三峡库区小江支流沉积物硝化反硝化速率在蓄水期和泄水期的特征

三峡库区是新形成的生态系统,沉积物特征较之成库前有显著改变;研究库区小江支流——南河沉积物的硝化与反硝化过程可以为库区氮素管理提供科学依据,而反季节蓄水和泄水,沉积物-水界面硝化与反硝化速率特征鲜见报道.实验选取库区开县南河沉积物为研究对象,在2015年泄水期(8月)和蓄水期(11月)采集上、下游以及南河与小流域菁林溪交汇处沉积物样品,测定其理化指标;同时通过实验室模拟沉积物水环境,以乙炔抑制法测定泄水期与蓄水期沉积物的硝化反硝化速率.结果表明,蓄水期沉积物总氮(total nitrogen,TN)、铵态氮(ammonium nitrogen,NH_4~+-N)、硝态氮(Nitrate nitrogen,NO_3~--N)及总有机碳(total organic carbon,TOC)等理化指标均显著高于泄水期(P0.05),这说明蓄水期有外源物质入库;沉积物硝化速率在蓄水期[194.06μmol·(m~2·h)~(-1)]显著高于泄水期[16.52μmol·(m~2·h)~(-1)],且硝化速率与沉积物理化特征(TN、NH_4~+-N、NO_3~--N、TOC)存在显著正相关;沉积物反硝化速率则与硝化速率相反,泄水期[647.20μmol·(m~2·h)~(-1)]高于蓄水期[24.04μmol·(m~2·h)~(-1)],其与沉积物理化指标(TN、NH_4~+-N、NO_3~--N)呈显著负相关.     

淀山湖沉积物的反硝化脱氮能力及其环境意义

于2016年5月和7月,使用乙炔抑制法对淀山湖湖区13个样点表层6 cm原状沉积物反硝化速率进行了测定.结果表明,淀山湖表层沉积物中的反硝化速率具有显著的时空变化特征,变化范围在5.72~65.82μmol·m~(-2)·h~(-1)之间,,春季反硝化速率为(28.52±26.21)μmol·m~(-2)·h~(-1),夏季反硝化速率为(29.31±17.11)μmol·m~(-2)·h~(-1).在空间上,表层0~3 cm沉积物中反硝化速率((17.91±11.80)μmol·m~(-2)·h~(-1))高于下层3~6cm沉积物反硝化速率((11.02±10.40)μmol·m~(-2)·h~(-1));反硝化速率与沉积物中可提取NH_4~+-N含量成显著正相关(p0.05),耦合的硝化-反硝化过程是沉积物反硝化作用的主要机制.淀山湖湖区上半年通过反硝化作用可去除约278.70 t的氮,对控制水体氮浓度和削减氮负荷具有重要意义.     

太子河流域中游地区河流硝酸盐来源及迁移转化过程

选取太子河中游地区为研究对象,联合硝酸盐(NO_3~-)、氯离子(Cl~-)、硝酸盐氮、氧同位素(δ~(15)N和δ~(18)O)和水的氧同位素(δ~(18)O)识别不同季节2016年5月和8月(对应枯水期和丰水期)地表水硝酸盐来源及迁移转化过程.结果表明通过ManWhitney U检验,枯水期ρ(Cl~-)、ρ(NO_3~-)、ρ(NH_4~+-N)和δ~(18)O-NO_3~-显著高于丰水期,δ~(15)N-NO_3~-无显著时间差异.根据NO_3~-/Cl~-,δ~(15)N-NO_3~-和δ~(18)O-NO_3~-的范围,发现不同采样期,硝酸盐主要来自于多种源的混合.丰水期,细河、蓝河和下达河硝酸盐来源是化学肥料、土壤氮和生活污水及畜禽粪便排放废水.二道河主要是土壤氮和化学肥料.枯水期,下达河硝酸盐主要来自于化学肥料和土壤氮,细河、蓝河和二道河硝酸盐来源主要是土壤氮和生活污水及畜禽粪便的排放.丰水期,ρ(NO_3~-)与ρ(NH_4~+)呈负相关关系,与δ~(15)N-NO_3~-呈正相关关系,说明研究区域发生了氨氮的挥发和硝化过程.二道河和蓝河随着ρ(NO_3~-)和ρ(Cl~-)降低,ρ(NH_4~+)和δ~(15)N-NO_3~-增加,说明有明显的反硝化过程发生.不同采样期NO_3~-和Cl~-呈显著正相关关系,表明各采样河流均发生了混合过程.研究结论为丘陵地区硝酸盐来源的季节差异分析提供参考.     

