氢氧化镁对水体内源磷释放的控制作用

本研究首先通过批量实验考察了氢氧化镁对水中磷酸盐的吸附性能,再通过底泥模拟释放实验考察了氢氧化镁覆盖和添加控制底泥中磷向上覆水体释放的效果及机制.结果表明,氢氧化镁对水中磷酸盐具有良好的吸附能力,其投加量的增加有利于水中磷酸盐被其所吸附去除,与Langmuir模型相比,其对水中磷酸盐的等温吸附行为更适合采用Freundlich和Dubinin-Radushkevitch(D-R)模型加以描述.氢氧化镁覆盖可以有效地控制底泥中磷向上覆水体的释放,使得上覆水中SRP浓度处于较低的水平,即使覆盖层的结构完整性受到扰动破坏而导致覆盖材料与表层底泥的混合,氢氧化镁仍然可以有效地控制底泥中磷向上覆水体的释放.氢氧化镁覆盖和添加均可以有效地降低最上层(0～10 mm)底泥间隙水中SRP的浓度,这对于其覆盖和添加有效控制底泥中磷向上覆水体的释放是至关重要的.人工合成的氢氧化镁对水中磷酸盐的吸附性能优于商业购买的氢氧化镁,前者控制水体内源磷向上覆水体释放的效果也优于后者.以上结果显示,氢氧化镁是一种有希望用于控制水体底泥内源磷释放的活性覆盖和改良材料.     

镧改性净水污泥水热炭对水体中磷的吸附特性及底泥内源磷的固定

以净水污泥和氯化镧为原料,通过一步水热炭化同时负载镧,制备了镧改性净水污泥水热炭.采用SEM-EDS、 BET、 FTIR、 XRD和XPS对材料进行表征,考察溶液初始pH、吸附时间、吸附等温线和吸附动力学等,研究其对水体磷酸盐的吸附特性.结果表明,制备的材料相比净水污泥原泥,比表面积和孔容孔径有明显提高,磷吸附量大幅提升.吸附过程符合准二级动力学模型,Langmuir模型拟合对磷的最大吸附量达到72.69 mg·g^-1.主要吸附机制为静电引力和配体交换.镧改性净水污泥水热炭添加入底泥,可以有效控制底泥内源磷向上覆水的释放.分析底泥磷形态,水热炭的添加促使底泥中不稳定的NH₄Cl-P、 BD-P和Org-P向非常稳定的HCl-P转变,降低了底泥中潜在活性磷含量,同时也大幅降低了底泥中生物有效磷含量.说明镧改性净水污泥水热炭可以有效吸附去除水体磷酸盐,同时也可作为底泥改良材料,有效稳定底泥内源磷,控制水体磷含量.     

CaO2不同投加方式对黑臭河道底泥内源磷释放抑制作用

以S市某黑臭河道底泥和上覆水为研究材料,研究了CaO_2在3种不同投加方式下对内源磷释放的抑制效果.结果表明CaO_2在3种投加方式下,均导致上覆水中pH和DO有所增加.注射条件下,上覆水DO浓度明显低于覆盖,说明注射确实延缓了CaO_2的氧化速度,有利于创造底泥微氧化环境.CaO_2覆盖和注射条件下,上覆水中TP和DIP浓度以及变化趋势基本一致,均明显低于混匀条件.但是,覆盖条件下,间隙水中DIP浓度最高,达到注射条件下的120.33~142.18倍.相反,注射条件下,间隙水中DIP浓度最低,并且上覆水中DIP浓度也较低,说明注射条件下CaO_2对内源磷的释放确有抑制作用,这与其创造的微氧化环境密切相关.底泥中不同形态磷数量分布也证实了这一点.投加CaO_2加快了有机磷的矿化速度,铁铝结合态磷和钙结合态磷也明显增加,使得内源磷持留能力增强.     

扰动与钝化剂对水/沉积物系统中磷释放及磷形态的影响

考察了扰动与钝化剂对滇池重污染底泥的磷释放的影响.结果表明,钝化剂(PAM+聚铝)有显著的抑制沉积物的磷释放和捕捉上覆水中含磷颗粒的效果.加钝化剂后,上覆水的总磷(TP)、溶解性总磷(DTP)和溶解性无机磷(DIP)分别比未加钝化剂组低50.0%～89.8%,85.5%～97.9%和96.5%～100.0%.扰动促进了沉积物的磷释放,这是因为扰动导致泥水混合程度增加;扰动导致沉积物氧化还原状态的改变.5d后扰动组的磷开始释放,而未扰动组在第52d仍未释放.沉积物中释放的磷主要是磷酸盐.扰动促进了DIP的释放,扰动后DTP/TP、DIP/DTP及DIP/TP均增加.投加的铝盐的量在试验期间导致的上覆水中残余铝的含量在安全范围内.扰动对上覆水中残余铝的含量影响不大.     

