失和重复利用率差等问题严重制约了其实际应用.通过水热法制备碳化三聚氰胺泡沫负载Co3O4非均相催化剂.采用X-射线衍射仪(XRD)和扫描电子显微镜(SEM)对催化剂的结构和表面形貌进行分析.研究不同因素对催化剂活化过硫酸氢钾(PMS)降解罗丹明B(RhB)的性能.其最优催化工艺参数:催化剂投加量为35 mg·L-1、PMS质量浓度为50 mg·L-1和pH为7、RhB初始质量浓度为10 mg·L-1,30 min反应后对RhB降解率为98%.结果表明,增大碳化泡沫负载Co3O4非均相催化剂投加量和PMS质量浓度能明显提高对RhB的降解率;而增加RhB初始质量浓度和提高pH值会明显抑制RhB的降解率.催化反应过程符合准一级动力学方程.温度对RhB降...  相似文献   

5.
采用溶剂热反应制备了分级微球结构的铁掺杂氯氧化铋(Fe-BiOCl),并用于光芬顿降解阿特拉津(Atrazine,ATZ).结合多因素实验,系统地分析了以Fe-BiOCl为催化剂构建的光芬顿体系氧化降解阿特拉津的性能与机理.结果表明,当催化剂用量为0.2 g·L-1、污染物浓度为20 mg·L-1、H2O2浓度为6.4 mmol·L-1时,Fe-BiOCl-2催化剂在120 min内降解阿特拉津的效率约为99.98%,且在较宽pH范围(3.04~6.02)内保持优异的降解效率.通过自由基猝灭实验和电子顺磁共振(EPR)测试发现,在光芬顿体系中羟基自由基(·OH)和超氧自由基(·O2-)是反应的主要活性物种.此外,通过超高效液相色谱测定降解过程中的中间产物,提出了可能的降解路径和转化机理.  相似文献   

6.
张李  付永胜  刘义青 《中国环境科学》2021,40(12):5260-5269
研究了Cu2+强化UV活化过氧乙酸(Cu2+/UV/PAA)对水中双氯芬酸(DCF)的降解,考察了pH值、PAA投加量、Cu2+投加量、无机阴离子(Cl-、SO42-、NO3-和CO32-)和溶解有机物(DOM)对DCF去除的影响;探讨了DCF在该体系中的降解产物和转化机理.结果表明:UV和Cu2+都能活化PAA产生活性自由基促进DCF降解.DCF在Cu2+/UV/PAA中的降解遵循准一级动力学,其降解可能归因于直接光解、HO·氧化和CH3COO·、CH3COOO·等其它自由基氧化.在pH=3~11范围内,DCF降解的最佳pH=8.5.DCF的降解效率随着PAA投加量的增大而逐渐增高,过量的PAA能与DCF竞争HO·.Cu2+用量的提高也能促进DCF的去除,但是过量的Cu2+可生成Cu(OH)2导致其催化能力下降.由于NO3-在UV照射下可以产生HO·,其对DCF降解有促进作用,且NO3-浓度越高,促进作用越明显.不同浓度的Cl-、SO42-、CO32-和DOM对DCF降解影响较小.在Cu2+/UV/PAA降解DCF的过程中,共检测出13种降解产物.根据这些降解产物,提出了DCF可能的转化机理,包括8种不同的反应路径.  相似文献   

7.
针对印染工业园生化尾水中生物难降解的有机氮难题,采用O3-SBBR(臭氧-序批式生物膜反应器)联合工艺进行深度处理.开展了影响因素实验、降解动力学和淬灭实验,测定了自由基种类、琥珀酸脱氢酶活性和脱氮功能基因.结果表明,适宜的臭氧氧化条件:pH为8.0~8.5、ρ(O3)为35.0 mg·L-1左右、 O3投加量(以O3/H2O计,下同)约为100.0 mg·L-1和反应时间为90.0~120.0 min.臭氧氧化生化尾水的有机氮符合拟一级动力学模型,最大速率常数k值为0.010 35 min-1[实验条件:pH为8.0、 O3投加量为150.0 mg·L-1和ρ(O3)为35.0 mg·L-1].臭氧氧化显著提高序批式生物膜反应器(SBBR)的脱氮性能,脱氮效率从19.8%(SBBR)提高到32.9%(O3  相似文献   

