亚热带土壤氮素反硝化过程中N2O的排放和还原

将采集于江西鹰潭的45个发育于不同成土母质和不同利用方式的土壤样本,在密闭、淹水、充N2的严格厌氧条件下进行了28d的培养试验(30℃),在培育过程中,定期测定NO3--N(加入量为200mg·kg-1)含量和培养瓶上部空间N2O的含量变化.实验结果表明,N2O含量(N)随培养时间t的变化可用方程N=A×(1-exp(-k1 t))-B×exp(k2 t)拟合(A表示培养过程中N2O总排放量;B为常数;k1和k2分别为N2O排放速率常数和还原速率常数,拟合值和实测值之间回归方程的决定系数R2=0.84±0.11).不同土壤之间培养期间N2O总排放量(A)的变异可以用培养7d内被反硝化的NO3--N量和N2O排放率(A值与28d内被反硝化的NO3--N总量的百分比)进行解释(R2=0.829,p＜0.01).被反硝化的NO3--N量则主要受土壤有机碳含量或有机氮矿化量控制,N2O排放率则随k2的增大而呈指数下降(p＜0.01).由此可见,在该实验条件下,还原N2O能力强的土壤,在相同量的NO3--N被反硝化的情形下,排放的N2O可能较少.但影响k2值的主要因素还有待进一步研究.     

亚热带土壤反硝化过程中NO-3-N对CH4排放的影响

研究了发育于不同成土母质和不同土地利用方式下的45个亚热带土壤样本,在反硝化严格厌氧培养条件下（密闭、淹水、充N₂）,加入KNO₃的处理（加入N量为200 mg·kg^-1）和不加KNO₃的空白对照对CH₄产生和排放的影响.结果表明,厌氧培养条件下无论加入KNO₃与否,CH₄的产生和排放首先取决于土壤有机碳总量水平及其有效性.对照土壤中花岗岩母质发育的土壤和KNO₃处理土壤中稻田利用方式下的土壤CH₄排放量最高.加入KNO₃显著抑制了CH₄的产生和排放,NO^-₃-N对CH₄产生的抑制效应可能较N₂O对CH₄产生的抑制效应更大.加入KNO₃处理中厌氧培养第1周内的NO^-₃-反硝化量和降低速率是决定CH₄排放量的关键因素.不加KNO₃的对照土壤中,73％的土样表现为 Fe²⁺的产生和CH₄的排放之间呈指数关系增长,表明Fe³⁺和CO₂的还原可同步进行.NO^-₃-N不仅显著抑制了CH₄的产生和排放,也抑制了Fe³⁺的还原.     

厌氧条件下砂壤水稻土N2、N2O、NO、CO2和CH4排放特征

了解厌氧条件土壤反硝化气体(N2、N2O和NO)、CO2和CH4排放特征,是认识反硝化过程机制的基础,并有助于制定合理的温室气体减排措施.定量反硝化产物组成,可为氮转化过程模型研发制定正确的关键过程参数选取方法或参数化方案.本研究选取质地相同(砂壤土)的两个水稻土为研究对象,通过添加KNO3和葡萄糖的混合溶液,将培养土壤的初始NO-3和DOC含量分别调节到50 mg·kg-1和300 mg·kg-1,采用氦环境培养-气体及碳氮底物直接同步测定方法,研究完全厌氧条件下土壤N2、N2O、NO、CO2和CH4的排放特征,并获得反硝化气态产物中各组分的比率.结果表明,在整个培养过程中,两个供试土壤的N2、N2O和NO累积排放量分别为6~8、20和15~18 mg·kg-1,这些气体排放量测定结果可回收土壤NO-3变化量的95%~98%,反硝化气态产物以N2O和NO为主,其中3种组分的比率分别为15%~19%(N2)、47%~49%(N2O)和34%~36%(NO);但反硝化气体产物组成的逐日动态均显现为从以NO为主逐渐过渡到以N2O为主,最后才发展到以N2为主.以上结果说明,反硝化气体产物组成是随反硝化进程而变化的,在以气体产物组成比率作为关键参数计算各种反硝化气体产生率或排放率的模型中,很有必要重视这一点.     

