产气肠杆菌燃料电池产电机制研究

基于铁还原菌的微生物燃料电池（MFCs）与基于产氢细菌的MFCs各有优劣,前者能量利用效率高,但底物利用范围有限;后者底物利用广泛,但其依靠悬浮细胞产电,电子回收率较低.本研究以1株具有铁还原活性的产氢菌Enterobacter aerogenes XM02为产电微生物,构建了3种不同阳极材料的空气阴极MFCs,通过输出电压和库仑效率的比较以及扫描电镜观察阳极形貌等方法对此菌的产电机制进行探讨.结果发现,采用比表面积大且具有氢催化活性的碳毡作为阳极材料时,可显著改善MFCs性能,库仑效率由载铂碳纸阳极MFC的1.68% 提高至42.49%,远高于已报道的其它产氢菌燃料电池.扫描电镜证实大量细菌细胞附着在阳极表面,形成阳极生物膜.采用非生长基质实验排除悬浮细胞的产电作用,证明附着在阳极的生物膜对产电起主导作用,认为生物膜原位产氢-氧化是此菌的主要产电机制.     

外加酶强化剩余污泥微生物燃料电池产电特性的研究

以剩余污泥作为接种液和基质,探讨了外加酶(中性蛋白酶、α-淀粉酶)强化单室型剩余污泥微生物燃料电池产电效率的可行性,研究了酶投加量对微生物燃料电池的产电特性及剩余污泥减量的影响.结果表明,在相同条件下,实验组产生的最大功率密度远远高于对照组;当酶的总投加量为10 mg.g-1时,最大输出功率密度及污泥水解效率达到最大,即中性蛋白酶组的最大功率密度、库仑效率、TCOD去除率、TSS去除率、VSS去除率分别为507 mW.m-2、3.98%、88.31%、83.18%、89.03%,而α-淀粉酶组则分别为700 mW.m-2、5.11%、94.09%、98.02%、98.80%.本实验采用向剩余污泥中投加酶的方法,成功增强了微生物燃料电池的产电效率,同时对剩余污泥有效地进行了处理,为微生物燃料电池的实际应用提供了新途径.     

阳极内添加阳离子交换树脂提升辊压“三合一”膜电极MFC性能

阳极-隔膜-阴极的"三合一"膜电极结构能够最大程度减小阴阳极间距,提高微生物燃料电池(microbial fuel cell,MFC)的输出功率.为进一步提高MFC性能,本研究使用非贵金属材料构建了辊压"三合一"膜电极系统,其欧姆内阻降低至3~5Ω.以乙酸钠为底物,MFC的最高功率密度达到446 m W·m-2.向阳极内添加固体小球(如聚苯乙烯球和玻璃微球)可在辊压过程中增加阳极表面和内部的大孔,强化电解液向阴极的传递从而使MFC的功率密度提升10%.添加阳离子交换树脂能够进一步强化阳极内部的质子传递,提高阴极电位,从而将功率密度提升至543 m W·m-2.此外,阳极内添加阳离子交换树脂还可提高电池运行的稳定性和库仑效率.     

石油污染物对海底微生物燃料电池性能的影响及加速降解效应

海底石油污染物在缺氧环境下导致其生物降解过程缓慢,对海洋环境造成长期危害.本文利用海底微生物燃料电池(BMFCs)原理,尝试通过电催化作用提高海底石油污染物的降解速率.对比测试了含油电池装置(BMFCs-A)与无油电池装置(BMFCs-B)的电化学性能,研究了石油污染物对电池性能的影响;比较了含油通路(BMFCs-A)和断路状态下(BMFCs-C)的石油降解率和细菌聚集量,分析了BMFCs对石油污染物降解的加速作用.结果表明,BMFCs-A和BMFCs-B阳极的交换电流密度分别为1.37×10-2A·m-2和1.50×10-3A·m-2,最大输出功率密度分别是105.79 m W·m-2和83.60 m W·m-2,BMFCs-A装置的抗极化能力增强,交换电流密度提高近9倍,最大输出功率密度提高1.27倍.BMFCs-A和BMFCs-C阳极表面的异养菌数量分别是(66±3.61)×107CFU·g-1和(7.3±2.08)×107CFU·g-1,细菌数量增加了8倍,高的异养菌数量导致石油降解加速进行,BMFCs的石油降解率是自然条件下的18.7倍.BMFCs在电化学性能提高的同时,加速石油污染物的降解.本文同时提出了一种海底微生物燃料电池对石油污染物加速降解的新模式.     

