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1.
紫外活化过硫酸盐降解磷酸氯喹   总被引:1,自引:1,他引:0  
李阳  许玻珲  邓琳  罗伟 《环境科学》2022,43(9):4597-4607
以抗新型冠状肺炎药物——磷酸氯喹(CQP)为研究对象,考察其在紫外活化过硫酸盐体系(UV/PS)中的降解效果.通过竞争动力学实验,确定了CQP与羟基自由基(HO·)和硫酸根自由基(SO4-·)的二级反应速率常数,同时考察了PS浓度、pH和常见无机阴离子对UV/PS体系中CQP降解的影响,并通过建立动力学模型预测CQP浓度和主要自由基浓度以探究其影响机制.结果表明,UV/PS体系对CQP的降解效果显著优于单一UV、单一太阳光或单一PS体系,在10 min内可降解91.3%的CQP;在pH为6.9的条件下,CQP与HO·和SO4-·的二级反应速率常数分别为8.9×109 L·(mol·s)-1和1.4×1010 L·(mol·s)-1,其中SO4-·是主要活性物种;CQP的降解速率随PS浓度增加而增大,HCO3-和Cl-的加入对UV/PS体系中CQP的去除起到抑制作用,碱性较强的条件不利于CQP的转化.经LC-MS分析,发现CQP在UV/PS体系中主要经过N-脱乙基化、C—N键断裂和抽氢等反应被逐步降解为其他有机中间产物.加大PS浓度和pH可提高其矿化率.此研究可为抗新冠肺炎医药废水的处理提供帮助.  相似文献   

2.
李鑫  尹华  罗昊昱  欧阳晓芳  刘航  祝铭韩 《环境科学》2021,42(10):4798-4806
环境中的多溴联苯醚(PBDEs)对人类健康和生态环境存在潜在危害,开发高效、经济和环保的高级氧化体系对其进行有效降解具有重要意义.利用水热法合成的磁性生物炭负载二氧化锰复合材料(α-MnO2/MWB)作为催化剂,有效活化过一硫酸盐(PMS)降解2,2'',4,4''-四溴联苯醚(BDE-47),通过SEM、XRD、FT-IR和BET等手段对材料进行表征分析,同时探究了材料对PMS的催化活化能力.结果表明,α-MnO2/MWB具有最佳的催化性能,在α-MnO2/MWB负载质量比为1:2、催化剂投加量为0.05 g·L-1、PMS浓度为5 mmol·L-1的条件下,对1 mg·L-1 BDE-47的降解率达到94%.溶液初始pH对体系的影响较小,氯离子(Cl-)和腐殖酸(HA)对BDE-47的降解有抑制作用,随其浓度升高抑制作用增强,硝酸根离子(NO3-)和碳酸氢根离子(HCO3-)对降解几乎无影响.通过自由基淬灭实验证明SO4-·和·OH是该体系降解BDE-47的两种关键自由基,其中SO4-·占主导地位.反应前后材料的XPS表征分析表明,Mn和Fe元素的价态转化是活化PMS的主要原因.α-MnO2/MWB经重复利用4次,仍保持着高效的催化性能.  相似文献   

3.
林涛  苑宇杰 《环境科学》2024,45(3):1553-1560
研究了紫外光活化亚硫酸盐高级氧化工艺降解水中典型新污染物——卡马西平(CBZ)的效能和降解机制.探究了不同溶解氧浓度[ρ(DO)]对紫外光活化亚硫酸盐降解CBZ的影响,并在模拟自然水体环境控制初始ρ(DO)为(8.0±0.2) mg·L-1条件下,考察了不同工艺参数(亚硫酸盐投加量、反应pH)与水环境要素(碳酸氢根离子、氯离子、腐殖酸)对CBZ降解效能的影响.结果表明,紫外光活化亚硫酸盐工艺可在30 min内降解85.3%的CBZ,降解过程遵循拟一级动力学,动力学常数为0.055 7 min-1.并采用电子顺磁共振波谱技术、活性物质淬灭实验和竞争反应动力学实验发现,CBZ的降解主要来自紫外光活化亚硫酸盐工艺中硫酸根自由基(SO4-·)与羟基自由基(·OH)等活性物质,且降解贡献率分别为43.9%和56.1%.而且CBZ降解率随HCO3-浓度升高而降低,但Cl-浓度变化对CBZ降解率影响不大,水中存在的腐殖酸可显著抑制CBZ的降解.反应过程中硫酸盐的积累量显著低于《生活饮用水卫生标准》(GB 5749-2022)限值,且亚硫酸盐消耗速率(0.004 4 min-1)显著低于CBZ的降解速率,说明亚硫酸盐可被紫外光高效活化用于降解水中存在的CBZ.  相似文献   

