辽河流域与英国中部河湖水体中溶解有机质的荧光特性

运用三维荧光光谱技术对辽河流域和英国中部水体中溶解有机质(DOM)的荧光光谱特性进行了分析.结果表明,辽河流域各研究水体中DOM包含4种荧光组分,即类色氨酸、类酪氨酸、可见光区和紫外光区类腐殖质,通过对荧光特性定量指标的分析可知,辽河流域各研究断面水体中类腐殖质物质内源作用大于陆源,DOM具有较强的新近自生源,各河流水体中DOM腐殖化程度顺序为:浑河中游海城河中游蒲河下游太子河下游.相比之下,英国河湖中,除了River Tame含有以上4种荧光组分外,其它水体中均没有发现类酪氨酸荧光物质,甚至在River Tern中仅含有类腐殖质荧光物质,河湖中DOM含有较少的新近自生源组分,以陆源影响为主.另外,辽河流域水体中类蛋白与类腐殖质荧光峰强度比值大于英国各河流水体的平均值.由此可以推断,辽河流域各研究断面大量污染物的输入,是造成其严重内源污染的主要原因,从而使水体中DOM含量增加,英国各河流断面其DOM主要来自于水体本身存在的大量微生物和浮游植物的代谢活动以及土壤有机质经雨水的冲刷流入水体的贡献.     

Characterization of extracellular polymeric substances in the biofilms of typical bacteria by the sulfur K-edge XANES spectroscopy

A combined approach of physicochemical extraction and sulfur K-edge X-ray absorption near-edge structure（XANES） spectroscopy was applied to characterize the extracellular polymeric substances（EPS） of typical bacterial biofilms in this study. Physicochemical analysis showed variation of the contents of DNA,polysaccharide and protein in different fractions of EPS in different mediums. The sulfur K-edge XANES analysis yielded a variety of spectra.Spectral fitting of the XANES spectra utilizing a large set of model compounds showed that there was more reduced sulfur in both LB-EPS（loosely bound EPS） and TB-EPS（tightly bound EPS） of all the biofilms in LB medium than in R2 A medium. More oxidized sulfur was identified in LB-EPS than that in TB-EPS,suggesting different niches and physiological heterogeneity in the biofilms. Our results suggested that the sulfur K-edge XANES can be a useful tool to analyze the sulfur speciation in EPS of biofilms.     

Mo-modified Pd/Al2O3 catalysts for benzene catalytic combustion

Mo-modified Pd/Al2O3catalysts were prepared by an impregnation method and tested for the catalytic combustion of benzene. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction（XRD）, X-ray photoelectron spectroscopy（XPS）, temperatureprogrammed desorption of NH3（NH3-TPD）, H2temperature-programmed reduction（H2-TPR）, and high-angle annular dark-field scanning transmission electron microscopy（HAADF-STEM）. The results showed that the addition of Mo effectively improved the activity and stability of the Pd/Al2O3catalyst by increasing the dispersion of Pd active components, changing the partial oxidation state of palladium and increasing the oxygen species concentration on the surface of catalyst. In the case of the Pd-Mo/Al2O3catalyst,benzene conversion of 90% was obtained at temperatures as low as 190°C, which was 45°C lower than that for similar performance with the Pd/Al2O3catalyst. Moreover, the 1.0% Pd-5% Mo/Al2O3catalyst was more active than the 2.0% Pd/Al2O3catalyst. It was concluded that Pd and Mo have a synergistic effect in benzene catalytic combustion.     

Pd/activated carbon sorbents for mid-temperature capture of mercury from coal-derived fuel gas

Higher concentrations of Hg can be emitted from coal pyrolysis or gasification than from coal combustion, especially elemental Hg. Highly efficient Hg removal technology from coal-derived fuel gas is thus of great importance. Based on the very excellent Hg removal ability of Pd and the high adsorption abilities of activated carbon（AC） for H2 S and Hg, a series of Pd/AC sorbents was prepared by using pore volume impregnation, and their performance in capturing Hg and H2 S from coal-derived fuel gas was investigated using a laboratory-scale fixed-bed reactor. The effects of loading amount, reaction temperature and reaction atmosphere on Hg removal from coal-derived fuel gas were studied. The sorbents were characterized by N2 adsorption, X-ray diffraction（XRD） and X-ray photoelectron spectroscopy（XPS）. The results indicated that the efficiency of Hg removal increased with the increasing of Pd loading amount, but the effective utilization rate of the active component Pd decreased significantly at the same time. High temperature had a negative influence on the Hg removal. The efficiency of Hg removal in the N2-H2S-H2-CO-Hg atmosphere（simulated coal gas） was higher than that in N2-H2S-Hg and N2-Hg atmospheres, which showed that H2 and CO, with their reducing capacity, could benefit promote the removal of Hg. The XPS results suggested that there were two different ways of capturing Hg over sorbents in N2-H2S-Hg and N2-Hg atmospheres.     