易悬浮和外源输入下原位覆盖对生物有效磷形成的影响

在有外源磷持续汇入的前提下,研究了底泥原位覆盖钙改性材料和锁磷剂被悬浮颗粒再覆盖后对沉积物生物有效磷(BAP)的影响.结果表明,与空白对照相比,底泥原位覆盖后,BAP平均下降34.30%,此外,上覆水及间隙水溶解性无机磷(DIP)的浓度分别平均下降了74.25%和47.48%(0～3 cm),说明覆盖材料可以有效减少水体DIP的浓度,促进易被生物利用态磷浓度的降低.然而,当覆盖材料受到悬浮颗粒影响后,BAP平均下降20.27%,其中,藻类可利用磷(AAP)、碳酸氢钠可提取磷(Olsen-P)和水溶性磷(WSP)的含量较未被悬浮颗粒覆盖组显著提高,分别增加了18.28%、17.41%和12.58%,说明覆盖材料受悬浮颗粒影响后不利于降低底泥磷的生物有效性.     

灼烧净水污泥投加方式对磷吸附和磷形态的影响

以灼烧净水污泥为研究对象,探讨在其不同投加方式(混匀和覆盖)下,各底泥对外源磷的吸附效果以及间隙水和底泥中各形态磷的数量分布.结果表明,相比未灼烧净水污泥,灼烧净水污泥对磷的吸附能力显著改善,磷最大吸附量(Smax)提高了43.7%、底泥磷平衡浓度(EPC0)降低69.1%、磷饱和度(DPS)降低54.4%.混匀和覆盖对上覆水中磷消失的贡献率几乎一致,但明显高于对照实验.但如果考虑灼烧净水污泥与上覆水的接触几率,则混匀条件下,单位净水污泥对磷的吸附量为覆盖条件下的2.3倍.覆盖条件下,间隙水(1~2 cm)中溶解性磷酸盐浓度是混匀条件的33.17倍(平均值),这主要源于覆盖导致溶解氧渗透深度明显降低.混匀条件下,外源磷更易形成Ca-P,而覆盖条件下,易释放的NH_4Cl-P和Fe/Al-P占比更多,这暗示了混匀对底泥微环境的改造更有利于外源磷的吸附和内源磷的持留.     

过氧化钙复合片剂对水体修复和底泥磷控制的作用

以受污染水体及底泥为研究对象,制备了2种过氧化钙复合片剂(CPCTs),并考察了在混合投加方式下对上覆水的影响及控磷效果.复合片剂由过氧化钙(CaO₂)、灼烧净水污泥、羟丙基甲基纤维素(HPMC)等粉末直压制成,其中B片剂含硫酸亚铁(FeSO₄),A不含. 2种片剂吸附效果均较好地符合Langmuir和Freundlich等温模型,对磷的理论最大吸附量分别达110.908 mg·g^-1和106.390 mg·g^-1.底泥模拟实验结果表明,与对照组相比,A、B组上覆水pH提高,Chl-a浓度降低(42.75%和60.82%),DO浓度提高(53.73%和63.30%). A、B组上覆水DIP浓度变化均显著,分别降低了54.93%和25.11%.对于底泥间隙水DIP, A、B组Ⅰ层(0～2 cm)变化均显著,分别降低了74.81%和65.66%;B组Ⅱ层(2～4 cm)变化显著,平均浓度降低了46.23%,而A组Ⅱ层变化不显著;A、B组Ⅲ层(4～6 cm)变化不显著.对于底泥形态磷,A、B组NH     

锆改性高岭土覆盖对底泥与上覆水之间磷迁移转化的影响

以无覆盖和高岭土覆盖作为对照,通过底泥磷释放控制模拟实验考察了厌氧条件下锆改性高岭土覆盖对重污染河道底泥与上覆水之间磷迁移转化的影响.结果表明,厌氧条件下,重污染河道底泥会释放出大量的磷进入上覆水中,且所释放出来的磷主要以溶解性磷酸盐为主.高岭土覆盖可以略微降低底泥磷向上覆水迁移的通量,而锆改性高岭土覆盖则可以极大降低底泥磷向上覆水迁移的通量.被高岭土覆盖层所吸附的磷中29%以氧化还原敏感态磷(BD-P)形式存在和63%以残渣态磷(Res-P)形式存在.被锆改性高岭土覆盖层所吸附的磷中绝大部分(90%)以金属氧化物结合态磷(NaOH-P)和Res-P形式存在,厌氧状态下很难被重新释放出来进入上覆水体.与无覆盖相比,厌氧条件下锆改性高岭土覆盖不仅不会促进底泥BD-P的释放,而且还会促进底泥NaOH-P的形成.X射线光电子能谱(XPS)和固相31P核磁共振(NMR)技术分析证实了锆改性高岭土覆盖层吸附水中磷酸盐的主要机制为配位体交换和形成内配合物.上述结果说明锆改性高岭土适合作为一种活性覆盖材料控制重污染河道底泥磷的释放.     

