超声、过硫酸钾协同去除水中诺氟沙星的效果

过硫酸钾活化可产生强氧化性硫酸根自由基(SO-4·),采用超声/过硫酸钾体系氧化降解诺氟沙星,考察了过硫酸钾浓度、诺氟沙星初始浓度、溶液初始p H值及自由基淬灭剂甲醇、叔丁醇对降解效果的影响.结果表明,超声/过硫酸钾体系能够显著降解和矿化诺氟沙星,与单独过硫酸钾、超声相比,超声/过硫酸钾对诺氟沙星的去除率分别提高了3.2和8.9倍,降解过程符合一级反应动力学.诺氟沙星的去除率随过硫酸钾浓度的增加趋于平缓.p H对诺氟沙星的降解影响较大,这是因为随p H的升高,体系中的氧化性物种由SO-4·转化为以SO-4·/HO·为主.TOC去除和大肠杆菌抗菌实验表明,反应180 min,超声/过硫酸钾能够实现49.12%的诺氟沙星矿化,且对大肠杆菌的抑菌圈直径由45 mm减小到14 mm(滤纸直径),完全去除其抗菌性.结果表明超声/过硫酸钾能够有效用于诺氟沙星废水处理.     

Activated carbon enhanced ozonation of oxalate attributed to HO. oxidation in bulk solution and surface oxidation： Effect of activated carbon dosage and pH

Ozonation of oxalate in aqueous phase was performed with a commercial activated carbon（AC）in this work. The effect of AC dosage and solution pH on the contribution of hydroxyl radicals（HOU） in bulk solution and oxidation on the AC surface to the removal of oxalate was studied. We found that the removal of oxalate was reduced by tert-butyl alcohol（tBA） with low dosages of AC,while it was hardly affected by tBA when the AC dosage was greater than 0.3 g/L. tBA also inhibited ozone decomposition when the AC dosage was no more than 0.05 g/L, but it did not work when the AC dosage was no less than 0.1 g/L. These observations indicate that HOUin bulk solution and oxidation on the AC surface both contribute to the removal of oxalate. HOU oxidation in bulk solution is significant when the dosage of AC is low, whereas surface oxidation is dominant when the dosage of AC is high. The oxalate removal decreased with increasing pH of the solution with an AC dosage of 0.5 g/L. The degradation of oxalate occurs mainly through surface oxidation in acid and neutral solution, but through HOUoxidation in basic bulk solution. A mechanism involving both HOUoxidation in bulk solution and surface oxidation was proposed for AC enhanced ozonation of oxalate.     

碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝

在课题组前期研究的基础上,以碳纳米管(MWCNTs)为载体制备了Fe3O4/MWCNTs复合物并作为催化剂,以染料亚甲基蓝(MB)为降解对象,研究了该催化剂催化H2O2对亚甲基蓝溶液的降解特性及其影响因素,并考察了催化剂的重复使用效果,探讨了催化反应的机理.结果表明,在pH值3~8的范围内,催化反应体系都能有效降解MB,最佳pH值为3.5.随着催化剂投量的增加,MB的降解率明显提高,500 mg·L-1催化剂投量条件下,MB的降解率最高.随着H2O2初始浓度的增加,MB的降解率增加,10 mmol·L-1时MB的降解率最高.溶液中共存的阴离子会降低MB的降解率.在最佳条件,即温度25℃、H2O2浓度10 mmol·L-1、催化剂浓度500 mg·L-1的条件下,0.20 mmol·L-1MB在30 min内的降解率达到99.1%.催化剂重复使用后仍然具有较好的催化活性,说明Fe3O4在MWCNTs表面负载比较牢固,催化剂具有反复使用的能力.催化反应机理是催化剂催化H2O2产生羟基自由基,高活性的羟基自由基氧化MB.     

Heterogeneous Fenton-like degradation of 4-chlorophenol using iron/ordered mesoporous carbon catalyst

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.     

An Empirical, Quantitative Approach to Predict the Reactivity of Some Substituted Aromatic Compounds Towards Reactive Radical Species (Cl2-·, Br2-·, ·NO2, SO3-·, SO4-·) in Aqueous Solution (3 pp)

The Hammett approach, applied to the reaction of various classes of aromatic compounds with the radicals Cl2-*, Br2-*, *NO2, SO3-*, and SO4-* yielded good predictive models, supported by high values of the correlation coefficient r2 in the case of phenols with Cl2-* and of phenolates with *NO2 and SO3-*. Lower but statistically significant correlation coefficients could be obtained for benzoates with Cl2-*, phenolates with Br2-*, and benzoates and anisoles with SO4-*.     