蓝藻水华对太湖水柱反硝化作用的影响

反硝化作用是湖泊水体最主要的脱氮过程,对减轻湖泊的氮素污染和富营养化控制具有重要意义.蓝藻水华暴发和衰亡可能会通过改变水体氮素循环途径及微环境来促使反硝化作用直接在水柱中发生,加速氮的去除.为了验证这一假设,取太湖湖水添加不同生物量的蓝藻和连续10 d的NO_3~--N、PO_4~(3-)-P营养盐,进行蓝藻生长与降解对反硝化影响的模拟实验,测定蓝藻水华期水体藻类生物量和各形态氮浓度的动态变化,同时利用~(15)N同位素添加培养结合膜进样质谱仪(MIMS)实时定量测定反硝化速率.结果表明,蓝藻在生长期吸收氮素转变为颗粒氮,在衰亡期藻细胞通过降解矿化释放了大量的NH_4~+-N,继而转化为NO_3~--N,为反硝化作用提供底物,是大幅度促进水体反硝化作用的关键;反硝化速率(以N2计,下同)最高达到(1 614. 52±301. 57)μmol·(m~2·h)~(-1),是同时期最低蓝藻生物量组反硝化速率[(534. 45±242. 18)μmol·(m~2·h)~(-1)]的3倍,实验结束时添加初始蓝藻生物量倍数最高组的TN去除率达最高(40. 02%),是未添加蓝藻组TN去除率(17. 72%)的2. 26倍,说明蓝藻堆积会显著促进反硝化作用的强度,加速水体氮素的去除.蓝藻衰亡时反硝化速率的快慢受NH_4~+浓度的影响显著,表明附着在藻团的微生物的耦合硝化-反硝化作用是氮盐去除的主要途径.本研究结果表明,水华蓝藻生长期快速吸收氮素转变为颗粒氮,蓝藻死亡降解后通过耦合硝化-反硝化作用加速氮素去除,这可能是太湖夏季氮素浓度降低的原因之一.     

底泥中氮的主要迁移转化过程及其转化模型的研究

研究了NO_3~--N,NH_4~+-N在底泥中的扩散、吸附以及NO_3~--N的反硝化等过程.结果表明,在泥-水界面间,NH_4~+-N主要向上浮水中扩散,NO_3~--N主要向间隙水中扩散.扩散到间隙水中的NO_3~--N45％被吸附,30％因反硝化作用而失掉,其反硝化速率常数在7—11cm层最大.氮的吸附速率常数在表层最大.建立了间隙水中NO_3~--N和NH_4~+-N的转化模型,并计算了氮在泥-水界面间的扩散量,计算结果与实测结果基本相符.     

闽江口互花米草入侵过程对短叶茳芏沼泽沉积物硝化-反硝化作用的影响

2014年4、7、10月和2015年1月在闽江口鳝鱼滩湿地选择未被入侵的短叶茳芏(Cyperus malaccensis)群落(A)、互花米草入侵斑块边缘(B)以及互花米草(Spartina alterniflora)入侵斑块中央(C)为研究对象,基于时空互代研究方法,探讨互花米草入侵序列下湿地沉积物硝化-反硝化变化规律.结果表明:在互花米草入侵序列中,湿地沉积物硝化速率为0.19~1.66μmol·m~(-2)·h~(-1),反硝化速率为12.41~27.19μmol·m~(-2)·h~(-1).沉积物硝化-反硝化作用存在明显的季节变化,硝化速率表现为夏季春季秋季冬季,反硝化速率表现为夏季秋季冬季春季;入侵不同状态下,沉积物硝化速率表现为BCA,反硝化速率表现为CBA.互花米草入侵提高了沉积物-水界面N_2O交换通量.互花米草入侵引起的沉积物pH、NH_4~+-N、含水量、容重和电导率等理化性质的改变是导致不同入侵阶段沉积物硝化-反硝化速率以及N_2O释放差异的重要原因.     

我国典型潮间带沉积物-水界面无机氮源汇效应

以中国东部沿海12个典型潮间带为研究对象,通过室内模拟测定了潮间带沉积物-水界面硝酸盐(NO_3~-)和氨氮(NH_4~+)的源汇通量,分析了沉积物对上覆水体无机氮源汇效应的空间分布特征,以及环境因子的影响.结果发现:(1)NO_3~--N的总通量范围是-2.91~3.34 mmol·(m~2·h)~(-1),NH_4~+-N的总通量范围是-4.36~2.34 mmol·(m~2·h)~(-1).12℃和35℃温度下,无机氮的平均值是-0.04 mmol·(m~2·h)~(-1),我国东部典型潮间带沉积物表现为氨氮和硝氮的有效汇库.(2)潮间带的硝氮和氨氮通量存在纬度分异.12℃时,纬度越高,氨氮硝氮通量值越大;25℃和35℃时,潮间带硝氮通量值大小随纬度的变化为,25°~35°N15°~25°N35°~45°N.而氨氮通量值,25°~35°N15°~25°N35°~45°N.(3)温度通过影响硝化反硝化的耦合作用影响无机氮通量.潮间带的NO_3~--N通量随温度的增加而减小,15°~25°N和35°~45°N地区NO_3~--N通量随温度先升高再降低,25°~35°N地区NO_3~--N通量随温度一直减小.每个纬度区,温度越高,NH_4~+-N通量值越低.(4)上覆水体的盐度、沉积物总有机碳(TOC)、总氮(TN)含量,孔隙水氨氮、硝氮浓度,容重等环境因子对通量没有单一的显著影响,协同影响NO_3~--N、NH_4~+-N在潮滩沉积物水界面的空间分异.     

