Fe-pillared clay as a Fenton-type heterogeneous catalyst for cinnamic acid degradation

Fe-pillared montmorillonite has been used as a Fenton-type heterogeneous catalyst for the removal of cinnamic acid in water. The influences of the cinnamic acid, catalyst and H2O2 concentrations and pH on the removal rate of cinnamic acid have been studied. The results show that the efficiency of Fe-pillared montmorillonite is higher than that of the Fe ions in the homogeneous phase, and less sensitive to pH.     

铁炭复配修复地下水中NO_3~--N的条件研究

采用了铁炭复配修复地下水中NO3--N,探讨了实验条件对修复效果的影响。结果表明,在pH值近中性条件(初始pH 6.42)下,反应时间为1 h时NO3--N修复率达到60.85%;Fe/C=1∶1时介质最佳用量分别为4~5 g;Fe/C=1/1.5时修复率为72.80%;反应速率在高振荡强度下大于低振荡强度;氧化铜的催化效果最好,可使修复率提高7.5个百分点。铁炭复配介质修复地下水中NO3--N是有效可行的,修复率随反应时间的增加而提高,在Fe/C=1∶1时修复率与介质用量呈正相关,无限减小Fe/C比并不能无限提高修复率,振荡强度对修复具有显著影响,低振荡强度下的修复过程较高强度存在滞后现象,并非所有金属氧化物催化剂对铁炭修复NO3--N均有促进作用。     

Photochemical behaviour of musk tibetene

BACKGROUND: Synthetic musk compounds are widely used as additives in personal care and household products. The photochemical degradation of musk tibetene in aqueous solutions or in acetonitrile/water mixtures under different conditions was studied in order to assess its environmental fate. METHODS: Musk tibetene dissolved (or suspended) in water and/or acetonitrile/water mixtures was irradiated at different times by UV-light and by solar light. The irradiation mixtures were analyzed by NMR and TLC. The photoproducts formed were identified by GC-MS and NMR data. RESULTS: The experimental results indicated that musk tibetene was photodegradable in water or acetonitrile/water mixtures with half-life reaction times close to 20 minutes. The irradiation mixtures were separated by chromatographic techniques yielding three photoproducts (3,3,5,6,7-pentamethyl-4-nitro-3H-indole, 3,3,5,6,7-pentamethyl-4-nitro-1H-indoline and 3,3,5,6,7-pentamethyl-4-nitro-3H-indolinone) identified by means of spectroscopic analysis. DISCUSSION: The numerical modelling of the photodegradation concentration-time profiles gave (8.13 +/- 0.15) x 10(-2) and (1.34 +/- 0.04) x 10(-2) mol/E for the overall primary quantum yield of direct photolysis for musk tibetene and the major intermediate (3,3,5,6,7-pentamethyl-4-nitro-3H-indolinone), respectively, in the wavelength range 305-366 nm. The half-life times of photodegradation of the both substances varied from 1-1.5 hours at 20 degrees N during the summer season to 6-10 hours for highest latitudes in winter. CONCLUSIONS: Under solar light, musk tibetene was photolabile in acetonitrile and acetonitrile/water 1/1, while it was slowly degraded when suspended in water. In all media, musk tibetene was photodegraded into three photoproducts. By using a kinetic model, the overall primary quantum yields of direct photolysis of musk tibetene and its main photoproduct, in the wavelength range 305-366 nm, were estimated, indicating that the photodegradation rate for musk tibetene is faster than the photolysis rate of the major by-product. RECOMMENDATIONS AND PERSPECTIVES: The results indicate that, in order to assess the environmental impact of musk tibetene on the aquatic ecosystem, great attention should be focused on the major photoproduct which is proved to be more persistent than the parent compound under light irradiation. The predicted half-life times of direct photolysis for both substances ranged from 1-1.5 hours at 20 degrees N during the summer season to about 6-10 hours for highest latitudes in winter, indicating that, from a photochemical point of view, the environmental persistence of these substances increases by increasing the latitudes and during the cold seasons, making more realistic an intake of these xenobiotic molecules into the food chain of aquatic living organisms. Tanabe reports in his Editorial (Tanabe 2005) that "It is necessary to have knowledge of the global picture of synthetic musk pathways. So, it is conceivable that now is the time to study the transport, persistency, distribution, bioaccumulation and toxic potential of this new environmental menace on a global scale, especially in developing countries". Therefore, the future environmental analysis and investigations on the eco-toxicity of nitro musk compounds should take into account not only the presence of the parent compounds but also their photochemical intermediates or end-by-products.     