厌气条件下百菌清对土壤N2O和CH4排放的影响

在密闭、淹水、充N2的严格厌氧条件下对土壤进行了14d的培养试验,研究了杀菌剂百菌清在添加水平为田间施用量（FR）(5.5 mg·kg-1),20倍(20FR)和40倍田间施用量(40FR)时对强酸性、酸性、中性和碱性土壤N2O和CH4排放的影响.结果表明,20FR和40 FR的百菌清能够显著促进N2O向N2的还原,降低N2O排放,在酸性、中性和碱性土壤中培养14d后,对照处理的N2O排放量为0.076~0.46mg·kg-1,而20FR和40FR处理的N2O排放量为0.004~0.06mg·kg-1,降低了１个数量级.反硝化作用和有机氮矿化作用强的土壤中,百菌清减少N2O排放作用更明显.反硝化底物NO-3的存在对CH4的产生与排放具有显著的抑制作用.在加入百菌清未对NO-3浓度产生显著影响的土壤中,百菌清对CH4排放量没有明显影响,在对NO-3浓度产生显著影响的土壤中,CH4排放量随着NO-3的增加而减少,说明百菌清可能通过影响反硝化过程中NO-3的消耗而影响CH4排放.     

亚硝酸盐对外碳源反硝化过程N2O还原的影响

本试验通过批次试验考察了亚硝酸盐对外碳源反硝化过程N2O还原的影响.结果表明NO2--N初始浓度为5.92~35.23mg/L时,随着NO2--N浓度的增加,反硝化过程中N2O的积累量逐渐增加;当NO2--N浓度为35.23mg/L时,NO2--N还原量的46.26%被转化为N2O.通过对比试验得出,N2O还原酶与亚硝酸盐还原酶对电子的竞争和游离亚硝酸(FNA)对N2O还原酶的抑制会导致N2O比还原速率下降,造成反硝化过程N2O积累.基于上述试验结果提出,污水处理厂可通过调控运行条件控制NO2--N浓度,降低反硝化过程的N2O的产生与释放;也可以通过短程硝化提高NO2--N浓度,促进反硝化过程N2O的积累,再通过N2O氧化甲烷减少N2O排放,同时提高产能37%.     

一株硝化脱氮除臭菌的筛选鉴定及其多途径氮代谢功能的研究

从江门某污水处理厂活性污泥中分离出一株能够高效脱除氨气的菌株JN-4.通过菌株形态观察、生理生化及16SrDNA分子鉴定,发现菌株JN-4与枯草芽孢杆菌(Bacillus subtilis)亲缘关系最为接近,同源性达到99%,认为JN-4为一株枯草芽孢杆菌(Bacillus subtilis).好氧培养条件下,以葡萄糖为碳源,JN-4在32h内对NH4+-N和NO2--N的总削减率能够达98.51%和84.50%,体系中总氮的削减率达到63.1%和16.9%,N2的产生量分别为3.72mmol·L-1和0.62mmol·L-1.好氧培养条件下,以KNO3为唯一氮源,NO3--N初始浓度为82.47mg·L-1,32h内体系中NO3--N的总削减率达到96.54%,体系中总氮的削减率达49.6%,产生1.44mmol·L-1的N2,反应中检测到有NH4+-N迅速积累,但会随着时间进行同步转化,可见JN-4不仅能够高效硝化脱氨,同时具有高效好氧反硝化的能力.JN-4在厌氧以及乙酸钠作为碳源的条件下,利用NH4+-N效率大大降低,但是能够在NO3--N存在时进行NO3--N还原(反硝化).JN-4能够进行多途径氮代谢,为一株异养硝化-好氧反硝化偶联的菌株,具有重要的应用价值.     

