Microbial community dynamics in uranium contaminated subsurface sediments under biostimulated conditions with high nitrate and nickel pressure

BACKGROUND, AIM, AND SCOPE: The subsurface at the Oak Ridge Field Research Center represents an extreme and diverse geochemical environment that places different stresses on the endogenous microbial communities, including low pH, elevated nitrate concentrations, and the occurrence of heavy metals and radionuclides, including hexavalent uranium [U(VI)]. The in situ immobilization of U(VI) in the aquifer can be achieved through microbial reduction to relatively insoluble U(IV). However, a high redox potential due to the presence of nitrate and the toxicity of heavy metals will impede this process. Our aim is to test biostimulation of the endogenous microbial communities to improve nitrate reduction and subsequent U(VI) reduction under conditions of elevated heavy metals. MATERIALS AND METHODS: Column experiments were used to test the possibility of using biostimulation via the addition of ethanol as a carbon source to improve nitrate reduction in the presence of elevated aqueous nickel. We subsequently analyzed the composition of the microbial communities that became established and their potential for U(VI) reduction and its in situ immobilization. RESULTS: Phylogenetic analysis revealed that the microbial population changed from heavy metal sensitive members of the actinobacteria, alpha- and gamma-proteobacteria to a community dominated by heavy metal resistant (nickel, cadmium, zinc, and cobalt resistant), nitrate reducing beta- and gamma-proteobacteria, and sulfate reducing Clostridiaceae. Coincidentally, synchrotron X-ray absorption spectroscopy analyses indicated that the resulting redox conditions favored U(VI) reduction transformation to insoluble U(IV) species associated with soil minerals and biomass. DISCUSSION: This study shows that the necessary genetic information to adapt to the implemented nickel stress resides in the endogenous microbial population present at the Oak Ridge FRC site, which changed from a community generally found under oligotrophic conditions to a community able to withstand the stress imposed by heavy metals, while efficiently reducing nitrate as electron donor. Once nitrate was reduced efficient reduction and in situ immobilization of uranium was observed. CONCLUSIONS: This study provides evidence that stimulating the metabolism of the endogenous bacterial population at the Oak Ridge FRC site by adding ethanol, a suitable carbon source, results in efficient nitrate reduction under conditions of elevated nickel, and a decrease of the redox potential such that sulfate and iron reducing bacteria are able to thrive and create conditions favorable for the reduction and in situ immobilization of uranium. Since we have found that the remediation potential resides within the endogenous microbial community, we believe it will be feasible to conduct field tests. RECOMMENDATIONS AND PERSPECTIVES: Biostimulation of endogenous bacteria provides an efficient tool for the successful in situ remediation of mixed-waste sites, particularly those co-contaminated with heavy metals, nitrate and radionuclides, as found in the United States and other countries as environmental legacies of the nuclear age.     

生物电催化方法处理三氯乙酸的研究

利用吸附法将血红蛋白(Hb)固定在碳纳米管修饰电极表面,研究了Hb在碳纳米管修饰电极的直接电化学行为.固载Hb碳纳米管修饰电极在pH=7.0的PBS缓冲溶液中于-0.300V(vsSCE)处有一对相当可逆的循环伏安还原氧化峰,为Hb血红素辅基Fe(Ⅲ)/Fe(Ⅱ)电对的特征峰.利用循环伏安法和恒电位电解法研究了固载Hb的碳纳米管修饰电极对有机氯模型污染物三氯乙酸的电催化还原脱氯,并通过鉴定中间产物探讨了其催化还原机理.结果表明,固载Hb的碳纳米管修饰电极对三氯乙酸的还原具有很高的催化活性,三氯乙酸是按照三氯乙酸→二氯乙酸→一氯乙酸→乙酸的途径分布还原脱氯.将固载Hb的碳纳米管修饰电极组装成三维填充床电解反应器,进行了三氯乙酸连续流动电解还原的初步研究.-0.6V(vs.SCE)电解180min,三氯乙酸去除率为40.13%.     

磷化氢液相催化氧化净化催化剂的初筛

传统的净化方法难以实现低成本、高效、选择性净化低浓度磷化氢尾气,这限制了含磷化氢尾气的资源化技术的实现。通过Pd(Ⅱ)、Fe(Ⅲ)、Cu(Ⅱ)、Pd(Ⅱ)-Cu(Ⅱ)、Pd(Ⅱ)-Fe(Ⅲ)对低浓度磷化氢连续净化的研究,筛选出在低温(<80℃)、常压下对低浓度磷化氢(850mg/m3)具有液相催化氧化净化活性的Pd(Ⅱ)、Pd(Ⅱ)-Cu(Ⅱ)、Pd(Ⅱ)-Fe(Ⅲ)3种催化剂,其中Pd(Ⅱ)催化氧化净化低浓度磷化氢的净化效率>60%,Pd(Ⅱ)-Cu(Ⅱ)及Pd(Ⅱ)-Fe(Ⅲ)催化氧化低浓度磷化氢(850mg/m3)的净化效率可达100%。     

芳烃燃烧钯催化剂的研究--载体、制备方法对催化活性的影响

以苯蒸气作为催化燃烧气，研究了３ 种不同载体和３ 种不同制备方法对金属负载型钯催化剂芳烃催化燃烧性能的影响，并用ＳＥＭ 对催化剂的表现形貌进行了分析．结果表明，载体及催化剂制备方法不同，催化剂的活性及耐热性不同．经一定的高温预处理后的含有稀土的ＦｅＣｒＡｌ 合金作载体性能较另两种载体优良；并提出了该催化剂较好的制备方法．     