大气光化学烟雾反应机理比较(Ⅰ)O3和NOx的比较

在相同初始和排放条件下,对四种应用较广的光化学烟雾反应机理(CB4-99,RADM2,RACM,SAPRC99)进行了比较.研究发现对于O3,在低VOCs/NOx时,四种机理模拟结果相关较小,平均相对标准偏差为7%,在高VOCs/NOx时,平均相对标准偏差为26%,差距较大;对于NOx,多数情况下RACM和RADM2的模拟结果较高,CB4-99和SAPRC99的模拟值偏低,其原因主要来源于不同机理中O3的生成对NOx及VOCs的敏感性不同而造成的.在用模式模拟O3和NOx时,应特别注意机理不同而带来的模拟结果差异.     

土壤与酸的反应时间对土壤酸度及土壤溶液中铝离子形态分布的影响

用两种土壤研究土壤与酸的反应时间对土壤酸度及土壤溶液中铝离子形态分布的影响。结果表明，土壤溶液pH随反应时间增加而增加，安徽红壤pH的增幅大于江西红壤。在pH3.0的HNO3溶液中，土壤溶液中的总铝及Al3 均随反应时间增加而减少，而在pH3．5的HNO3溶液中，土壤溶液中总铝及Al－F络合物先随反应时间的增加而减小．然后又有所增加。     

The use of physiological characteristics for comparison of organic compounds phytotoxicity

The influence of intact (FLT) and photomodified (phFLT) fluoranthene (0.05, 0.5 and 5 μmol l⁻¹) and herbicide Basagran (5, 20, 35 and 50 nmol l⁻¹) on the germination, growth of seedlings and photosynthetic processes in pea plants (Pisum sativum L., cv. Garde) was investigated. The germination was significantly inhibited already by the lowest concentration (0.05 μmol l⁻¹) of FLT and phFLT, while Basagran caused inhibition only in higher concentrations (35 and 50 nmol l⁻¹). The growth of roots was significantly inhibited by higher concentration 5 μmol l⁻¹ of both FLT and phFLT and the shoot of seedlings was significantly influenced only by photomodified form. The length of root and shoot was inhibited already by concentration 5 nmol l⁻¹ of Basagran. Organic compounds applied on chloroplasts suspension influenced primary photochemical processes of photosynthesis. In chlorophyll fluorescence parameters, the significant increase of F₀ values and the decrease of F_V/F_M and Φ_II values by application of FLT (0.5 and 5 μmol l⁻¹) and phFLT (0.05, 0.5 and 5 μmol l⁻¹) was recorded. The maximum capacity of PSII (F_V/F_M) was influenced by the highest (50 nmol l⁻¹) and the effective quantum yield of PSII (Φ_II) already by the lowest (5 nmol l⁻¹) concentration of Basagran. Hill reaction activity decreased and was significantly inhibited by higher concentration (0.5 and 5 μmol l⁻¹) of FLT and phFLT and already by the lowest concentration (5 nmol l⁻¹) of Basagran.     

