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.     

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.     

Nitrifying population dynamics in a redox stratified membrane biofilm reactor (RSMBR) for treating ammonium-rich wastewater

Nitrogen removal performance and nitrifying population dynamics were investigated in a redox stratified membrane biofilm reactor (RSMBR) under oxygen limited condition to treat ammonium-rich wastewater. When the NH4+-N loading rate increased from 11.1±1.0 to 37.2±3.2 gNH4+-N·m-2·d-1, the nitrogen removal in the RSMBR system increased from 18.0±9.6 mgN·d^-1 to 128.9±61.7 mgN·d^-1. Shortcut nitrogen removal was achieved with nitrite accumulation of about 22.3±5.3 mgNO2--N·L-1. Confocal micrographs showed the stratified distributions of nitrifiers and denitrifiers in the membrane aerated biofilms (MABs) at day 120, i.e., ammonia and nitrite oxidizing bacteria (AOB and NOB) were dominant in the region adjacent to the membrane, while heterotrophic bacteria propagated at the top of the biofilm. Real-time qPCR results showed that the abundance of amoA gene was two orders of magnitude higher than the abundance of nxrA gene in the MABs. However, the nxrA gene was always detected during the operation time, which indicates the difficulty of complete washout of NOB in MABs. The growth of heterotrophic bacteria compromised the dominance of nitrifiers in biofilm communities, but it enhanced the denitrification performance of the RSMBR system. Applying a high ammonia loading together with oxygen limitation was found to be an effective way to start nitrite accumulation in MABs, but other approaches were needed to sustain or improve the extent of nitritation in nitrogen conversion in MABs.     

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.     

沉降除藻协同沉积物覆盖对藻华水体甲烷释放的影响

本研究以藻华水体甲烷释放为对象,利用模拟柱培养实验,探究了沉降除藻和沉积物覆盖复合技术对富营养化甲烷释放的影响.结果表明,沉降除藻结合沉积物覆盖处理可有效改善水环境,实现对甲烷释放的控制,但不同覆盖材料的效果存在差异;活性炭效果要优于土壤和沸石.相比于对照体系水体溶解氧(DO)2. 5 mg·L-1和氧化还原电位(ORP)100 m V,沉积物界面ORP -125 m V,沉降除藻协同活性炭覆盖体系中水体DO和ORP分别升高至3. 1 mg·L-1和174 m V,沉积物界面ORP逆转为168 m V,实验期间甲烷释放量相对于对照组减少90. 2%.研究结果在富营养水体甲烷减排方面具有指导性意义.     

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).     

Variations of dominant microbial populations in groundwater in response to the leachate from Laogang Landfill

Temporal changes of dominant microbial populations in groundwater in response to the leachate from Shanghai Laogang Landfill were investigated. Concentrations of dissolved redox-relevant species in groundwater suggested that the dominating redox process had changed from denitrification to methane-production/sulfate-reduction due to landfilling. Dominant microbial populations were determined using restriction fragment length polymorphism(RFLP) analyses of 16S rRNA gene libraries, which were further studied by sequencing and phylogenetic analyses. The results indicated that obvious shifts of dominant microbial populations had occurred in groundwater in response to the pollution of leachate. The closest relatives of some dominant clones are accordant with the dominating redox processes determined by hydrochemical analyses, based on the GenBank‘s indications on the ability to perform redox reactions.     

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.     

污染场地地下水中汞污染反应运移模拟

汞（Hg）是人们持续关注的全球环境污染物之一,其对地下水的污染严重威胁着与地下水相关的生态环境系统.汞在地下水系统中的物理与地球化学反应过程的准确刻画是研究汞迁移转化规律的重点和难点.基于某工业场地汞污染数据,首先采用PHREEQC研究地下水中无机二价汞的存在形态,然后利用PHT3D程序建立汞污染物反应性溶质运移二维剖面模型.该模型考虑了汞污染物在地下水系统中的对流、弥散过程及地球化学反应过程（包括水相络合作用、表面络合吸附作用及受动力学控制的氧化还原作用）.结果表明,无机二价汞的存在形态以HgCl₂和Hg（OH）Cl占主导地位,氧化还原作用是影响地下水中汞污染反应性运移的主要控制因素;另一方面,水合氧化铁HFO对汞迁移的阻滞影响较小,而溶解性有机质对汞较强的络合作用不能忽视.本文研究成果可为预测与评估特定污染场地地下水汞污染的变化趋势及制定相应的修复策略提供科学依据.