Shewanella oneidensis MR-1对针铁矿的还原与汞的生物甲基化

在实验室模拟条件下,研究了铁还原菌奥奈达希瓦氏菌Shewanella oneidensis MR-1对针铁矿的异化还原及其对汞生物甲基化的影响.结果表明,S.oneidensis MR-1能溶解针铁矿,并能将溶解出的Fe3+还原成Fe2+;S.oneidensis MR-1也是一种汞甲基化细菌,能够将无机汞转化成甲基汞.铁的溶解还原作用随着初始针铁矿剂量的大幅增加而减弱,针铁矿的异化还原在一定程度内促进汞的生物甲基化.弱酸性条件比中碱性和强酸条件有利于汞的甲基化;腐殖酸在低浓度促进汞甲基化,浓度过高则会抑制汞的甲基化.     

针铁矿、磁铁矿和石膏对2,4-二氯苯酚厌氧降解的影响

2,4-二氯苯酚(2,4-dichlorophenol,2,4-DCP)常用于农药生产,在水体和土壤中广泛分布,具有难降解、高毒性的特点.通过模拟自然过程,在厌氧反应体系中投加铁氧化物和硫酸盐矿物,重点考察了不同矿物对2,4-DCP降解的影响.结果发现,厌氧体系中针铁矿、磁铁矿和石膏对2,4-DCP均没有明显的吸附作用;质量衡算结果表明所有反应体系中仅发生2,4-DCP向4-氯苯酚(4-chlorophenol,4-CP)的转化;与无外加碳源组相比,乙酸钠的加入使得2,4-DCP的还原脱氯反应速率增大一倍.分析表明针铁矿和磁铁矿加入可刺激脱氯功能菌的生长或活性,进而提高微生物的电子传递能力和2,4-DCP的降解速率;石膏加入强烈抑制脱氯功能菌的生长或活性,进而抑制2,4-DCP的降解.研究结果对认识难生化降解卤代酚在厌氧环境中的迁移转化及环境工程中此类物质的处理具有潜在意义.     

重金属-柠檬酸-针铁矿三元体系的表面络合模型研究

根际环境产生的柠檬酸等小分子有机酸可能影响重金属的溶出效应.本文研究了 4种重金属Cd、Pb、Cu、Ni及柠檬酸在针铁矿表面的三元体系吸附行为,结果发现柠檬酸促进了 4种重金属酸性条件下在针铁矿表面的吸附量,而Cu、Ni促进了柠檬酸碱性条件下的吸附.结合红外光谱图发现,重金属-柠檬酸-针铁矿主要存在以下2种三元体系形态...     

针铁矿对城市生活垃圾有机组分厌氧发酵的影响

利用PVC管构建厌氧发酵反应器,研究了铁氧化物对有机垃圾厌氧发酵过程中产气及垃圾渗滤液特性的影响.结果表明,添加针铁矿能够促进垃圾的水解酸化效率和产气速率,提高产气量至163.4 L,较空白提高了20%.通过对厌氧消化中间产物Fe2+、NH+4-N、NO-3-N、COD以及有机酸的分析表明,铁氧化物的存在有利于降低系统氧化还原电位,有助于提高厌氧微生物的水解酸化效率;铁氧化物的加入能够促进有机酸的转化,从而降低有机酸对厌氧微生物的抑制作用.     

天然和水热合成针铁矿对有机物厌氧分解释放CH4的影响

以乙酸钠为碳源,通过序批式实验研究了天然和水热合成针铁矿对铁还原菌-甲烷菌厌氧微生物生化系统中CH4释放量的影响.通过对实验过程中气体组分、溶液中总有机碳(TOC)、总无机碳(TIC)、Fe2+等主要组分的分析测定和固体产物的X-射线衍射(XRD)分析,结合对矿物的比表面(BET)、XRD、X-射线荧光光谱(XRF)分析表征,探讨了针铁矿在铁还原菌存在下对有机物厌氧消化产CH4的影响和作用机制.利用修正Gompertz方程对累计产CH4和CO2量进行拟合.结果表明,与对照实验组相比,添加针铁矿能使CH4累计释放量提前60～78 d达到最大值,并且能有效降低CO2释放量达30%～67%,添加水热合成针铁矿较之天然针铁矿更能促进CH4释放和减少CO2释放;固体产物分析表明添加针铁矿促使菱铁矿形成固定部分CO2.     

十二烷基二甲基甜菜碱(BS-12)在合成针铁矿表面的吸附特征

为了探究十二烷基二甲基甜菜碱(BS-12)在水合针铁矿(α-FeOOH)表面的吸附过程和机理,在不同pH值、离子强度以及温度下采用批处理法研究了针铁矿对BS-12的吸附特征;并对BS-12在针铁矿表面的吸附机制进行了探讨.研究结果表明:针铁矿对BS-12的吸附平衡时间约为8 h,吸附过程符合伪二级动力学模型,吸附速率受化学吸附机理控制.Freundlich等温吸附模型能较好地描述针铁矿对BS-12的吸附,pH值对针铁矿吸附BS-12影响显著,主要取决于针铁矿的电荷零点和BS-12的等电点;离子强度的增加对BS-12的吸附有促进作用;温度的升高促进BS-12的吸附.热力学参数结果表明,针铁矿对BS-12的吸附是一个具有熵增和焓增特征的自发性吸热过程.BS-12在针铁矿表面的吸附是一个较慢发生的吸热的化学吸附的过程,主要吸附机制为化学键作用和疏水结合模式.     