HRT及氮素负荷对厌氧氨氧化系统的影响

为了考察水力停留时间(HRT)、氮素负荷(NH4+-N和NO2--N)对厌氧氨氧化系统处理效果的影响,通过启动试验、HRT影响试验、NH4+-N负荷试验、NO2--N负荷试验,以好氧硝化污泥、厌氧污泥、花园土壤渗出液为接种污泥,历经114d培养厌氧氨氧化反应器成功启动.结果表明:①系统HRT过短会导致含氮污染物去除不完全,HRT过长则污泥可能已经解体,取HRT为10d是合理的;②厌氧氨氧化系统HRT、微生物总量确定的情况下,系统NH4+-N氧化能力也随之确定,以污泥负荷描述厌氧氨氧化系统NH4+-N氧化能力较为恰当,控制进水NH4+-N污泥负荷小于0.009g.g-1.d-1;③高NO2--N负荷对厌氧氨氧化系统中NH4+-N氧化步骤不产生明显抑制影响,但当NO2--N负荷大于14g.m-3.d-1后,会对厌氧氨氧化系统中NO2--N还原步骤产生抑制,所以控制进水NO2--N容积负荷小于14g.m-3.d-1或折合为污泥负荷0.018g.g-.1d-1是合适的.本研究对厌氧氨氧化系统的设计、运行、管理控制有重要参考意义.     

硫化物型自养反硝化中NO_2~--N与S~0的积累条件

厌氧氨氧化所需的电子受体NO2--N可由亚硝化过程获得也可由半反硝化过程获得。对于含有NO3--N的废水,可通过以S2-为电子供体的自养反硝化过程把NO3--N还原为NO2--N。文章从pH值、S/N摩尔比、硫化物浓度、HRT、COD等方面,探讨以S2-为基质的硫自养反硝化中NO2--N与S0的积累条件,为硫化物型自养反硝化-ANAMMOX工艺提供理论依据。     

S~(2-)/NO_3~--N对硫自养反硝化与厌氧氨氧化耦合脱氮除硫启动的影响

为寻求经济、有效的同步脱氮除硫工艺,采用HABR(复合式厌氧折流板反应器),接种厌氧氨氧化活性污泥,以人工模拟废水为研究对象,在进水p H为8.0、温度为(32±1)℃、HRT为6.5 h的条件下,调整进水S2-/NO3--N〔n(S2-)∶n(NO3--N)〕分别为2.0∶5、3.5∶5、5.0∶5、6.5∶5,研究其对硫自养反硝化和厌氧氨氧化耦合工艺启动的影响,试验连续进行了54 d.结果表明:当S2-/NO3--N1时,S2-的供应量相对不足,导致硫自养反硝化生成的NO2--N量不足,进而影响后续厌氧氨氧化效果,NH4+-N去除率较低,平均值为53.5%,同时剩余NO3--N继续氧化硫自养反硝化生成的S0,致使出水中ρ(SO42-)增大;当S2-/NO3--N=1时,S2-供应量充足,硫自养反硝化生成NO2--N量最大,厌氧氨氧化效果最好,NH4+-N去除率最高,平均值为65.1%;当S2-/NO3--N1时,S2-过量,S2-去除率下降.试验通过控制S2-/NO3--N,在HABR内成功实现了硫自养反硝化和厌氧氨氧化耦合工艺启动,NH4+-N、S2-、NO3--N最大去除率分别为74.3%、99.0%、99.5%,S2-/NO3--N=1为最佳比例.     