On the effect of Fe(III) on proliferation of Microcystis aeruginosa at high nitrate and low chlorophyll condition

The impact of Fe concentrations on the growth of Microcystisaeruginosa in aquatic systems under high nitrate and low chlorophyll conditions was studied. The responses of cell density, total and cell chlorophyll-a intracellular Fe content and organic elemental composition of M. aeruginosa to different concentration gradients of Fe(III) in the solutions were analysed. The results showed that the proliferation speeds of M. aeruginosa were: (1) decelerated when the Fe(III) concentration was lower than 50 μg/L in the solutions, (2) promoted and positively related to the increase of Fe(III) concentration from 100 to 500 μg/L in the solutions over the experimental period, and (3) promoted in the early stage but decelerated in later stages by excess adsorption of Fe by cells when the Fe(III) concentration was higher than 500 μg/L in the solutions. The maximum cell density, total and cell chlorophyll-a were all observed at 500 μg Fe(III)/L concentration. The organic elemental composition of M. aeruginosa was also affected by the concentration of Fe(III) in the solutions, and the molecular formula of M. aeruginosa should be expressed as C_7–7.5H₁₄O_0.8–1.3N_3.5–5 according to the functions for different Fe(III) concentrations. Cell carbon and oxygen content appeared to increase slightly, while cell nitrogen content appeared to decrease as Fe(III) concentrations increased from 100 to 500 μg/L in the solutions. This was attributed to the competition of photosynthesis and nitrogen adsorption under varying cell Fe content.     

微生物燃料电池改性阳极处理PTA废水

探讨了不同改性阳极对微生物燃料电池(microbial fuel cell,MFC)产电性能及其对MFC处理难降解废水能力的影响.以单室空气阴极为基础,利用0.1 g电气石、质量分数75%二氧化锰/埃洛石纳米管(manganese bioxide/halloysite nanotube,MnO_2/HNT)和多壁碳纳米管-羧基(multi-walled carbon nanotube-carboxyl,MWCNT-COOH)对MFC阳极进行修饰.结果表明,不同改性阳极的MFC对含精对苯二甲酸(purified terephthalic acid,PTA)废水的去除率均高于70%,且化学需氧量(chemical oxygen demand,COD)去除率在79%以上.相较于其他几种改性阳极,以MWCNT-COOH改性材料作阳极的MFC产生的最大输出电压最高,获得的最大功率密度最高,分别为529 mV和252.73 mW·m~(-2).     

Impact of disinfection on drinking water biofilm bacterial community

Disinfectants are commonly applied to control the growth of microorganisms in drinking water distribution systems. However, the effect of disinfection on drinking water microbial community remains poorly understood. The present study investigated the impacts of different disinfectants (chlorine and chloramine) and dosages on biofilm bacterial community in bench-scale pipe section reactors. Illumina MiSeq sequencing illustrated that disinfection strategy could affect both bacterial diversity and community structure of drinking water biofilm. Proteobacteria tended to predominate in chloraminated drinking water biofilms, while Firmicutes in chlorinated and unchlorinated biofilms. The major proteobacterial groups were influenced by both disinfectant type and dosage. In addition, chloramination had a more profound impact on bacterial community than chlorination.     