8.
高晶度Mn-Fe LDH催化剂活化过一硫酸盐降解偶氮染料RBK5   总被引:4,自引:2,他引:2  
李立  吴丽颖  董正玉  王霁  张倩  洪俊明 《环境科学》2020,41(6):2736-2745
采用改进的共沉淀结合水热法制备高晶度锰铁层状双金属氢氧化物作为催化剂,用于高效活化过一硫酸盐(PMS)降解活性黑5(RBK5).通过X射线粉末衍射仪(XRD)、扫描电子显微镜(SEM)、X射线能谱分析(EDS)、傅里叶变换红外光谱仪(FTIR)以及X射线光电子能谱(XPS)对材料进行表征,证明成功合成了结晶度高、层状结构突出的Mn-Fe LDH.同时探究了锰铁量比,催化剂投加量,PMS浓度和初始pH值等因素对RBK5的吸附效果、催化降解及反应动力学的影响.结果表明,高晶度Mn-Fe LDH催化剂具有良好的吸附能力和高效的催化效率,在n(Mn)/n(Fe)比为1∶1,催化剂投加量为0.2 g·L-1,PMS浓度为1 mmol·L-1,初始pH为7时,RBK5(20 mg·L-1)在90 min内降解率可达86%,整个反应过程符合拟一级动力学(R2>0.9).自由基猝灭实验表明,Mn-Fe LDH/PMS体系降解RBK5为SO-4·和·OH两种活性自由基...  相似文献   

9.
张李  付永胜  刘义青 《中国环境科学》2020,40(12):5260-5269
研究了Cu2+强化UV活化过氧乙酸(Cu2+/UV/PAA)对水中双氯芬酸(DCF)的降解,考察了pH值、PAA投加量、Cu2+投加量、无机阴离子(Cl-、SO42-、NO3-和CO32-)和溶解有机物(DOM)对DCF去除的影响;探讨了DCF在该体系中的降解产物和转化机理.结果表明:UV和Cu2+都能活化PAA产生活性自由基促进DCF降解.DCF在Cu2+/UV/PAA中的降解遵循准一级动力学,其降解可能归因于直接光解、HO·氧化和CH3COO·、CH3COOO·等其它自由基氧化.在pH=3~11范围内,DCF降解的最佳pH=8.5.DCF的降解效率随着PAA投加量的增大而逐渐增高,过量的PAA能与DCF竞争HO·.Cu2+用量的提高也能促进DCF的去除,但是过量的Cu2+可生成Cu(OH)2导致其催化能力下降.由于NO3-在UV照射下可以产生HO·,其对DCF降解有促进作用,且NO3-浓度越高,促进作用越明显.不同浓度的Cl-、SO42-、CO32-和DOM对DCF降解影响较小.在Cu2+/UV/PAA降解DCF的过程中,共检测出13种降解产物.根据这些降解产物,提出了DCF可能的转化机理,包括8种不同的反应路径.  相似文献   