北京夏季典型PM2.5与O3相继重污染事件分析

根据北京市环境保护监测中心发布的PM2.5和O3小时质量浓度及气象、卫星遥感数据,分析了2013年7月2日至10日北京典型PM2.5及O3重污染过程的质量浓度特征及在大气边界层过程各个阶段的质量浓度演变.结果表明,北京夏季O3质量浓度先于PM2.5达到峰值,而天气型演变是导致这一现象的主要原因.具体过程为:1)重污染初始阶段,高压天气型利于前体物积累,PM2.5及O3质量浓度升高;2)在反气旋中部,由于各种污染物质量浓度较低,对大气紫外波段辐射的吸收较弱,导致该阶段紫外辐射强,因而加快了O3生成的光化学反应,O3质量浓度最先达到峰值;3)在反气旋后部,随PM2.5质量浓度增加,辐射变弱,因此O3质量浓度增加速度下降,而受高压后部影响,区域内PM2.5经东南风输送通道进入北京,导致北京PM2.5质量浓度相继达到峰值;4)在重污染清除阶段,在北方反气旋前部的冷锋清除作用下,PM2.5及O3质量浓度同时降低至谷值.     

前车突然切入时驾驶人应激生理特性研究

为研究前车突然切入对驾驶人生理负荷的影响,利用MP150生理监测系统对22名被试进行虚拟驾驶试验。采集记录前车突然切入时被试的生理参数。研究驾驶人心率增长率和心率变异性(HRV)指标与车速、应激距离之间的关系。结果表明:自车速度为100 km/h时,随着前车切入距离从55.6 m减小到27.8 m,被试的平均心率增长率从16.21%增大到23.27%,HRV参数低频(LF)值也呈现下降趋势。前车切入距离一定,随着自车车速从60 km/h增加到120 km/h,被试的平均心率增长率存在显著性差异,平均从13.05%上升到21.85%。差异性检验结果表明,前车切入距离和自车速度发生变化时驾驶人的生理负荷变化趋势一致,但自车速度因素对驾驶人生理负荷的影响程度高于切入距离因素。     

反应气氛对绿色合成纳米铁的组分及其活性的影响

成本低廉和无二次污染的"绿色"合成纳米材料是发展原位纳米环境修复技术的前沿研究课题之一.本文以绿茶提取液为还原剂和稳定剂进行"绿色"合成纳米铁,探讨在不同的气氛下"绿色"合成的纳米铁颗粒的主要成分,以期为调控合成纳米铁系材料提供基础研究.首先,利用扫描电子显微镜(SEM)、X射线能谱(EDS)、X射线光电子能谱分析(XPS)和傅里叶变换红外光谱(FTIR)等表征手段对不同反应气氛下合成的纳米铁颗粒的表面微观形貌、尺寸和价态结构进行分析.结果发现,在通入N2情况下,合成的纳米铁颗粒粒径为(84.7±11.5)nm,其主要成分以纳米零价铁为主;在通入空气情况下,合成的纳米铁粒径为(117.8±26.2)nm,其主要成分是纳米零价铁、氧化铁和四氧化三铁的混合物;通入O2时,合成的纳米铁粒径为(141.2±26.3)nm,其主要成分以四氧化三铁为主.其次,评价在不同气氛条件下合成纳米铁颗粒对去除亚甲基蓝(MB)的反应活性.结果表明,在反应温度313 K下降解初始浓度为50 mg·L-1的MB溶液,反应5 min时已达到平衡,通入N2合成的纳米铁降解MB,去除率高达98.7%,而通入O2合成的纳米铁反应效率低,对MB的去除率仅为65.3%.最后,从以上发现提出不同气氛下可以调控"绿色"合成的铁系纳米材料成分,从而导致不同的纳米修复环境中污染物的能力.     

内循环厌氧反应器流动模型及反应过程模拟

为揭示内循环厌氧反应器放大过程中所出现的规律,本文对反应器中流动模型和反应过程进行了模拟研究,通过对主反应区的停留时间分布的实验研究,确定了主反应区流型可用一平推流与两个并联的全混流进行串联的三参数组合模型进行模拟.在实验范围内,平推流区所占的体积分数约为36%,两个全混流区所占的体积分数分别为53%和11%.结合厌氧反应动力学方程,应用组合模型模拟了实际反应器的状态,并和实验值进行了对比,发现反应器出口处CH_4体积流量最大误差为9.67%,在可允许的范围内.同时,模拟了基质初始COD和温度变化对反应器出口状态的影响.研究表明,与其它模型相比,组合模型计算简洁,同时又有较好的精度,能够满足反应器的设计需要.