4.
文焱  齐晶瑶  李欣 《环境科学学报》2021,41(10):3969-3975
针对电催化还原工艺处理氯酚类有机废水受到限制等问题,制备了过渡金属O-NiCoP/Ni2P催化电极,并用于目标污染物2,4-二氯苯酚废水的电催化还原降解.同时,主要考察了2,4-二氯苯酚浓度、电流密度、电解质浓度、pH和温度等因素对O-NiCoP/Ni2P催化电极降解效能的影响.结果表明,在2,4-二氯苯酚初始浓度为10 mg·L-1,温度为25℃,溶液pH=7,Na2SO4电解质浓度为50 mmol·L-1,电流密度为10 mA·cm-2的条件下,O-NiCoP/Ni2P电极催化降解180 min,对2,4-二氯苯酚去除率可达到72.2%.同时,催化电极循环使用10次,2,4-二氯苯酚的去除效率保持在72.1%~72.7%,表明电极具有良好的稳定性和实际应用的潜在价值.  相似文献   

5.
Fe2+可激活过二硫酸盐(PDS)快速产生硫酸根自由基(SO4-·),但Fe2+会快速转化为低活性的Fe3+,且Fe2+的投加量普遍较大,限制了该体系的广泛应用.采用亚硫酸氢盐(BS)强化微量Fe2+-PDS体系降解水中的扑热息痛(APAP).结果表明,投加BS可促进Fe2+-Fe3+的循环,明显改善Fe2+-PDS体系对APAP的降解效果,在最优条件下(PDS=0.6 mmol·L-1;BS=0.4 mmol·L-1;Fe2+=10 μmol·L-1;pH=4)下,APAP (4 μmol·L-1)可在180 s内被完全降解.同时,APAP的降解速率随BS (0~0.6 mmol·L-1)和PDS (0.2~1.5 mmol·L-1)浓度的增大而升高,适量提高Fe2+浓度可促进APAP的降解,但增加BS的投加次数对降解速率影响不大.HCO3-与HPO42-明显抑制了体系降解APAP的效率,Cl-和NO3-有轻微抑制作用,腐殖酸(HA)则影响不大.通过淬灭实验和电子顺磁共振波谱检测,证实了体系中SO4-·、·OH和单线态氧的产生,其中SO4-·是降解APAP的主要活性物种.利用三维荧光光谱技术对APAP降解过程进行了表征,表明APAP降解产物具有荧光特性.此外,还鉴定出5种中间产物,并提出了3种可能的降解途径.体系在实际水体中的效能低于超纯水中的表现,但延长反应时间可明显增强降解效果,表明BS-Fe2+-PDS体系是一种有前景的有机污染物降解方法.  相似文献   

6.
采用非自由基活化的过一硫酸盐(PMS)氧化降解水中的喹啉,考察了PMS浓度、初始pH、反应温度及水中共存物质对喹啉降解效率的影响.结果表明,非自由基活化PMS体系可以有效降解喹啉,喹啉的降解过程符合伪一级反应动力学.初始喹啉浓度为10.0 mg·L-1、PMS浓度为4.0 mmol·L-1、pH 为7.0、温度为25 ℃的条件下,反应150 min喹啉降解率达到95.8%. HCO3-、NO3-、SO42-和腐殖酸对喹啉的降解没有影响, 高浓度Cl-可促进喹啉的降解.淬灭实验证实,反应体系中没有SO4-·和·OH的生成,而存在单线态氧(1O2),PMS的直接氧化是喹啉降解的主导作用机制.通过GC-MS检测了喹啉降解的中间产物,并推测了喹啉降解的可能路径.毒性实验表明,反应体系降解喹啉过程中产生了毒性更强的中间产物,而在最佳反应条件下体系可以有效脱毒.  相似文献   