铜离子对双室微生物燃料电池电能输出的影响研究

通过分别或同时向阳极室和阴极室添加Cu2+,借助铜在体系中的分布解析,研究了Cu2+对体系内阻及其分布、电能输出、库仑效率等的影响,以期为微生物燃料电池(microbial fuel cell,MFC)处理含铜废水的相关研究提供有益参考.结果表明,阳极添加10 mg·L-1的Cu2+会增大体系阳极反应的活化内阻及总体表观内阻,降低体系的电能输出和库仑效率,而阴极添加500 mg·L-1的Cu2+可显著降低阴极反应的活化内阻及总体表观内阻,提高体系产电效率.铜在体系中分布的研究表明,阳极室Cu2+不会向阴极室迁移扩散;当阴极添加Cu2+时,大部分被还原沉淀,另一部分因浓度梯度透过质子交换膜(proton exchange membrane,PEM)迁移扩散至阳极室(2.8%),影响产电微生物活性及系统的电能输出,仅有少部分Cu2+残留于阴极上清液中.     

生物强化膜生物反应器(MBR)处理邻苯二甲酸二乙酯(DEP)效果及微生物群落结构分析

为强化邻苯二甲酸二乙酯(DEP)降解,将从活性污泥中分离的高效DEP降解菌Arthrobacter sp.LMS13运用到MBR反应器,考察强化系统对DEP去除效果,并通过实时荧光定量(q-PCR)和Illumina Mi Seq技术分别对系统运行期间邻苯二甲酸双加氧酶降解基因(phtA)数量以及微生物群落结构特征进行了分析.结果表明,强化系统能加快反应器启动,对进水浓度为800 mg·L-1的DEP,强化系统和未经强化系统在运行后期(61 d)对DEP平均去除率分别为81%和19%.q-PCR结果显示,在驯化阶段,phtA基因拷贝数上升,但当DEP浓度大于400 mg·L-1时,phtA基因数量下降;phtA基因拷贝数与DEP降解率呈正相关.Mi Seq测序结果进一步表明,高浓度DEP导致系统中群落多样性指数下降,但对强化系统多样性影响相对较小.反应器运行过程中,原活性污泥中占有较高比例的拟杆菌门(Bateroidetes)和厚壁菌门(Firmicutes)丰度降低,ε-变形纲(ε-Proteobacteria)、绿弯菌门(Chloroflexi)在反应系统中逐渐被淘汰,而β-变形纲(β-Proteobacteria)和放线菌门(Actinobacteria)成为系统中的优势菌门,其中红环菌属(Rhodocyclus)、博得氏杆菌属(Bordetella)、节杆菌属(Arthrobacter)为优势菌属,在DEP降解系统中起着主要作用,是保证DEP生物处理效果和维持反应器稳定运行的重要菌属.     

Bioreduction of vanadium (V) in groundwater by autohydrogentrophic bacteria: Mechanisms and microorganisms

As one of the transition metals, vanadium(V)(V(V)) in trace amounts represents an essential element for normal cell growth, but becomes toxic when its concentration is above 1 mg/L. V(V) can alter cellular differentiation, gene expression, and other biochemical and metabolic phenomena. A feasible method to detoxify V(V) is to reduce it to V(IV), which precipitates and can be readily removed from the water. The bioreduction of V(V) in a contaminated groundwater was investigated using autohydrogentrophic bacteria and hydrogen gas as the electron donor. Compared with the previous organic donors,H2 shows the advantages as an ideal electron donor, including nontoxicity and less production of excess biomass. V(V) was 95.5% removed by biochemical reduction when autohydrogentrophic bacteria and hydrogen were both present, and the reduced V(IV)precipitated, leading to total-V removal. Reduction kinetics could be described by a first-order model and were sensitive to p H and temperature, with the optimum ranges of p H 7.5–8.0 and 35–40°C, respectively. Phylogenetic analysis by clone library showed that the dominant species in the experiments with V(V) bioreduction belonged to theβ-Proteobacteria. Previously known V(V)-reducing species were absent, suggesting that V(V)reduction was carried out by novel species. Their selective enrichment during V(V)bioreduction suggests that Rhodocyclus, a denitrifying bacterium, and Clostridium, a fermenter known to carry out metal reduction, were responsible for V(V) bioreduction.     

