基于蒙特卡洛模拟与PMF模型的黄河流域沉积物重金属污染评价及源解析

沉积物是河流的重要组成部分,而沉积物中重金属的富集严重威胁着水环境安全.黄河流域沿程分布着众多工业城市,且流域水土流失量大,泥沙携带重金属进入河流导致沉积物重金属污染问题日趋严重,研究黄河流域沉积物中重金属污染状况对流域生态安全具有重要意义.收集2000~2020年发表的关于黄河流域沉积物中重金属（铅、镉、铬、砷、锌、铜、镍和汞）含量的数据,首先基于描述性统计及地统计法分析重金属的空间分布特征,进一步采用蒙特卡洛法进行地累积指数（I_geo）、潜在生态风险及毒性单位概率的评价,最后结合正定矩阵因子分解模型（PMF）与Pearson相关性分析确定污染源个数及贡献率.结果发现,黄河流域沉积物中ω（Pb）、ω（As）、ω（Zn）、ω（Ni）、ω（Cu）、ω（Hg）、ω（Cr）和ω（Cd）的均值分别为26.92、11.78、87.17、31.13、24.96、0.07、73.36和0.58 mg·kg^-1,分别超过黄河流域各省土壤背景值均值1.27、1.08、1.26、1.05、1.09、2.32、1.14和5.95倍,其中Cd超标倍数最大,应当引起重视;I_geo：Cd>Hg>Cr>Cu>Pb>Zn>As>Ni,Cd和Hg存在中度-严重污染;数据表明黄河流域上、中和下游沉积物重度生态风险占比分别为18.6%、15.7%和7.1%,呈递减趋势;黄河流域沉积物中重金属处于低毒性状态;溯源分析表明黄河流域沉积物重金属的4个来源分别是矿业源（42.2%）、自然活动（38.3%）、农业活动（11.6%）和电镀废水（7.9%）.研究结果可为黄河流域制定相关污染防控措施提供依据.     

Biodegradation of coplanar polychlorinated biphenyls by anaerobic microorganisms from estuarine sediments.

In this study, we investigated the biodegradability of biphenyl and 5 congeners (one non-planar and four coplanar) of polychlorinated biphenyl (PCB). Biphenyl, the non-planar congener 2,3',4',5-tetrachlorobiphenyl (25-34 CB), and the four coplanar congeners 3,3',4,4'-tetrachlorobiphenyl (34-34 CB), 3,4,4',5-tetrachlorobiphenyl (345-4 CB), 3,3',4,4',5-pentachlorobiphenyl (345-34 CB), and 3,3',4,4',5,5'-hexachlorobiphenyl (345-345 CB) were amended at a concentration of 10 mg/L into anoxic sediment slurries collected from the estuaries of the Tansui River and the Erjen River. During 2 years' incubation under sulfidogenic conditions, biphenyl was persistent, while all other chlorinated congeners, except for 345-345 CB, were dechlorinated with or without a lag period in sediment slurries collected from both rivers. Dechlorination of coplanar and non-planar congeners began with para chlorine removal. All para chlorines from the mono-, di-, and trichlorobiphenyl groups could be removed by sediment slurries from both rivers. Microbial communities in sediment from the Erjen River additionally fostered meta-dechlorination activity, but only after removal of all the para chlorines. Addition of Tween 20 (0.05%, v/v) into sediment slurries from the Tansui River did not enhance dechlorination rates or extents, but the addition of toluene- or 3-chlorobenzoate-adapted sediments enhanced dechlorination of 34-34 CB and 345-4 CB.     

Bacterial diversity in paclobutrazol applied agricultural soils

The aim of this study was to investigate the bacterial communities on paclobutrazol [(2RS, 3RS)-1-(4-Chlorophenyl)-4, 4-dimethyl-2-(1H-1,2,4-triazol-1-yl) pentan-3-ol]–applied agricultural soils by denaturing gradient gel electrophoresis (DGGE) of polymerase chain reaction (PCR) amplified 16S rDNA gene fragments. Three different agricultural soil samples were collected from paclobutrazol applied mango and waxapple orchards, peanut fields and untreated rice fields as a control for DGGE analysis. The DGGE pattern of PCR- generated 16S rDNA gene fragments indicated that the bacterial populations from four paclobutrazol–applied soils of peanut fields were closely related to each other and two paclobutrazol–applied soils of mango and waxapple orchards harbored closely related bacterial communities. But, paclobutrazol–free agricultural soils comprised relatively a different bacterial group. However, the bacterial populations of mango and waxapple orchard are completely different from the bacterial communities of peanut field. Further purification and sequence analysis of 40 DGGE bands followed by phylogenetic tree assay showed similar results that soil bacteria from paclobutrazol applied mango and waxapple orchard are phylogenetically related. Based on the phylogenetic analysis, the clone M-4 was clad 100 % (bootstrap value) with Mycobacterium sp. The Mycobacterium sp. has been proved to degrade the phenolic compounds such as phenol, 4-chlorphenol, 2,4-dichlorophenol and paclobutrazol molecule containing chlorobenzene ring.     