Biosorption mechanisms involved in immobilization of soil Pb by Bacillus subtilis DBM in a multimetal-contaminated soil

Mechanisms of soil Pb immobilization by Bacillus subtilis DBM, a bacterial strain isolated from a heavy-metal-contaminated soil, were investigated. Adsorption and desorption experiments with living bacterial cells as well as dead cells revealed that both extracellular adsorption and intracellular accumulation were involved in the Pb2＋removal from the liquid phase. Of the sequestered Pb（II）, 8.5% was held by physical entrapment within the cell wall, 43.3% was held by ion-exchange, 9.7% was complexed with cell surface functional groups or precipitated on the cell surface, and 38.5% was intracellularly accumulated.Complexation of Pb2＋with carboxyl, hydroxyl, carbonyl, amido, and phosphate groups was demonstrated by Fourier transform infrared spectroscopic analysis. Precipitates of Pb5（PO4）3OH, Pb5（PO4）3Cl and Pb10（PO4）6（OH）2that formed on the cell surface during the biosorption process were identified by X-ray diffraction analysis. Transmission electron microscopy–energy dispersive spectroscopic analysis confirmed the presence of the Pb（II）precipitates and that Pb（II） could be sequestered both extracellularly and intracellularly.Incubation with B. subtilis DBM significantly decreased the amount of the weak-acid-soluble Pb fraction in a heavy-metal-contaminated soil, resulting in a reduction in Pb bioavailability, but increased the amount of its organic-matter-bound fraction by 71%. The ability of B.subtilis DBM to reduce the bioavailability of soil Pb makes it potentially useful for bacteria-assisted phytostabilization of multi-heavy-metal-contaminated soil.     

Ultrasonic preparation of nano-nickel/activated carbon composite using spent electroless nickel plating bath and application in degradation of 2,6-dichlorophenol

Ni was effectively recovered from spent electroless nickel （EN） plating baths by forming a nano-nickel coated activated carbon composite. With the aid of ultrasonication, melamine- formaldehyde-tetraoxalyl-ethylenediamine chelating resins were grafted on activated carbon （MFT/AG）. PdC12 sol was adsorbed on MFT/AC, which was then immersed in spent electroless nickel plating bath; then nano-nickel could be reduced by ascorbic acid to form a nano-nickel coating on the activated carbon composite （Ni/AC） in situ. The materials present were carefully examined by Fourier transform infrared spectroscopy, X-ray diffraction, field emission scanning electron microscopy, X-ray photoelectron spectroscopy and electro- chemistry techniques. The resins were well distributed on the inside and outside surfaces of activated carbon with a size of 120 ± 30 nm in MFT/AC, and a great deal of nano-nickel particles were evenly deposited with a size of 3.8 ± 1.1 nm in Ni/MFT. Moreover, Ni/AC was successfully used as a catalyst for ultrasonic degradation of 2.6-dichloronhenol.     

电子受体类型对聚磷污泥胞外聚合物的影响研究

采用3种电子受体(硝氮、亚硝氮、氧),在SBR反应器中分别驯化了具有稳定除磷能力的聚磷污泥。对比研究了不同聚磷污泥胞外聚合物(EPS)的组分与含量,结合三维荧光光谱对EPS中有机物质进行分析。研究表明,以硝氮、亚硝氮为电子受体的聚磷污泥EPS平均浓度较为接近,分别为115.6mg/gVSS、133.5 mg/gVSS,由厌氧段至缺氧段,EPS总浓度有所下降。以氧为电子受体聚磷污泥的EPS平均浓度相对较高,为194.5 mg/gVSS,由厌氧段至好氧段,EPS总浓度略有升高。不同聚磷污泥的EPS组分均以胞外蛋白为主,占EPS总量的53%~65%,多糖与核酸占EPS总量28%~34%、5%~7%。三维荧光光谱显示3种聚磷污泥EPS均具有芳香结构蛋白质、可溶性代谢物的荧光峰,另外,以硝氮为电子受体的聚磷污泥还具有明显的腐殖酸类物质的荧光峰。研究结果表明电子受体对聚磷污泥EPS的组分、浓度、有机质类别有一定的影响。     

便携β射线法手工监测PM_(2.5)的可行性研究

提出利用自动射线原理结合重量法的简捷便携特点的便携射线仪手工监测PM2.5的思路,平行比对了便携射线法和手工重量法所测60组PM2.5浓度的监测结果,采用线性回归及T检验、F检验等理论分析了两者数据结果间的有效性和可比性。结果表明,便携式射线仪监测结果与重量法监测结果之间有效可比且得到了两者间的线性回归方程;此外进行了20组数据的实样验证,换算值和真值之间相对误差在8%以内,因而确定了便携射线仪手工监测PM2.5的可行性。     

重金属阳离子荧光传感器合成及光谱性研究

通过亚胺缩合的反应制备出阳离子荧光传感器（Cation Fluorescent Sensors,CFSs）,并对其结构、光谱性能检测、荧光量子产率等进行了详细的研究.通过荧光化学传感器产生的荧光光谱一直是高效的分析方法,因此合成了新的基于席夫碱的荧光化学传感器,并研究了对各种金属离子的结合特性.在CH3CN溶液中测试了阳离子荧光传感器时不同阳离子的选择性响应,发现对Cu2＋有较好的选择性,可用于Cu2＋的检测.该类阳离子荧光传感器是基于2,2-联噻吩-5-乙醛的荧光发射基团和邻氨基苯甲醚为识别基团的一类阳离子荧光传感器.     

三维荧光光谱应用于海水中有色溶解有机物分析的探讨

对三维荧光光谱(excitation emission matrix spectroscopy,EEMs)应用于海水中有色可溶性有机物(chromophoricdissolved organic matter,CDOM)分析进行了综述。阐明了海水中CDOM在海洋生物地球化学循环和气候变化中的重要作用,指出了传统分析方法的不足,论述了EEMs用于CDOM分析的优势和不足,总结了国内外在该领域的研究概况,详述了影响海水中CDOM三维荧光光谱特性的主要影响因素,最后对EEMs技术在海水CDOM分析中应用的前景和待解决的问题进行了展望。