7.
为发展废水中氯代酚的处理技术和保护水环境安全,采用"浸渍-干燥-电沉积"法制备钯-多壁碳纳米管-泡沫镍电极,研究电极对2,4-二氯苯酚(2,4-DCP)的去除能力和动力学特征,并探讨了2,4-DCP的脱氯机理.结果表明,在MWCNTs和Pd负载量分别为0.7 mg·cm-2和0.01 mmol·cm-2时制备的电极对2,4-DCP去除效果最好;掺入多壁碳纳米管(MWCNTs)可增大电极的表面积,提高Pd的分散性,增强电极的催化效率.当Na2SO4浓度为0.05 mol·L-1,工作电压为-1 V,反应液初始pH为7时,50 mg·L-1的2,4-DCP降解90 min的去除率达到99.74%,降解过程符合一级反应动力学模型,速率常数为0.0667 min-1.采用高效液相色谱法监测2,4-DCP的降解产物,发现苯酚为2,4-DCP还原的最终产物,降解途径包括直接脱去2个氯原子转化为苯酚和分步脱去2个氯原子再转化为苯酚,但以直接脱去2个氯原子为主要途径.活性基淬灭实验证明,电极通过产生的吸附态氢原子(Hads)对2,4-DCP进行加氢脱氯.  相似文献   

8.
全氟化合物(PFCs)是一种新兴的持久性有机污染物,具有环境持久性、高毒性和难降解性,因此急需研发高效的降解方法.本文采用电化学恒电位电解法活化过硫酸盐,利用得到的具有强氧化性的SO4·-有效降解全氟辛酸(PFOA),考察了恒定电位值、过硫酸钠的初始浓度、溶液初始pH值和共存离子对电活化过硫酸盐降解PFOA的影响.同时,结合超高效液相色谱-三重串联四级杆质谱联用仪(UPLC-MS/MS)和气相色谱与质谱联用仪(GC-MS),对其降解的液相和气相中间产物进行探究.结果表明,在控制阴极电位为-1.8 V,初始过硫酸钠溶液浓度为200 mmol·L-1,初始溶液pH=3.29,恒电位电解4 h后,PFOA去除率约达到60%.当体系中有NO3-、异丙醇和过硫酸钠共存时,PFOA降解效率明显提高(91%,4 h),当有ClO4-存在时PFOA去除率约达到76.8%,但HCO3-和Cl-的存在会出现抑制效果.通过对降解中间产物(短链PFCAs和加氢产物)和TOC去除率(62.5%,24 h)的监测分析,进而推断其可能的降解机理为SO4·-介导的Kolbe脱羧过程和羧酸逐步被加氢还原的过程.  相似文献   

9.
针对高负荷餐厨垃圾和剩余污泥混合发酵系统在实际应用过程中存在的盐度抑制问题,通过批次试验探究了不同钠盐(CH3COONa、NaCl和Na2SO4)对中温混合发酵体系的影响,考察了添加不同浓度钠盐时混合发酵体系的甲烷累积产量、有机物去除率、挥发性脂肪酸(VFAs)累积量及水解、酸化、乙酸化和产甲烷速率的抑制作用.结果表明,随着CH3COONa浓度的增加,相应的甲烷产量逐渐增加,但在高浓度时理论甲烷产量降低,当Na+浓度为8 g·L-1时,对产甲烷抑制率为21%.此外,NaCl和Na2SO4对甲烷累积产量具有抑制作用,相同Na+浓度下,Na2SO4对混合发酵体系甲烷产量的抑制作用更大;当SO42-浓度为8.3 g·L-1时,相应甲烷抑制率为23%.相反,Cl-浓度为3.1~6.2 g·L-1时,对混合发酵过程中甲烷抑制率为4.6%~7.7%;但随着Cl-浓度增至9.3~12.3 g·L-1时,甲烷产量提升了14.5%~37.6%.分析认为,NaCl对混合发酵过程有机物去除率的抑制作用主要是Na+的影响,而Na2SO4的抑制作用主要来源于SO42-和Na+的协同作用.NaCl和Na2SO4对水解速率和产甲烷速率的抑制作用较大,而对酸化速率和乙酸化速率抑制作用较小.  相似文献   