Characteristics of organic precursors and their relationship with disinfection by-products

The molecular weight distribution and chemical composition of precursors and their relationship with disinfection by-products (DBPs) were investigated. Most of the organic matter responsible for the major DBP precursors in the Pan-Hsin water are small compounds with a molecular weight less than 1 kDa. The hydrophobic acids display the greatest ability to produce DBP. Therefore, effective removal of small molecules or hydrophobic acidic organics prior to disinfection process will significantly reduce the DBP concentration in the finished water. Although the coagulation process is effective in removing large organic precursors and the removal efficiencies of CHCl3 formation potential and organic carbon increase proportionally to the molecular weight of the precursors, the conventional treatment methods have limited efficiency in eliminating small precursors, which have high DBP formation potential.     

Characteristics of springtime profiles and sources of ozone in the low troposphere over northern Taiwan

To quantify the possible sources of the high ambient ozone concentration in the low troposphere over Taiwan, ozone sounding data from a two-year intensive field measurement program conducted in April and early May of 2004 and 2005 in northern Taiwan has been examined. We found that the vertical ozone distributions and occurrence of enhanced ozone in the lower troposphere (below 6 km) mainly resulted from (1)Type NE: the long-range transport of ozone controlled by the prevailing northeasterly winds below 2 km, (2)Type LO: the local photochemical ozone production process, and (3)Type SW: the strong southwest/westerly winds aloft (2–6 km). In the boundary layer (BL), where Asian continental outflow prevails, the average profile for type NE is characterized by a peak ozone concentration of nearly 65 ppb at about 1500 m altitude. For type LO, high ozone concentration with an average ozone concentration greater than 80 ppb was also found in the BL in the case of stagnant atmospheric and sunny weather conditions dominated. For type SW, significant ozone enhancement with average ozone concentration of 70–85 ppb was found at around 4 km altitude. It is about 10 ppb greater than that of the types NE and LO at the same troposphere layer owing to the contribution of the biomass burning over Indochina. Due to Taiwan's unique geographic location, the complex interaction of these ozone features in the BL and aloft, especially features associated with northeasterly and south/southwesterly winds, have resulted in complex characteristics of ozone distributions in the lower troposphere over northern Taiwan.     

Development of regenerative dye impregnated mesoporous silica materials for assessing exposure to ammonia

The mesostructured materials MCM-41 and SBA-15 were studied as possible supports of bromocresol green (BG) dye impregnation for the ammonia gas detection because of their large surface area, high regenerative property, and high thermal stability. X-ray diffraction, transmission electron microscopy, scanning electron microscope, and N2 adsorption analysis were used to characterize the prepared materials. These materials could sense ammonia via visible color change from yellowish-orange to blue color. The color change process of the nanostructured materials was fully reversible during 10 cyclic tests. The results indicated that the ammonia absorption responses of the two nanostructured materials were both very sensitive, and high linear correlation and high precision were achieved. As the gaseous ammonia concentrations were 50 and 5 ppmv, the response times for the SBA-15/BG were only 1 and 5 min, respectively. Moreover the BG dye-impregnated SBA-15 was less affected by the variation in the relative humidity. It also had faster response for the detection of NH3, as well as lower manufacturing price as compared to that of the dye-impregnated MCM-41. Such feature enables SBA-15/BG to be a very promising material for the detection of ammonia gas.     