Bioreduction of vanadium (V) in groundwater by autohydrogentrophic bacteria: Mechanisms and microorganisms

As one of the transition metals, vanadium (V) (V(V)) in trace amounts represents an essential element for normal cell growth, but becomes toxic when its concentration is above 1 mg/L. V(V) can alter cellular differentiation, gene expression, and other biochemical and metabolic phenomena. A feasible method to detoxify V(V) is to reduce it to V(IV), which precipitates and can be readily removed from the water. The bioreduction of V(V) in a contaminated groundwater was investigated using autohydrogentrophic bacteria and hydrogen gas as the electron donor. Compared with the previous organic donors, H₂ shows the advantages as an ideal electron donor, including nontoxicity and less production of excess biomass. V(V) was 95.5% removed by biochemical reduction when autohydrogentrophic bacteria and hydrogen were both present, and the reduced V(IV) precipitated, leading to total-V removal. Reduction kinetics could be described by a first-order model and were sensitive to pH and temperature, with the optimum ranges of pH 7.5–8.0 and 35–40°C, respectively. Phylogenetic analysis by clone library showed that the dominant species in the experiments with V(V) bioreduction belonged to the β-Proteobacteria. Previously known V(V)-reducing species were absent, suggesting that V(V) reduction was carried out by novel species. Their selective enrichment during V(V) bioreduction suggests that Rhodocyclus, a denitrifying bacterium, and Clostridium, a fermenter known to carry out metal reduction, were responsible for V(V) bioreduction.     

高温堆肥过程对猪粪来源抗生素抗性基因的影响

为研究大规模好氧高温堆肥过程对猪粪来源抗生素抗性基因的影响,采用荧光定量PCR法检测了4个大环内酯类抗性基因(erythromycin resistance methylase,erm A、erm B、erm C和erm F)、3个β-内酰胺抗性基因(beta-lactamase,bla TEM、bla CTX和bla SHV)和2个喹诺酮类抗性基因(quinolone resistance,qnr A和qnr S)在堆肥过程中的变化趋势.结果表明,堆肥初期大环内酯类抗性基因含量显著高于β-内酰胺类和喹诺酮类抗性基因(P0.01),其中erm B基因丰度最高为9.88×10~8copies·g~(-1),其次是erm F为9.40×10~8copies·g~(-1).在高温堆肥结束时β-内酰胺抗性基因和喹诺酮类抗性基因丰度维持在较低水平,而大环内酯类抗性基因在堆肥结束后仍然具有较高含量.其中,erm F基因与堆肥初期相比甚至出现了增加的情况,这表明高温堆肥过程不能有效去除所有抗生素抗性基因.对于某些抗生素抗性基因,堆肥可能还是良好的生物反应器而导致抗性基因的增殖,农田中堆肥产品的施用有可能会造成抗生素抗性基因的传递.     

酸性含硒含镉废水低温生物强化处理技术研究

本研究将枯草芽孢杆菌接种于活性污泥中,系统考察了酸性含硒含镉废水的低温生物强化处理效果.研究发现,活性污泥联合枯草芽孢杆菌对硒、镉的去除效率(Se:94.9%,Cd:99.1%)高于单一枯草芽孢杆菌(B菌)、混合枯草芽孢杆菌及活性污泥.影响因素试验结果表明,在20℃、pH 4.0、甲醇为碳源时生物强化硒、镉去除效率较高.利用SBR反应器处理酸性(pH 4.0)含硒(3.7～10.0 mg·L~(-1))含镉(5.0～11.2 mg·L~(-1))废水,在低温(8.0～10.8℃)条件下运行80个周期,硒、镉和COD的平均去除率分别为97.4%、90.7%和95.0%.红外光谱分析表明,酰胺基、芳香族C—H伸缩健在硒、镉去除中起到主要作用.透射电镜与能谱分析证实了生物强化污泥对硒、镉去除之后形成纳米颗粒物.通过高通量测序分析微生物群落结构,发现生物强化污泥中富集了Pseudomonas(假单胞菌属)、Dechloromonas(脱氯单胞菌)等典型硒还原菌.     

