磺胺氯哒嗪在海水中的间接光降解

以有色溶解有机物(CDOM)作为主要光敏剂研究磺胺氯哒嗪(SCP)间接光降解行为和机理,分析CDOM组成、盐度和pH值对SCP间接光降解的影响.SCP间接光降解速率随CDOM浓度升高而逐渐加快.CDOM产生的光化学反应活性中间体对SCP间接光降解的贡献率不同,其中³CDOM^*起主要作用,对SCP间接光降解的贡献率高达77.94%.所用CDOM由4种荧光组分组成,包含3种外源腐殖质(C1,C2,C3)和1种内源腐殖质(C4), SCP间接光降解去除率和³CDOM^*浓度分别与荧光组分的相关性大小顺序均为C3>C2>C4>C1.其中C3和C2与[³CDOM^*]具有较高线性相关性(R²>0.97),是³CDOM^*的主要贡献者.盐度和pH值对SCP间接光降解的影响作用显著.在盐度为15‰时,SCP的间接光降解速率最大.在低盐度范围(0~15‰)内,离子强度效应对间接光降解的促进作用大于无机阴离子带来的抑制作用,使得间接光降解速率随着盐度的升高而加快.溶液pH=(5.00±0.10)时,SCP的间接光降解速率最大.SCP的间接光降解速率随着溶液pH值的升高而减慢,中性和碱性环境不利于SCP的间接光降解.     

分子识别作用下光催化降解偶氮染料酸性红GR

合成了β-环糊精(β-CD)与偶氮染料酸性红GR(ARGR)的包结物,并采用红外光谱仪对ARGR、β-CD及β-CD与ARGR的包结物进行了表征,表征结果显示,β-CD与ARGR的包结物的特征峰的峰形和强度与β-CD相似,但峰位有明显的偏移,说明ARGR进入了β-CD空腔与β-CD发生了分子识别作用。采用TiO2作为催化剂,研究了β-CD分子识别后ARGR的光催化降解行为,实验结果表明,在ARGR质量浓度为20.0 mg/L、β-CD浓度为1.8×10-5 mol/L、体系pH为4.0、TiO2加入量为1.0 g/L、光催化反应时间为60 min的条件下,经β-CD分子识别后ARGR的光催化降解率可达100%。     

Efficiency and degradation products elucidation of the photodegradation of mefenpyrdiethyl in water interface using TiO2 P-25 and Hombikat UV100

The photodegradation of mefenpyrdiethyl (MFD), an herbicide safener, was investigated in aqueous suspensions by using Degussa P-25 and Hombikat UV100 titanium oxide under simulated sunlight irradiation. The effects of initial concentration of the herbicide, pH, catalysts and hydrogen peroxide doses as well as their combinations were studied and optimized. Accordingly, the kinetic parameters were determined and the effectiveness of the processes was assessed by calculating the rate constants. A pseudo first-order kinetics was observed. Under experimental conditions, the degradation rate constants were strongly influenced using P-25 and no noticeable effect was observed for Hombikat UV100. DFT calculations with B3LYP/6-311+G(2d,p)//B3LYP/6-31+G(d,p) level of theory were performed to check whether significant conformational changes occur when the charge state of the MFD substrate changes and whether these changes could play a role in the dependency of photodegradation rate constant on the studied pH. High resolution mass spectrometry (FT-ICR/MS) was implemented to identify the main degradation products.     

Photodegradation of amoxicillin by catalyzed Fe3+/H2O2 process

Three oxidation processes of UV-Fe³⁺(EDTA)/H₂O₂ (UV: ultraviolet light; EDTA: ethylenediaminetetraacetic acid), UV-Fe³⁺/H₂O₂ and Fe³⁺/H₂O₂ were simultaneously investigated for the degradation of amoxicillin at pH 7.0. The results indicated that, 100% amoxicillin degradation and 81.9% chemical oxygen demand (COD_Cr) removal could be achieved in the UV-Fe³⁺ (EDTA)/H₂O₂ process. The treatment efficiency of amoxicillin and COD_Cr removal were found to decrease to 59.0% and 43.0% in the UV-Fe³⁺/H₂O₂ process; 39.6% and 31.3% in the Fe³⁺/H₂O₂ process. Moreover, the results of biodegradability (biological oxygen demand (BOD₅)/COD_Cr ratio) revealed that the UV-Fe³⁺ (EDTA)/H₂O₂ process was a promising strategy to degrade amoxicillin as the biodegradability of the effluent was improved to 0.45, compared with the cases of UV-Fe³⁺/H₂O₂ (0.25) and Fe³⁺/H₂O₂ (0.10) processes. Therefore, it could be deduced that EDTA and UV light performed synergetic catalytic effect on the Fe³⁺/H₂O₂ process, enhancing the treatment efficiency. The degradation mechanisms were also investigated via UV-Vis spectra, and high performance liquid chromatography-mass spectra. The degradation pathway of amoxicillin was further proposed.     