太湖西部河湖氮污染物来源及转化途径分析

通过2014年枯水、丰水两期监测,综合分析了太湖西部入湖河流与湖区水体及其沉积物的无机氮形态与同位素特征,并利用δ~(15)N识别了太湖西部上游区氮污染来源及转化途径的生物化学作用机制.结果表明:NO_3~--N与NH_4~+-N为研究区域入湖河流无机氮的主要形态,而NO_3~--N为西部湖区水体无机氮的主要形态;δ~(15)N-NO_3~-的数值范围揭示了西部入湖河流在枯水季NO_3~--N主要来源于农用化肥,有少量矿化土壤有机氮,而丰水季则以生活污水为主,有少量矿化土壤有机氮及农用化肥;δ~(15)N-NH_4~+的数值范围说明了生活污水是河流水体NH_4~+-N的主要来源;通过水体及沉积物样品NO_3~--N、NH_4~+-N、δ~(15)N-NO_3~-、δ~(15)N-NH_4~+的协同分析可知,湖区氮的赋存形态主要受湖区水体硝化作用及沉积物内反硝化作用的影响.     

宛山荡农田土壤氮迁移过程反硝化与厌氧氨氧化

为探究中国南方农田土壤氮迁移过程的反硝化与厌氧氨氧化(anaerobic ammonia oxidation,ANAMMOX)速率变化和脱氮贡献本研究采集宛山荡麦稻轮作区农田不同层深土壤及农田、沟道、河岸带和湖泊沉积物等不同土地利用类型土壤样品,分析其理化性质采用Illumina MiSeq测序和实时荧光定量PCR (quantitative real-time PCR,qPCR)技术探究土壤样品的微生物群落组成和功能基因丰度应用同位素培养实验测定各样品的潜在反硝化与厌氧氨氧化速率(以N_2计,下同).结果表明,土壤反硝化速率与TOC、NH_4~+-N和NO_3~--N含量均显著正相关(P0.05),与nirS、nirK及nosZ等功能基因丰度亦呈显著正相关(P 0.05).农田表层土壤反硝化速率为(11.51±1.04) nmol·(g·h)~(-1),显著高于农田其他土壤层以及其他土地利用类型(P 0.05),而农田土壤中厌氧氨氧化速率在20～30 cm层最高,达到(0.48±0.07) nmol·(g·h)~(-1).此外,反硝化作用是农田表层土壤氮损失的主要原因,占91.9%～99.7%,而厌氧氨氧化在深层土壤N_2的产生过程中占有重要地位.     

于桥水库沉积物-水界面氮磷剖面特征及交换通量

于桥水库是天津市重要的饮用水源地,但近年来呈现富营养化加重趋势,而其内源负荷及污染分布特征尚不清楚.本研究利用Peeper(pore water equilibrium)技术获取沉积物-水界面氮磷剖面特征,分析于桥水库间隙水氮磷分布的空间差异;采集沉积物无扰动柱样分析沉积物中易释放态氮及磷的赋存特征,并利用原柱样静态培养法对其水土界面氮磷交换速率进行估算.结果表明:(1)沉积物中活性磷、氨氮、硝态氮和亚硝态氮的含量分别为0.5~6.5、0.5~10.9、2.2~16.2和0.05~0.6 mg·kg~(-1),在垂直方向随深度增加营养盐含量降低,而在空间分布上差异显著.(2)上覆水中PO_4~(3-)-P和NH_4~+-N质量浓度较低,间隙水中PO_4~(3-)-P和NH_4~+-N质量浓度远大于上覆水,表明于桥水库间隙水具有向上覆水体扩散营养盐的潜力.在垂直方向上间隙水中PO_4~(3-)-P和NH_4~+-N具有在0~5 cm快速增加,之后表现出逐渐降低的趋势.(3)静态释放结果表明,PO_4~(3-)-P和NH_4~+-N从沉积物间隙水扩散至上覆水中,其释放通量分别为1.1~13.3 mg·(m~2·d)~(-1)和20.6~250.5 mg·(m~2·d)~(-1);NO-3-N交换通量在-20.4~33.4 mg·(m~2·d)~(-1)之间,NO_2~--N交换通量在-7.4~0.4 mg·(m~2·d)~(-1)之间.PO_4~(3-)-P和NH_4~+-N为于桥水库主要的沉积物内源向上覆水释放营养盐,总体释放速率在空间上呈现南高北低、淋河口和水坝前较高的释放特征.与类似研究比较可知,于桥水库沉积物-水界面通量相对较高,表明沉积物是于桥水库上覆水营养盐的重要来源.     

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.     

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.     

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.     

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

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