10.
以乙腈作为含氰废气的典型组分,考察吸收协同不同高级氧化体系下低浓度乙腈的去除效率以及产物分配情况.研究结果表明:UV/PS和VUV/PS体系均能有效吸收并降解乙腈,在60 min内其脱除效率近100%,且矿化率近80%或以上.主要原因是吸收液中的过硫酸盐(PS)可以在紫外光的激发下产生大量的HO·和SO4·-,这些自由基可以促进乙腈和中间产物的氧化.同时实验还观察到乙腈中的氮元素主要被转化为NO3-和NH4+,这说明乙腈的直接氧化和水解反应同时进行.NO3-的累积会竞争消耗反应体系中的自由基,这是其稳定性实验中乙腈矿化率下降的主要原因.此外,干扰离子Cl-也会由于自由基的捕获作用抑制乙腈的降解.最后,根据产物的分析结果,提出了包含氧化与水解路径的乙腈总体降解反应途径.  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.
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   

14.
RemovalofheavymetalsfromsewagesludgebylowcostingchemicalmethodandrecyclinginagricultureWuQitang,NyirandegePascasie,MoCehuiF...  相似文献   

15.
Single and joint effects of pesticides and mercury on soil urease   总被引:6,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   

16.
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   

17.
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   

18.
The contribution of aliphatic-rich plant biopolymer to sorption of hydrophobic organic compounds is significantly important because of their preservation and accumulation in the soil environment,but sorption mechanism is still not fully understood.In this study, sorption of 1-naphthol by plant cuticular fractions was examined to better understand the contributions of respective fraction.Toward this end,cuticular materials were isolated from the fruits of tomato by chemical method.The tomato cuticle sheet consisted of waxes (6.5 wt%),cuticular monomer (69.5 wt%),and polysaccharide (24.0 wt%).Isotherms of l-naphthol to the cuticular fractions were nonlinear (N value (0.82-0.90)) at the whole tested concentration ranges.The KodKow ratios for bulk cuticle (TC1),dewaxed cuticle (TC2),cutin (TC4),and desugared cuticle (TC5) were larger than unity,suggested that tomato bulk cuticle and cutin are much powerful solption medium.Sorption capability of cutin (TC4) was 2.4 times higher than the nonsaponifiable fraction (TC3).The 1-naphthol interactions with tomato cuticular materials were governed by both hydrophobic-type interactions and polar (H-bonding) interactions. Removal of the wax and polysaccharide materials from the bulk tomato cuticle caused a significant increase in the sorption ability of the cuticular material.There was a linear negative trend between K_(oc) values and the amount of polysaccharides or fraction's polarities ((N O)/C);while a linear positive relationship between K_(oc) values and the content of cutin monomer (linear R~2=0.993) was observed for present in the cuticular fractions.Predominant sorbent of the hydrophobic organic compounds (HOCs) in the plant cuticular fraction was the cutin monomer,contributing to 91.7% of the total sorption of tomato bulk cuticle.  相似文献   

19.
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   

20.
Seed induces and promotes the crystallization of calcium phosphate, and acts as carrier of the recovered phosphorus (P). In order to select suitable seed for P recovery from wastewater, three seeds including Apatite (AP), Juraperle (JP) and phosphate-modified Juraperle (M-JP) were tested and compared. Batch and fixed-bed column experiments of seeded crystallization of calcium phosphate were undertaken by using synthetic wastewater with 10 mg/L P phosphate. It shows that AP has bad enduring property in the crystallization process, while JP has better performance for multiple uses, and M-JP is a hopeful seed for P recovery by crystallization of calcium phosphate.  相似文献   

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