紫外光降解对生物过滤塔去除氯苯性能的影响机制研究

紫外-生物过滤联合工艺中的紫外单元促进了后续生物过滤单元的氯苯去除性能.为了进一步揭示紫外光降解对生物过滤塔运行性能的影响机制,本研究系统分析了紫外光降解对生物过滤塔填料层pH、生物膜特性和填料层结构特性等方面的影响.结果表明,氯苯紫外光降解产物导致了生物过滤单元填料层pH的下降(从pH 6～8降至pH 4～7);另外,紫外单元产生的臭氧降低了生物过滤单元生物膜厚度和生物膜的EPS含量,改善了生物膜的特性,提高了氯苯和营养物质在生物膜内的传质效率.同时,臭氧可以有效控制生物量过量积累,增加了填料层的比表面积(从784 m2.m-3增加至880 m2.m-3),优化了填料层的结构特性,提高了污染物的反应速率.上述各方面的综合作用最终促进了生物过滤单元的氯苯去除性能.     

阿替洛尔在硝酸根溶液中的光降解研究

以氙灯为模拟太阳光光源,研究了β阻滞剂阿替洛尔(ATL)在硝酸根溶液中的光解,探讨了硝酸根离子浓度、溶液pH值、碳酸氢根离子浓度和腐殖质浓度对ATL光解的影响.结果表明,ATL在不同浓度硝酸根溶液中的光解反应符合准一级动力学规律,增大硝酸根离子浓度促进了ATL的光降解率,当硝酸根离子浓度由0增至5 mmol.L-1时其速率常数由0.002 26min-1增至0.009 4 min-1;酸性或碱性溶液有利于ATL在硝酸根溶液中的光解,碳酸氢根离子浓度对光解无明显影响,而加入Suwannee富里酸(SRFA)对光解产生抑制作用.采用异丙醇作为羟基自由基分子探针检测到.OH存在于ATL光解过程中.采用SPE-LC-MS方法鉴定了ATL在硝酸根溶液中的主要光解产物,并提出了可能的光解途径.     

Photodegradation mechanism of deltamethrin and fenvalerate

To understand the degradation and environmental fate of pyrethroids, the process of their photodegradation under simulated natural conditions was investigated. The results showed that the degradation process follows first-order kinetics. The degradation intermediates were identified with gas chromatography-mass spectrometry. A plausible mechanism was discussed to explain the process. Several influences on degradation process were investigated and reported such as the e ects of initial concentration of pyrethroids, total time of light irradiation, solvents, and light source, as well as the e ect of a few substances that exist in the environment. This study could be a good reference for the degradation of pyrethroids in practical circumstances.     

β-环糊精衍生物对甲基对硫磷的增溶洗脱和光降解

研究了3种新型β-环糊精衍生物(谷氨酸-β-环糊精、乙二胺-β-环糊精、羧甲基-β-环糊精)对甲基对硫磷的增溶作用、土壤中甲基对硫磷的洗脱作用以及对甲基对硫磷的光降解作用.研究表明,这三种β-环糊精衍生物都能显著地增加甲基对硫磷在水中的溶解度,并且相对增溶倍数与β-环糊精衍生物的浓度成正相关;120g/L的上述3种β-环糊精衍生物溶液中,甲基对硫磷的溶解度比在纯水中分别提高了117.82倍、80.99倍、47.28倍;β-环糊精衍生物能有效洗脱去除土壤中的甲基对硫磷,其中120g/L的谷氨酸-β-环糊精溶液的累积去除率最高,达103.9%,洗脱液浓度是影响洗脱去除率的主要因素;β-环糊精衍生物能促进甲基对硫磷的光降解,在3g/L的谷氨酸-β-环糊精、乙二胺-β-环糊精、羧甲基-β-环糊精溶液中甲基对硫磷光解速率分别为80.26%、91.53%、76.39%。     

对硝基苯胺的光化学降解研究

系统研究了氙灯和高压汞灯照射下对硝基苯胺(PNA)在蒸馏水、人工海水和天然海水中的光化学降解情况.结果表明,PNA光降解速率会受到光源、溶液介质、温度、起始浓度、重金属离子、甲醇及过氧化氢浓度的影响.随着光源强度的增强、起始浓度的增大、温度的增高和过氧化氢量的增加,PNA在海水中光降解速率相应加快;然而甲醇的加入可有效...     

水热法制备BiVO4及其可见光催化降解糖蜜酒精废水

以Bi(NO3)3•5H2O为铋源,NH4VO3为钒源,采用简单的水热法制备了BiVO4 光催化剂,并用X-射线衍射(XRD)、扫描电子显微镜(SEM)、红外光谱(IR)和紫外-可见光漫反射光谱(UV-vis)对产品进行了结构表征。同时,在BiVO4光催化降解糖蜜酒精废水反应中考察了催化剂用量、通氧量、溶液pH值、双氧水用量及光照强度对糖蜜酒精废水脱色率的影响。实验结果表明,水热产品属于单斜晶系BiVO4,其带隙能为2.398 eV,并具有良好的可见光催化活性。当降解经30倍稀释的糖蜜酒精废水,BiVO4添加量为3.0 g•L−1 ,通氧量为120 L•h-1,助氧化剂H2O2添加量为9 %,不改变废水pH值,在400W镝灯离液面11cm照射反应180 min的条件下,糖蜜酒精废水的脱色率为88.60 %,COD去除率为25.84%,而添加5g•L−1的FeSO4•7H2O后其脱色率和COD去除率分别提高到90.90 %和91.26%。单斜晶型BiVO4晶体的可见光催化糖蜜酒精废水过程符合一级动力学反应。