生物炭覆盖对底泥污染物释放的影响

为研究生物炭对底泥污染物释放的影响,将芦竹茎、芦苇茎、花生壳及玉米芯利用限氧升温炭化法烧制成生物炭(Biochar),在模拟反应器中覆盖在受污染底泥上,研究生物炭对上覆水NH4+-N、NO3--N、NO2--N、COD及PO34--P浓度的影响,并计算各指标累积释放量及释放速率;同时测定了生物炭可溶性NH4+-N和PO34--P的释放量.结果表明,未覆盖生物炭的对照组上覆水氨氮浓度在第25 d达到最大值4.27 mg·L-1,之后稳定在4.02 mg·L-1左右,而4种生物炭处理组在第25 d以后,氨氮浓度稳定在0.3 mg·L-1以下,其中芦苇处理组抑制效果最明显,氨氮累积释放量减少了85.61%;4种生物炭组COD累积释放量较未添加生物炭处理组减少了28.83%～30%;玉米芯生物炭处理组磷酸盐浓度高于对照组,芦竹及花生壳处理组对底泥磷的释放抑制效果较好.生物炭NH4+-N和PO34--P的释放量在前3 d最大,花生壳生物炭组氨氮释放量最大,为36.79mg·kg-1,玉米芯生物炭处理组磷酸盐释放量最大,为70.64 mg·kg-1.结果表明生物炭对底泥NH4+-N、COD及PO34--P的释放有削减作用,具有应用到污染水体底泥修复的潜力.     

锆改性高岭土原位改良技术控制重污染河道底泥磷释放效果

采用锆对高岭土进行改性,通过批量吸附实验考察了锆改性高岭土对水中磷酸盐的吸附性能,并通过底泥培养实验考察了锆改性高岭土原位改良技术对底泥磷释放的控制效果.结果表明,锆改性高岭土对水中磷酸盐的吸附能力随改性所用锆投加量的增加而增加.在制备锆改性高岭土过程中,溶液沉淀p H值由8增加到10时,锆改性高岭土对水中磷酸盐的吸附能力增加;沉淀p H值由10增加到11时,锆改性高岭土对磷的吸附能力基本不变;沉淀p H值由11增加到12时,锆改性高岭土的吸磷能力则下降.沉淀p H值为10时制备得到的锆改性高岭土对水中磷酸盐的吸附平衡数据可以采用Langmuir模型加以描述.大部分被锆改性高岭土中锆所吸附的磷酸盐(84%左右)主要以Na OH提取态磷(Na OH-P)和残渣态磷(Res-P)形态存在,低溶解氧情况下不容易被重新释放出来,同时重污染河道底泥会释放出大量的溶解性磷酸盐进入上覆水体;向重污染河道底泥中添加锆改性高岭土可以极大地削减底泥中磷向上覆水体迁移的通量.采用锆改性高岭土对底泥进行改良不仅增强了底泥对水中磷的吸附能力,而且降低了底泥的磷吸附-解吸平衡浓度(EPC0).因此,应用锆改性高岭土作为底泥改良剂可以有效控制重污染河道底泥磷释放.     

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.     

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.     

Effects of two sludge application on fractionation and phytotoxicity of zinc and copper in the soil

The potential harm of heavy metals is a primary concern in application of sludge to the agricultural land. A pot experiment was conducted to evaluate the effect of two sludges on fractionation of Zn and Cu in soil and their phytotoxicity to pakchoi. The loamy soil was mixed with 0%, 20%, 40%, 60% and 80% (by weight) of digested sewage sludge (SS) and composted sludge (SC). The additions of both sludges caused a significant raise in all fractions, resulting in that exchangeable (EXCH) and organic bound (OM) became predominance of Zn and organic bound Cu occupied the largest portion. There was more available amount of Zn and Cu in SS treatments than SC treatments. During the pot experiment, the concentration of Zn in EXCH, carbonate (CAR) and OM and Cu in EXCH and OM fractions decreased in all treatments, so their bioavailability reduced. Germination rate and plant biomass decreased when the addition rate was high and the best yield appeared in 20% mixtures at the harvest of pakchoi. The two sludges increased tissue contents of Zn and Cu especially in the SS treatments. Zn in pakchoi was not only in relationship to ΔEXCH and ΔCAR forms but also in ΔOM forms in the sludge-soil mixtures. Tissue content of Cu in pakchoi grown on SC-soils could not be predicted by ΔEXCH. These correlation rates between Zn and Cu accumulation in pakchoi and variation of different fractions increased with time, which might indicate that sludges represented stronger impacts on the plant in long-term land application.     