10.
填埋场已成为氯乙烯污染的重要来源,明晰覆盖层土壤中氯乙烯的降解特性及功能微生物群落组成对氯乙烯污染控制具有重要意义.基于填埋场覆盖土系统开展了典型氯乙烯的好氧/厌氧共代谢降解研究.结果显示,好氧和厌氧条件下CH4均可发生降解,二氯乙烯(DCE)只能在好氧条件下被降解,净降解速率为50μg·h-1·L-1;三氯乙烯(TCE)可同时发生好氧共代谢和厌氧共代谢转化,净降解速率分别为38和5μg·h-1·L-1;四氯乙烯(PCE)只能发生厌氧共代谢,降解速率为0.77μg·h-1·L-1,发现好氧共代谢速率远高于厌氧共代谢速率.构建了覆盖层中氯乙烯的分布模型并评估了CH4及氯乙烯好氧/厌氧共代谢贡献度,CH4好氧和厌氧降解贡献度分别为59%~70%和30%~41%,TCE好氧和厌氧共代谢降解贡献度分别为73%和27%.对氯乙烯厌氧/好氧共代谢降解过程的微生物群落组成及潜在功能菌属进行了分析,发现好氧...  相似文献   

11.
Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis (DGGE) and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity (both in gene richness and diversity index values) and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor (50 mg/kg) recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos (150 mg/kg) caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos (250 mg/kg) produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes (bands) responded differently to the impact of agrochemicals: four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.  相似文献   

12.
The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.  相似文献   

13.
Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.  相似文献   

14.
Several main metabolites of benzo[a]pyrene (BaP) formed by Penicillium chrysogenum, Benzo[a]pyrene-1,6-quinone (BP 1,6- quinone), trans-7,8-dihydroxy-7,8-dihydrobenzo[a]pyrene (BP 7,8-diol), 3-hydroxybenzo[a]pyrene (3-OHBP), were identified by high-performance liquid chromatography (HPLC). The three metabolites were liable to be accumulated and were hardly further metabolized because of their toxicity to microorganisms. However, their further degradation was essential for the complete degradation of BaP. To enhance their degradation, two methods, degradation by coupling Penicillium chrysogenum with KMnO4 and degradation only by Penicillium chrysogenum, were compared; Meanwhile, the parameters of degradation in the superior method were optimized. The results showed that (1) the method of coupling Penicillium chrysogenum with KMnO4 was better and was the first method to be used in the degradation of BaP and its metabolites; (2) the metabolite, BP 1,6-quinone was the most liable to be accumulated in pure cultures; (3) the effect of degradation was the best when the concentration of KMnO4 in the cultures was 0.01% (w/v), concentration of the three compounds was 5 mg/L and pH was 6.2. Based on the experimental results, a novel concept with regard to the bioremediation of BaP-contaminated environment was discussed, considering the influence on environmental toxicity of the accumulated metabolites.  相似文献   

15.
In this study an effort has been made to use plant polyphenol oxidases; potato (Solanum tuberosum) and brinjal (Solanum melongena), for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.  相似文献   

16.
RemovalofheavymetalsfromsewagesludgebylowcostingchemicalmethodandrecyclinginagricultureWuQitang,NyirandegePascasie,MoCehuiF...  相似文献   

17.
A study was conducted to compare the diversity of 2-, 3-, and 4-chlorobenzoate degraders in two pristine soils and one contaminated sewage sludge. These samples contained strikingly different populations of mono-chlorobenzoate degraders. Although fewer cultures were isolated in the uncontaminated soils than contaminated one, the ability of microbial populations to mineralize chlorobenzoate was widespread. The 3- and 4-chlorobenzoate degraders were more diverse than the 2-chlorobenzoate degraders. One of the strains isolated from the sewage sludge was obtained. Based on its phenotype, chemotaxonomic properties and 16S rRNA gene, the organism S-7 was classified as Rhodococcus erythropolis. The strain can grow at temperature from 4 to 37℃. It can utilize several (halo)aromatic compounds. Moreover, strain S-7 can grow and use 3-chlorobenzoate as sole carbon source in a temperatures range of 10-30℃ with stoichiometric release of chloride ions. The psychrotolerant ability was significant for bioremediation in low temperature regions. Catechol and chlorocatechol 1,2-dioxygenase activities were present in cell free extracts of the strain, but no (chloro)catechol 2,3- dioxygenase activities was detected. Spectral conversion assays with extracts from R. erythropolis S-7 showed accumulation of a compound with a similar UV spectrum as chloro-cis,cis-muconate from 3-chlorobenzoate. On the basis of these results, we proposed that S-7 degraded 3-chlorobenzoate through the modified ortho-cleave pathway.  相似文献   