利用氧化亚氮还原酶基因 (nosZ) 评价人工湿地系统中的反硝化菌

应用人工潜流湿地净化微污染地表水,出水用于补给人工景观河.利用定量PCR测定了湿地植物根际土壤和景观河底泥中16S rDNA和nosZ的丰度,并采用PCR-DGGE技术考察了样品中含nosZ基因的群落结构及其相似性.定量PCR结果表明,潜流湿地及人工景观河16S rDNA、nosZ平均绝对丰度(以DNA计)分别为1.91E+07、1.26E+06和2.68E+07、8.37E+05 copies.ng-1,以干土计时分别为1.45E+11、9.31E+09和5.31E+11、1.45E+10 copies.g-1.景观河底泥中微生物总量和反硝化菌数量要高于湿地根际土壤,但是后者nosZ相对丰度(3.8%～10.1%)则明显高于前者(1.7%～4.1%).根际土壤和底泥样品聚类分析相似度低,根际土壤优势菌种大部分与红杆菌目(Rhodobacearales)、根瘤菌目(Rhizobiales)和伯克氏菌目(Burkholderiales)的细菌相似,而底泥的优势菌种均为不可培养的微生物.     

一株克雷伯氏菌(Klebsiella sp.)Z6的分离及其产电特性研究

产电微生物是驱动微生物燃料电池(Microbial fuel cell,MFC)运行的关键.采用分离培养-MFC产电实验的方法,从以污水处理厂活性污泥为接种物的MFC阳极生物膜中分离到一株产电微生物,命名为Z6.菌株Z6的16S rDNA序列与已知菌株Klebsiell aoxytoca An16-2具有100%的同源性,结合该菌生理和形态特征将其初步鉴定为克雷伯氏菌属.菌株Z6接种MFC的产电结果表明,以柠檬酸钠为底物时MFC的最大体积功率密度达到14.35W·m-3,内阻为400Ω,显示出较强的电化学活性.通过循环伏安分析和外源AQDS添加实验结果推测,菌株Z6很可能通过分泌电子传递中间体传递电子.     

颗粒直链藻水华生消对婆罗异剑水蚤（桡足类）种群动态的影响

近年来,国内外学者对湖库型水华的发生机理和生态效应都做了大量研究,但有关水华生消对浮游动物群落结构影响的研究还很少.因此,本研究利用两个室外水泥池在中等尺度上考察了颗粒直链藻水华生消过程对婆罗异剑水蚤(桡足类)种群动态的影响,以及后者摄食对水华生消的下行调控作用.结果发现,颗粒直链藻水华发展迅速,仅5 d时间叶绿素浓度就从(21.24±0.75)μg·L-1上升到(240.34±11.00)μg·L-1;随后水华进入快速消退期,3 d后叶绿素a浓度下降到(53.63±0.47)μg·L-1.婆罗异剑水蚤的摄食压力对颗粒直链藻水华具有明显的抑制作用,水华生消期间含有婆罗异剑水蚤的藻液叶绿素a浓度比对照组低20μg·L-1左右,最大差异为26.08μg·L-1.期间婆罗异剑水蚤的丰度也由接入时的(56.50±4.32)ind·L-1增加到(142.11±6.35)ind·L-1,增加了1.5倍.该研究结果表明,在无鱼类摄食压力情况下,颗粒直链水华的爆发和消亡对婆罗异剑水蚤的生长和繁殖没有负面影响,反而促进了其种群数量的增加,这可能是由于水华期间为其提供了充足的饵料供应.     

短短芽胞杆菌及其芽胞对芘的降解

考察短短芽胞杆菌(Brevibacillus brevis)菌体及芽胞对四环多环芳烃芘的降解性能.结果表明,菌体5 d内对1 mg·L-1芘的降解率可达53%.菌体和胞内酶降解芘过程中检测到1-羟基芘、9-羟基菲、α-萘酚和β-萘酚这4种单羟基降解产物,在完整菌体降解体系中,产物呈现先积累后下降的趋势,而在胞内粗酶液降解体系中,大分子代谢产物表现为一直积累的趋势,说明B.brevis完整菌体在降解初期并不具备一些中间产物的降解酶,但随着时间推移,可被诱导产生相关酶对生成的新产物进行进一步降解.芽胞悬液在添加芘的无机盐培养基中5 d内萌发生成的营养细胞可达到1.5×109个·L-1,对1 mg·L-1芘的降解率达到15%.     

