Effects of WOx modification on the activity, adsorption and redox properties of CeO2 catalyst for NOx reduction with ammonia

A series of WO₃/CeO₂ (WOx/CeO₂) catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO₂ support. The resulting solid acid catalysts were characterized by X-ray diffraction (XRD), UV-Vis spectroscopy (UV-Vis), Raman spectroscopy (Raman), in-situ Fourier transform infrared spectroscopy (in-situ FT-IR) of ammonia adsorption, NH₃-TPD, H₂ temperature-programmed reduction (H₂-TPR), NH₃/NO oxidation and activity measurements for NOx reduction by NH₃ (NH₃-SCR). The results show that polytungstate (WOx) species are the main species of tungsten oxide on the surface of ceria. The addition of tungsten oxide enhances the Brönsted acidity of ceria catalysts remarkably and decreases the amount of surface oxygen on ceria, with strong interaction between CeO₂ and WOx. As a result, the N₂ selectivity of NH₃ oxidation and NH₃-SCR at high temperatures (> 300℃) is enhanced. Therefore, a wide working temperature window in which NOx conversion exceeds 80% (NOx conversion > 80%) from 200 to 450℃, is achieved over 10 wt.% WOx/CeO₂ catalyst. A tentative model of the NH₃-SCR reaction route on WOx/CeO₂ catalysts is presented.     

零价铁（ZVI）去除Cu2+的特性及机制研究

研究了零价铁去除水溶液中铜离子的影响因素及动力学特性,并利用X射线衍射(XRD)分析对反应机制进行了探讨.结果表明,当溶液中Cu2+的浓度为300 mg/L,零价铁的用量为1 g/L时,Cu2+的去除率99%.Cu2+的去除速度很快,且反应前30min零价铁去除Cu2+的过程可以用一级反应动力学方程模拟.零价铁去除Cu2+的机制主要基于氧化还原反应,Cu2+的还原产物主要为Cu和Cu2O.     

水固液微界面氧化还原反应过程与污染物控制研究

本文介绍了3个反应体系,包括铁锰复合氧化物氧化吸附除砷体系、铁氧化物包覆零价铁光芬顿催化和负载型多价态锰氧化物臭氧催化体系,通过固液微界面不同的氧化还原反应,实现了对水中砷和难降解有机污染物的高效去除.重点介绍了不同氧化还原反应对污染物转移转化的作用机制,说明了水体中固液微界面氧化还原反应,对污染物的转移转化起着重要作用.     

Quinone-mediated decolorization of sulfonated azo dyes by cells and cell extracts from Sphingomonas xenophaga

The effects of various quinone compounds on the decolorization rates of sulfonated azo dyes by Sphingomonas xenophaga QYY were investigated. The results showed that anthraquinone-2-sulfonate (AQS) was the most effective redox mediator and AQS reduction was the rate-limited step of AQS-mediated decolorization of sulfonated azo dyes. Based on AQS biological toxicity tests, it was assumed that AQS might enter the cells to kill them. In the cytoplasmic extracts from strain QYY, AQS effectively increased decolorization rates of sulfonated azo dyes than other quinone compounds. In addition, we found a NADH/FMN-dependent AQS reductase using nondenaturing polyacrylamide gel electrophoresis (Native-PAGE).     

高盐条件下染料酸性橙7的生物降解特性

对偶氮染料废水厌氧-好氧生物处理中的高盐度抑制生物活性和芳香胺自氧化问题,通过多种强化策略,考察了NaCl为100g/L时酸性橙7(AO7)的生物降解特性.结果表明,加入葡萄糖(0.5g/L)、蛋白胨(1g/L)和酵母粉(0.5g/L)有利于高盐条件下AO7的生物降解.进水中加入酸性红B对AO7的脱色有加速作用.耐盐污泥中加入蒽醌形成的蒽醌-污泥自固定化体系可以促进AO7脱色,当蒽醌浓度为100mg/L时,AO7最大脱色率约为92%.以活性炭毡作为生物载体,厌氧和好氧体系均可实现稳定运行,且体系污泥沉降性良好,脱色速率达26.67mg/(L×h),且可有效抑制脱色中间产物1-氨基-2-萘酚的好氧自氧化,使COD去除率始终保持在90%以上.     