负载型铜酞菁的制备及其催化氧化巯基乙醇

以3-(环己氧基)-邻苯二腈和氯化铜为原料,通过钼酸铵固相法合成了一种烷氧基取代的铜酞菁配合物α-四(环己氧基)铜酞菁(CuPc),采用浸渍法将其负载在MCM-41和SBA-15介孔分子筛中,制备了CuPc/MCM-41和CuPc/SBA-15催化剂,并且负载后的酞菁还能回收利用,仍然具有催化效果。采用紫外-可见吸收光谱(UV-vis)、红外光谱(IR)对目标产物进行表征,并用TG对酞菁进行热稳定性分析,结果表明酞菁在200℃时开始失重,350℃时失重率最大为58%;通过氮气吸附对催化剂进行表征,证明酞菁已经进入到分子筛孔道,孔容积分别从0.132 cm3/g减至0.055 cm3/g和0.420 cm3/g减至0.202 cm3/g。研究了2种催化剂在不同pH、催化剂浓度下对巯基乙醇(ME)催化氧化性能的影响,结果表明,CuPc/SBA-15对巯基乙醇(ME)具有较高的催化活性,且2种催化剂的活性在pH=12时都达到最大。     

催化湿式氧化法处理高浓度有机废水的动力学模型

在２７０℃、８．８ＭＰａ条件下用催化湿式氧化法试验处理高浓度工业有机废水,反应时间１０￣１５ｍｉｎ时,废水中ＴＯＣ浓度可由１７９００ｍｇ／Ｌ降至１００ｍｇ／Ｌ以下。针对这一多相催化氧化反应过程,以ＴＯＣ为目标污染和,研究建立了涉及液、气、固三相的反应动力学模型。反应时间、瓜器ＴＯＣ浓度、反应压力和反应温度等主要因素对反应器净化ＴＯＣ性能影响的试验表明,该模型计算值与实验值有很好的相关性（相关系数Ｒ     

Mn-Co/蜂窝陶瓷催化剂制备及催化臭氧化对苯二酚效能

为了提高金属催化剂的活性和使用寿命,以硝酸钴Co(NO3)2·6H2O和硝酸锰Mn(NO3)2作为前驱体,蜂窝陶瓷(ceramic honeycomb,CH)作为载体,采用涂覆法制备了4种不同质量比的Mn-Co/CH催化剂,通过XRD、N2-吸附/脱附、FESEM和XPS等方法分析了催化剂的结构,研究了催化剂的材料力学性能,建立了单独臭氧和催化臭氧化对苯二酚的反应动力学模型,考察了催化剂催化臭氧化的效能.结果表明,Mn1Co1/CH(Mn∶Co=1∶1)催化剂的晶相主要以Mn3O4和Co O为主,具有较大的比表面积、孔容和孔径,分别达到190 m~2·g~(-1)、0.25 cm3·g-1和4.8 nm;Mn1Co1/CH催化剂的催化活性最高,对苯二酚和COD的去除率分别达到78%和54%.Mn-Co/CH催化剂的抗压缩强度大(15.89~16.94 MPa).当添加叔丁醇时,对苯二酚去除率显著下降,·OH在Mn1Co1/CH催化臭氧化过程中起着重要的作用,催化臭氧化对苯二酚符合一级反应动力学模型.Mn-Co/CH催化剂用量少、催化效率高、使用寿命长,易于实现工业化.     

Effects of Ce on catalytic combustion of methane over Pd-Pt/Al2O3 catalyst

Activity and stability of 1%Pd-0.2%Pt/Al₂O₃ and 1%Pd-0.2%Pt/0.6%Ce/Al₂O₃ catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction were characterized by BET, CO chemisorption, XRD and XPS techniques. Results showed that the presence of Ce significantly increased the activity and thermal stability of the Pd-Pt/Al₂O₃ catalyst towards methane combustion, which could be attributed to more highly-dispersed active PdO particles over the Pd-Pt/Ce/Al₂O₃ catalyst surface as well as the retarded sintering of PdO and the maintained oxidized state of surface Pd during the combustion process in the presence of Ce.     

金属催化剂对油漆板材催化热解产物的影响

研究使用CaCO3、CaO、Fe2O3、还原铁粉、Na2CO35种金属催化剂对油漆板材进行热解,收集固、液两相产物进行产率计算和检测分析.结果表明,5种催化剂都有效提高了热解固相产物的产率,CaCO3、Na2CO3以及还原铁粉可以增加液相产品产率.钛元素在所有催化热解固相产物含量均较高,可能造成潜在的环境污染.热解液相...     

钯/泡沫镍对水体中4-氯酚的氢解脱氯研究

采用置换沉积法制备泡沫镍负载钯(Pd/Ni)催化剂,研究了其在H2作为供氢体时对水相中4-氯酚(4-CP)的催化氢解脱氯作用.考察了Pd负载量、H2流量和反应液pH值对4-CP转化率的影响.结果表明,在相对较低的Pd负载量和H2流量下即可实现4-CP的快速高效去除,且反应液pH值在3.04~10.97的范围对反应影响不显著.当Pd负载量为0.1%、H2流量为10mL/min、pH值为6.80时,反应1h,4-CP转化率达92.6%.Pd/Ni具有较高的稳定性,重复实验表明,该催化剂使用3次后,催化活性仅下降了2.0%.