SO2对MnOx/PG催化剂低温脱硝的影响机理研究

采用等体积浸渍法制备了锰氧化物负载凹凸棒石(MnO_x/PG)低温SCR催化剂,通过SO₂暂态响应、程序升温表面反应(TPSR)等实验技术研究了烟气中SO₂对催化剂SCR脱硝活性的影响行为.采用程序升温脱附(TPD)、BET比表面及孔径分布测定、XPS等表征技术对催化剂硫中毒的机理及化学本质进行了深入分析.结果表明,低温下烟气中SO₂对MnO_x/PG催化剂的SCR脱硝活性存在显著的抑制作用,催化剂中毒主要由烟气中SO₂的催化氧化引起.一方面SO₂氧化为SO₃后与NH₃及H₂O竞争反应形成复杂的硫酸铵盐堵塞催化剂孔道,另一方面与活性组分MnO₂结合形成MnSO₄使得部分活性组分形态发生变迁.其中硫酸铵盐的形成可通过适当的热处理得以去除,而MnSO₄则不可恢复,但催化剂SCR活性却显著增加,表明MnSO₄的形成不是催化剂失活的主要因素.吸附态的硫可显著增加催化剂表面酸性,因此对SCR活性有促进作用.催化剂失活主要机理为:由气相SO₂的连续氧化并与NH₃相结合形成硫酸铵盐,并且在低温下难以分解,以致堵塞催化剂活性中心.     

Effect of MoO3 on vanadium based catalysts for the selective catalytic reduction of NOx with NH3 at low temperature

The selective catalytic reduction(SCR) activities of the MoO_3 doped V/WTi catalysts prepared by the incipient wetness impregnation method at low temperature were investigated.The results showed that the addition of MoO_3 could enhance the NO_ xconversion at low temperature and the best SCR activity was obtained when the dosage of MoO_3 reached5 wt.%. The NH3-TPD and DRIFTS experiments indicated that the addition of MoO_3 changed the type and number of acid sites on the surface of catalysts and reaction activities of acid sites were altered at the same time. The redox capacity and amount of active oxygen species got improved for V3Mo5/WTi catalyst, which could be confirmed by the H_2-TPR and transient response experiments. Water vapor inhibited the NO_xconversion at low temperature. Deposition of ammonium sulfate or bisulfate might be main reason for the loss of catalytic activity in the presence of SO_2 at low temperature. Choosing the suitable NH_3/NO ratio and elevation of reaction temperature both could weaken the influence of SO_2 on the SCR activity of the V3Mo5/WTi catalyst. Thermal treatment of the deactivated catalyst at350°C could get the low temperature activity recovered. The decrease of GHSV improved the de NO_x efficiency at low temperature and we speculated that the rational technological process and operation parameters could contribute to the application of this kind of catalysts in real industrial environment.     

Microbial reduction of uranium (VI) by Bacillus sp. dwc-2: A macroscopic and spectroscopic study

The microbial reduction of U(VI) by Bacillus sp. dwc-2, isolated from soil in Southwest China, was explored using transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge spectroscopy (XANES). Our studies indicated that approximately 16.0% of U(VI) at an initial concentration of 100 mg/L uranium nitrate could be reduced by Bacillus sp. dwc-2 at pH 8.2 under anaerobic conditions at room temperature. Additionally, natural organic matter (NOM) played an important role in enhancing the bioreduction of U(VI) by Bacillus sp. dwc-2. XPS results demonstrated that the uranium presented mixed valence states (U(VI) and U(IV)) after bioreduction, which was subsequently confirmed by XANES. Furthermore, the TEM and high resolution transmission electron microscopy (HRTEM) analysis suggested that the reduced uranium was bioaccumulated mainly within the cell and as a crystalline structure on the cell wall. These observations implied that the reduction of uranium may have a significant effect on its fate in the soil environment in which these bacterial strains occur.