Intraspecific differences in effects of co-contamination of cadmium and

A hydroponic experiment was carried out to study intraspecific differences in the effects of different concentrations of cadmium (Cd)(0-10 mg/L) and arsenate (As(V)) (0-8 mg/L) on the growth parameters and accumulation of Cd and As in six wheat varieties Jing-9428, Duokang-1, Jingdong-11, Jing-411, Jingdong-8 and Zhongmai-8. The endpoints of wheat seedlings, including seed germination,biomass, root length and shoot height, decreased with increasing the Cd and As concentrations. Significant differences in seed germination, biomass, root length, shoot height and the accumulation of Cd and As were observed between the treatments and among the varieties (p ＜ 0.05). The lethal dosage 50% were about 20, 80, 60, 60, 80 and 20 mg As/L for Jing-9428, Duokang-1, Jingdong-11,Jing-411, Jingdong-8 and Zhongmai-8, respectively, and the corresponding values for Cd were about 30, 80, 20, 40, 60 and 10 mg Cd/L, respectively. Among the six varieties, Duokang-1 was found to be the most resistant to Cd and As toxicity, and Zhongmai-8 was the most sensitive to Cd and As co-contamination. The resistance of the six varieties was found dependant on the seedling uptake of Cd and As. Duokang-1 was the most suitable for cultivation in Cd and As co-contaminated soils.     

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

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Isolation and preliminary characterization of a 3-chlorobenzoate degrading bacteria

A study was conducted to compare the diversity of 2-, 3-, and 4-chlorobenzoate degraders in two pristine soils and one contaminated sewage sludge. These samples contained strikingly different populations of mono-chlorobenzoate degraders. Although fewer cultures were isolated in the uncontaminated soils than contaminated one, the ability of microbial populations to mineralize chlorobenzoate was widespread. The 3- and 4-chlorobenzoate degraders were more diverse than the 2-chlorobenzoate degraders. One of the strains isolated from the sewage sludge was obtained. Based on its phenotype, chemotaxonomic properties and 16S rRNA gene, the organism S-7 was classified as Rhodococcus erythropolis. The strain can grow at temperature from 4 to 37℃. It can utilize several （halo）aromatic compounds. Moreover, strain S-7 can grow and use 3-chlorobenzoate as sole carbon source in a temperatures range of 10-30℃ with stoichiometric release of chloride ions. The psychrotolerant ability was significant for bioremediation in low temperature regions. Catechol and chlorocatechol 1,2-dioxygenase activities were present in cell free extracts of the strain, but no （chloro）catechol 2,3- dioxygenase activities was detected. Spectral conversion assays with extracts from R. erythropolis S-7 showed accumulation of a compound with a similar UV spectrum as chloro-cis,cis-muconate from 3-chlorobenzoate. On the basis of these results, we proposed that S-7 degraded 3-chlorobenzoate through the modified ortho-cleave pathway.     

Single and joint effects of pesticides and mercury on soil urease

The influence of two pesticides including chlorimuron-ethyl and furadan and mercury （Hg） on urease activity in 4 soils （meadow burozem and phaeozem） was investigated. The soils were exposed to various concentrations of the two pesticides and Hg individually and simultaneously. Results showed that there was a close relationship between urease activity and organic matter content in soil. Chlorimuron-ethyl and furadan could both activate urease in the 4 soils. The maximum increment of urease activity by chlorimuronethyl was up to 14%-18%. There was almost an equal increase （up to 13%-21%） in the urease activity by furadan. On the contrary, Hg markedly inhibited soil urease activity. A logarithmic equation was used to describe the relationship （P〈0.05） between the concentration of Hg and the activity of soil urease in the 4 tested soils. Semi-effect dose （ED50） values by the stress of Hg based on the inhibition of soil urease in the 4 soils were 88, 5.5, 24 and 20 mg/kg, respectively, according to the calculation of the corresponding equations. The interactive effect of chlorimuron-ethyl or furadan with metal Hg on soil urease was mainly synergic at the highest tested concentrations.