18.
Single and joint effects of pesticides and mercury on soil urease   总被引:3,自引:3,他引:3  
The influence of two pesticides including chlorimuron-ethyl and furadan and mercury (Hg) on urease activity in 4 soils (meadow burozem and phaeozem) was investigated. The soils were exposed to various concentrations of the two pesticides and Hg individually and simultaneously. Results showed that there was a close relationship between urease activity and organic matter content in soil. Chlorimuron-ethyl and furadan could both activate urease in the 4 soils. The maximum increment of urease activity by chlorimuronethyl was up to 14%-18%. There was almost an equal increase (up to 13%-21%) in the urease activity by furadan. On the contrary, Hg markedly inhibited soil urease activity. A logarithmic equation was used to describe the relationship (P〈0.05) between the concentration of Hg and the activity of soil urease in the 4 tested soils. Semi-effect dose (ED50) values by the stress of Hg based on the inhibition of soil urease in the 4 soils were 88, 5.5, 24 and 20 mg/kg, respectively, according to the calculation of the corresponding equations. The interactive effect of chlorimuron-ethyl or furadan with metal Hg on soil urease was mainly synergic at the highest tested concentrations.  相似文献   

19.
A field study was conducted in the Taihu Lake region, China in 2004 to reveal the organochlorine pesticide concentrations in soils after the ban of these substances in the year 1983. Thirteen organochlorine pesticides (OCPs) were analyzed in soils from paddy field, tree land and fallow land. Total organochlorine pesticide residues were higher in agricultural soils than in uncultivated fallow land soils. Among all the pesticides, ΣDDX (DDD, DDE and DDT) had the highest concentration for all the soil samples, ranging from 3.10 ng/g to 166.55 ng/g with a mean value of 57.04 ng/g and followed by ΣHCH, ranging from 0.73 ng/g to 60.97 ng/g with a mean value of 24.06 ng/g. Dieldrin, endrin, HCB and α-endosulfan were also found in soils with less than 15 ng/g. Ratios of p,p'-(DDD DDE)/DDT in soils under three land usages were: paddy field > tree land > fallow land, indicating that land usage inlfuenced the degradation of DDT in soils. Ratios of p,p'-(DDD DDE)/DDT >1, showing aged residues of DDTs in soils of the Taihu Lake region. The results were discussed with data from a former study that showed very low actual concentrations of HCH and DDT in soils in the Taihu Lake region, but according to the chemical half-lives and their concentrations in soils in 1980s, the concentration of DDT in soils seemed to be underestimated. In any case our data show that the ban on the use of HCH and DDT resulted in a tremendous reduction of these pesticide residues in soils, but there are still high amounts of pesticide residues in soils, which need more remediation processes.  相似文献   

20.
Common silver barb,Puntius gonionotus,exposed to the nominal concentration of 0.06 mg/L Cd for 60 d,were assessed for histopathological alterations(gills,liver and kidney),metal accumulation,and metallothionein(MT)mRNA expression.Fish exhibited pathological symptoms such as hypertrophy and hyperplasia of primary and secondary gill lamellae,vacuolization in hepatocytes,and prominent tubular and glomerular damage in the kidney.In addition,kidney accumulated the highest content of cadmium,more than gills and liver.Expression of MT mRNA was increased in both liver and kidney of treated fish.Hepatic MT levels remained high after fish were removed to Cd-free water.In contrast,MT expression in kidney was peaked after 28 d of treatment and drastically dropped when fish were removed to Cd-free water.The high concentrations of Cd in hepatic tissues indicated an accumulation site or permanent damage on this tissue.  相似文献   

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