Herbicide Roundup® and its main constituents cause oxidative stress and inhibit acetylcholinesterase in liver of Carassius auratus

Roundup® is a glyphosate-based herbicide containing a mixture of surfactants. This paper evaluates the toxic effects of Roundup® and its main constituents on the goldfish, Carassius auratus, after 7 days exposure. Fish were exposed to 0.16, 0.032 and 0.0064 mg/L of Roundup® [containing 41% isopropylamine salt of glyphosate (G.I.S) and 18% polyoxyethylene amine (POEA)], G.I.S, and POEA. Their livers were taken for determining reactive oxygen species (ROS), superoxide dismutase (SOD) activity, malondialdehye (MDA) content and acetylcholinesterase (AChE) activity. Hydroxyl radical (·OH) could be induced by exposing Roundup® at a rate of 43%–111%, G.I.S at 90%–124% and POEA at142%–157%. A decreased SOD activity was observed in fish exposed to G.I.S and POEA. The contents of MDA significantly increased when exposed to Roundup® at all concentrations, 0.16 mg/L G.I.S and 0.032 mg/L POEA. The exposure led to an inhibition of AChE in livers overall during the experimental periods. POEA was more toxic than Roundup® or G.I.S during this experiment. AChE and ·OH are supposed to be sensitive biomarkers of the exposure of Roundup® and its main constituents to C. auratus.     

高级氧化技术处理垃圾渗滤液的研究进展

本文介绍了包括化学氧化法、电化学氧化法、光催化氧化法、超声氧化法、辐照氧化法和催化湿式氧化法等在内的高级氧化技术的机理和运用于垃圾渗滤液处理的研究进展,并提出高级氧化技术与生物处理联合运用和各种高级氧化工艺之间的优化组合将是实现高级氧化技术在垃圾渗滤液处理中工程化运用的发展方向.     

亚铁－过氧化氢氧化法处理染料中间体H酸生产废液的研究

Ｈ酸生产过程中排出的废液中含有大量萘的衍生物,对生物具有毒性,是目前最难处理的废水之一。本研究采用亚铁－过氧化氢氧化法对该废液进行处理,以改善它的可生化性能,降低水中有机物的溶解性,提高混凝处理效率。结果表明,最佳pH值为2～4,亚铁的适宜投加量为200mg/L,当H₂O₂投加量为30g/L时,COD去除率为50％,废水已具有可生化性。经亚铁－过氧化氢氧化处理（H₂O₂的投加量为3g/L）后的废液,再用FeCl₃进行两级混凝处理（FeCl₃的量分别为15和5g/L）,COD的去除率达90％,H酸氧化过程中,HO先和萘环上的钝化基团发生置换反应,使萘环活化,进一步氧化,萘环裂解,最终转化为无机物。研究结果对提高该种废水生物处理效率有实用意义。     

电化学法直接快速测定COD初步研究

对一种全新的方法—电化学法测定COD进行了初步研究。制备出析氧超电位很大的铂基α PbO2 和 β PbO2 双镀层电极 ,并用以电解产生羟基自由基直接氧化废水中有机物。在本研究确定的条件下 ,COD标液在 0～ 30 0mg L呈良好的线性关系 ,一次测定仅需 30s。     

负载型TiO2催化臭氧化去除腐殖酸的实验研究

以实验室自制的负载型TiO2为催化剂,研究了其对水中溶解性腐殖酸的催化臭氧化效能。结果表明负载型TiO2对臭氧化去除溶解性腐殖酸有明显的催化作用,反应25min,对腐殖酸的去除率可达到86.8%,较单独臭氧化提高了28.8%;通过Na2CO3对催化反应的影响间接推断TiO2催化臭氧化反应遵循自由基反应的原理;实验最佳条件为:催化剂涂膜层数6层、焙烧温度700℃、溶液pH=10、放电电流0.4A、反应溶液初始浓度10mg/L;催化剂重复使用8次后,其催化活性变化较小,溶液中无钛离子溶出。