3,5-二甲基吡唑对尿素氮转化及NO3--N淋溶的影响

采用室内培养和田间试验相结合的方法,探讨了新型硝化抑制剂3,5-二甲基吡唑(DMP)对尿素氮转化及玉米田硝酸盐淋溶损失的影响.结果表明,DMP对尿素水解仅起短暂的抑制作用,但可在较长时间内显著抑制土壤铵的氧化,且随DMP用量的增加,抑制效应显著增强.培养第10 d时,DMP各处理(0.002 5、0.01及0.025 g/kg)的土壤NH4 -N累积量分别比CK提高了5.17、9.36和11.04倍,而NO3--N累积量于培养第14 d时差异最大,与CK相比分别降低了33.30%、61.19%和73.72%(p＜0.01).土壤NO2--N只在尿素施用前期有少量累积,但第3 d DMP各处理土壤NO2--N含量降低幅度达95.77%～96.13%;土壤矿质氮总量于10 d以后,随DMP用量的增加,显著降低,而DMP1处理的土壤微生物量N在培养14～56 d期间显著提高.连续2 a的玉米田间试验原位取土测定结果表明,2004和2005年,DMP的施用使作物根系密集层以下(40～100 cm)土层的NO3--N累积总量分别比CK降低了28.77%和44.70%.因此,硝化抑制剂DMP与尿素配合施用是调控氮素转化、缓解氮肥污染的有效措施.     

Toxic effects of acetochlor, methamidophos and their combination on nifH gene in soil

Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis （DGGE） and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity （both in gene richness and diversity index values） and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor （50 mg/kg） recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos （150 mg/kg） caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos （250 mg/kg） produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes （bands） responded differently to the impact of agrochemicals： four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.     

Arsenic uptake by arbuscular mycorrhizal maize （Zea mays L.） grown in an arsenic-contaminated soil with added phosphorus

The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.     

Degradation of metabolites accumulated of benzo[a]pyrene by coupling Penicillium Chrysogenum with KMnO4

Several main metabolites of benzo[a]pyrene （BaP） formed by Penicillium chrysogenum, Benzo[a]pyrene-1,6-quinone （BP 1,6- quinone）, trans-7,8-dihydroxy-7,8-dihydrobenzo[a]pyrene （BP 7,8-diol）, 3-hydroxybenzo[a]pyrene （3-OHBP）, were identified by high-performance liquid chromatography （HPLC）. The three metabolites were liable to be accumulated and were hardly further metabolized because of their toxicity to microorganisms. However, their further degradation was essential for the complete degradation of BaP. To enhance their degradation, two methods, degradation by coupling Penicillium chrysogenum with KMnO4 and degradation only by Penicillium chrysogenum, were compared; Meanwhile, the parameters of degradation in the superior method were optimized. The results showed that （1） the method of coupling Penicillium chrysogenum with KMnO4 was better and was the first method to be used in the degradation of BaP and its metabolites; （2） the metabolite, BP 1,6-quinone was the most liable to be accumulated in pure cultures; （3） the effect of degradation was the best when the concentration of KMnO4 in the cultures was 0.01% （w/v）, concentration of the three compounds was 5 mg/L and pH was 6.2. Based on the experimental results, a novel concept with regard to the bioremediation of BaP-contaminated environment was discussed, considering the influence on environmental toxicity of the accumulated metabolites.     

Impact of atrazine and nitrogen fertilizers on the sorption of chlorotoluron in soil and model sorbents

Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.     

Distribution and ecological effect of mercury in Laogang landfill, Shanghai, China

Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury （HgT）, combinative mercury （Hgc） and gaseous mercury （HgG）, and content of total organic carbon （TOC）, but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of （HgG,/HgT）1992〉（HgG/HgT）1996〉〉（HgG/HgT）2000. A simple outline of Hg release in landfill could be drawn： with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants （e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum） are capable of enriching more Hg than herbaceous plants.     

EDTA-enhanced phytoremediation of lead contaminated soil by Bidens maximowicziana

Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.     

Decomposition of alachlor by ozonation and its mechanism

Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.     

Enzymatic oxidation of aqueous pentachlorophenol

The influence of the nonionic surfactant Tween 80 on pentachlorophenol （PCP） oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration （CMC）. Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.     

Removal of heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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