针铁矿的非生物还原解离特征及Slogistic模型拟合

以针铁矿为研究对象,分析了电子供体和针铁矿浓度以及氧化还原中介体AQS对针铁矿非生物还原解离作用的影响.结果表明,在没有氧化还原中介体的参与下,针铁矿的非生物还原作用十分微弱;AQS加入体系后,针铁矿的非生物还原程度在经历一定的反应时间后显著加剧,且还原过程中生成的解离态Fe(ΙΙ)含量随时间的变化趋势符合典型的Slogistic曲线特征.Slogistic拟合结果表明:一定电子供体浓度下,不同浓度针铁矿的非生物还原Slogistic模型拟合的校正R2在0.9887~0.9953之间.当针铁矿浓度维持为一恒定值时,电子供体浓度不足的情况下,针铁矿的非生物还原的Slogistic 曲线特征较弱;当电子供体浓度充足的条件下,Slogistic模型拟合的校正R2系数可高达0.9967.电子供体和针铁矿浓度以及氧化还原中介体AQS的参与对Slogistic模型拟合参数均有一定的影响.     

胡敏酸-针铁矿复合胶体对Pb2+的吸附特征

采用批平衡试验法,研究了胡敏酸-针铁矿复合胶体对Pb2+的等温吸附特征及pH值、离子强度、温度及共存Cd2+对复合胶体吸附Pb2+的影响.结果表明:在相同离子强度和温度条件下,pH值升高,最大吸附量(Smax)和吸附平衡常数(k)均增大,有利于吸附反应的进行.等温吸附方程以Langmuir方程拟合效果最好.当Pb2+平衡浓度为124.7mg/L时,吸附量增幅最大,达35mg/g.复合胶体对Pb2+的吸附动力学方程以Elovich方程拟合效果最好.pH值增大,平衡吸附速率提高.在相同pH值和离子强度条件下,温度升高,最大吸附量、吸附平衡常数、自由能变△G°的绝对值均增加,表明升高温度有利于吸附反应的进行.在相同温度和pH值条件下,复合胶体对Pb2+的吸附量随着离子强度的增加而增加.当存在Cd2+时,复合胶体对Pb2+的吸附量有所降低,但Cd2+对Pb2+竞争吸附影响不大.     

Characteristics and model studies for fluoride and arsenic adsorption on goethite

Fluoride and arsenic are major anionic elements of concern in drinking water treatment. The effects of contact time, pH, surface loading and ionic strength on adsorption of fluoride and As(V) were investigated using batch methods. Adsorption of fluoride and As(V) onto goethite obeyed a pseudo second-order rate law. Through experimental data and adsorption kinetic analysis, the affinity of As(V) onto goethite was stronger than fluoride. Fluoride and As(V) uptake by goethite all decreased with pH increasing at the same surface loading; however, ionic strength had slight influence on their adsorption. A surface sites-species model was used to quantify the adsorption of fluoride and As(V) onto goethite as function of pH and surface loading. This model can satisfactorily predict their adsorption characteristics with several adsorption constants.     

Comparative characterization of two natural humic acids in the Pearl River Basin, China and their environmental implications

Two humic acids (HAs) were isolated from contaminated river sediments present under comparative conditions in the Pearl River Basin, China. YFHA (the HA extracted at an open pyrite mining area in Yunfu) exhibited a lower absorption intensity for certain bands in the Fourier transform infrared spectra, a lower E4/E6 value (the UV absorbances at 465 nm (E4) and 665 nm (E6)), a lower apparent molecular weight, a lower polarity and a lower oxygen functionality in comparison with GZHA (the HA isolated at an urban living area in Guangzhou). All these differences indicated a higher degree of humification of YFHA than GZHA. Overall, the enrichment patterns of permanent heavy metals in the studied HAs were similar to those in corresponding sediments. In particular, YFHA exhibited high enrichment of trace element Tl, a characteristic concomitant from the mining of the pyrite minerals. The adsorption isotherms of two HAs for goethite and pyrolusite, two representative geological materials, conformed to the Langmuir equation. Based on the qualitative relationships between the Langmuir constants of the adsorption isotherms and the chemical characteristics of HAs, the main mechanism of HA adsorption on these materials was suggested to be hydrophobic interaction. This study highlighted the promising use of HA as a peculiar bio-indicator of uncommon trace metal contaminations. The HA adsorption mechanism on representative geological materials further provided a theoretical basis for the study on the unusual metal behavior in complex environmental settings.