介体厌氧催化活性艳红K-2BP脱色及构效特性研究

研究了筛选出的4种结构相似的醌类氧化还原介体对活性艳红K-2BP厌氧脱色的促进作用,并分析了介体促进效果与其化学结构活性相关性. 在35℃中温厌氧条件下,采用间歇批量实验法,测定不同体系中介体催化活性艳红K-2BP脱色效果.结果表明,①结构相似的醌类氧化还原介体蒽醌(AQ)、1,5-二氯蒽醌(1,5-AQ)、1,8-二氯蒽醌(1,8-AQ)和1,4,5,8-四氯蒽醌(1,4,5,8-AQ),均促进活性艳红K-2BP脱色,反应速率提高了1.4～3倍;②当醌类介体投加浓度为4 mmol·L^-1,活性艳红K-2BP染料浓度为300 mg·L^-1时,促进作用由大到小的顺序为:1,8-AQ>1,5-AQ>AQ>1,4,5,8-AQ;③ 当活性艳红K-2BP染料浓度为300 mg·L^-1时,1,8-AQ促进效果最佳且脱色速率常数随1,8-AQ浓度的增加而增加呈线性关系;④介体促进效果与介体取代基团数量、位置和电子共轭效应相关.本研究初步建立了氧化还原介体定性/定量构-效关系数学模型,探究和完善非水溶性氧化还原介体催化强化理论体系.     

无砾石微孔管地下渗滤系统试验研究

针对传统无砾石管式地下渗滤系统存在的处理性能差,渗滤通量低两个问题,通过去掉包裹织物,提高渗滤管开孔率、改变开孔方式,设计了无砾石微孔管地下渗滤系统。通过实验研究表明,无砾石微孔管地下渗滤系统对COD、氨氮的去除率比传统管式系统分别提高了10.8%、12.7%,总磷去除率并无显著差异,ORP值提高约85 mV,渗滤通量提高26.8%。在3.3 cm/d的水力负荷下,无砾石微孔管地下渗滤系统出水COD、氨氮、总磷平均浓度分别为19 mg/L,0.62 mg/L,0.048 mg/L。渗滤管下10 cm的土壤层去除了约70%的COD,80%的氨氮和91%的总磷,向下随着土壤深度的增加,单位厚度的土壤层去除的污染物量呈显著下降趋势。     

填埋场中铁的生物化学循环对反硝化的影响

在模拟填埋体系中,以填埋场稳定的垃圾为接种物,通过控制有机物和硝氮负荷,研究了铁的生物化学循环对反硝化的影响.结果表明,垃圾填埋场内蕴藏着能实现铁的厌氧氧化还原并同步还原硝氮的复合功能菌群.通过改变有机物和硝氮的负荷,可使得填埋场内持续进行着铁的氧化还原循环和同步氮素转化.从氮素转化产物来看,铁的循环体系中氨氮浓度比传统的反硝化体系低4 mmol·L-1.填埋场内铁的生物化学循环过程对于原位脱氮具有极大贡献.     

Phosphorous cycling and biogeochemistry in a Venezuelan-flooded savanna

In 1970, a programme of land recuperation started in Venezuelan savannas, strongly affected by the seasonality of precipitation; therefore, a network of dykes has been built to alleviate the floods and retain water throughout the dry period. Under the dyked system, the environment has been altered, allowing a change in the herbaceous vegetation towards aquatic species and an increase in primary production. It is assumed that a considerable quantity of nutrients is lost from the ecosystem through the floodgates, a situation that could be worsened with the climate change. This contribution describes the atmospheric input and total output in stream run-off of phosphorous (P) in a flooded savanna. Internal pools of the biogeochemical cycle of P associated with terrestrial compartments are described. In the flooded savanna, a large amount of P is immobilised (29.6?kg?ha^?1) in their above ground biomass by grasses, and in soil microbial biomass. The P budget was nearly balanced, as measured losses were cancelled out by the inputs in rainfall. Soils act as a sink, retaining P coming either from precipitation or from desorption/mineralisation processes. That interruption can be maximised, and losses of P and other nutrients can be minimised with an adequate management of the floodgate.     

1,4-二氯苯在褐土中的残留量变化及对几种土壤酶活性的影响

1,4-二氯苯(1,4-DCB)作为农药和化工产品生产的原料和中间体,在环境中的含量越来越多.采用气相色谱法对不同浓度1,4-DCB处理后土壤中药物残留量进行了测定;对1,4-DCB处理后褐土土壤中几种重要的氧化还原酶(多酚氧化酶、过氧化氢酶、脱氢酶)和脲酶活性进行测定,用其改变来反应1,4-DCB残留对土壤生态系统的影响.结果发现:在1,4-DCB处理30 d后,土壤中1,4-DCB残留保持在44%~50%;1,4-DCB处理后土壤中多酚氧化酶活性呈现先升高后降低的现象,酶活性峰值因作用时间和作用浓度不同而不同.与多酚氧化酶活性改变趋势不同,1,4-DCB处理后土壤脱氢酶活性降低.两种酶活性与1,4-DCB处理浓度之间均具有一定的浓度-效应和时间-效应关系.与多酚氧化酶和脱氢酶活性变化结果不同,1,4-DCB处理后土壤脲酶和过氧化氢酶的活性则随着处理浓度升高和处理时间延长而升高.因此,土壤中不同酶活性对1,4-DCB污染产生了不同的响应.