Adsorption characteristics of benzene on biosolid adsorbent and commercial activated carbons

This study selected biosolids from a petrochemical waste-water treatment plant as the raw material. The sludge was immersed in 0.5-5 M of zinc chloride (ZnCl2) solutions and pyrolyzed at different temperatures and times. Results indicated that the 1-M ZnCl2-immersed biosolids pyrolyzed at 500 degrees C for 30 min could be reused and were optimal biosolid adsorbents for benzene adsorption. Pore volume distribution analysis indicated that the mesopore contributed more than the macropore and micropore in the biosolid adsorbent. The benzene adsorption capacity of the biosolid adsorbent was 65 and 55% of the G206 (granular-activated carbon) and BPL (coal-based activated carbon; Calgon, Carbon Corp.) activated carbons, respectively. Data from the adsorption and desorption cycles indicated that the benzene adsorption capacity of the biosolid adsorbent was insignificantly reduced compared with the first-run capacity of the adsorbent; therefore, the biosolid adsorbent could be reused as a commercial adsorbent, although its production cost is high.     

Determination of estrogenic compounds in wastewater using liquid chromatography-tandem mass spectrometry with electrospray and atmospheric pressure photoionization following desalting extraction

Two complementary LC-MS ionization methods, electrospray (ESI) and atmospheric pressure photoionization (APPI), have been optimized to determine three natural estrogenic compounds (estrone, 17beta-estradiol and estriol) and two synthetic estrogenic compounds (17alpha-ethynylestradiol and diethylstilbestrol) in the influent and effluent of wastewater treatment plants (WWTPs). The wastewater samples were first subjected to solid-phase extraction coupled with desalting extraction to remove matrix interference. The analytes were then detected using liquid chromatography-tandem mass spectrometry (LC-MS-MS) with ESI and dopant-assisted (DA) APPI to evaluate the ion suppression effect and to complement the detection and quantification of estrogenic compounds in complex wastewater samples. The average ion suppression factors for the extracts of the WWTP influent analyzed using ESI and APPI were 52+/-5% and 27+/-7%, respectively. The sensitivity and ionization efficiency of the LC-ESI-MS-MS system decreased dramatically when a complex matrix was present in the WWTP influent sample. Estrogenic compounds could be detected in the WWTP influent and effluent samples at concentrations below the parts-per-billion level. The lower detection limits obtained when using ESI and the higher matrix tolerance of the APPI method allowed the complete quantification of estrogenic compounds in very complex samples in a complementary manner.     

Fate of polycyclic aromatic hydrocarbons during vitrification of incinerator ash in a coke bed furnace

Fate of polycyclic aromatic hydrocarbons (PAHs) during the vitrification of fly ash and bottom ash from the municipal waste incinerator in a coke bed furnace was investigated. In this system, both coke and lime were added to enhance the melting reaction. The major PAH sources in this system were ash and coke, which respectively contributed 97% and 3% of PAHs in the input-mass. During vitrification process, low molecular PAHs (LM-PAH, 2-3-ring), median molecular PAHs (MM-PAH, 4-ring) and high molecular PAHs (HM-PAH, 5-7-ring) mass respectively accounted for >99%, >99% and 84% of the output-mass emitted as the stack flue gas; while those discharged from the slag were <1%, <1% and 16%, respectively. The O/I (output-mass/input-mass) ratio of LM-, MM- and HM-PAHs were 0.063, 0.002 and <0.001, respectively. The high distribution in flue gas and O/I ratio of LM-PAHs is reasonable since they are more easily evaporated, hence difficult to be removed by air pollution control devices. On the contrary, the HM-PAHs, having lower vapor pressure, primarily stays mainly in slag. Based on the 21 total PAH content in feeding ash and slag, the reduction efficiency of the coke bed furnace was >99.9%. To minimize the risk of secondary pollution, the efficiency of coke bed furnace should be improved to reduce the PAH emission into ambient air.     

Monolignol biosynthesis and genetic engineering of lignin in trees, a review

This paper summarizes our previous and current research on genetic engineering of lignin biosynthesis for the purposes of improving wood pulping and bleaching efficiency. For these purposes, our targets were to produce transgenic trees with low content of lignin that is also chemically reactive (high lignin S/G ratio). Using aspen as a model species, we have characterized the biochemical functions of various genes and the kinetic properties of these gene products involved in monolignol biosynthetic pathway. The results of these characterizations proved strong evidence for a principle phenolic flux leading to the formation of monolignols. Biochemical evidence further demonstrated that, in this principle flux, 4CL could be the enzyme limiting total lignin accumulation, whereas CAld5H might control the lignin S/G ratio. These propositions were fully supported by the in vivo functions of these enzymes. Transgenic trees with inhibited 4CL enzyme activity exhibited 5–45% reduction in lignin contents. The chemical structure of the resulting lignin remained essentially unchanged. More importantly, the lignin reduction was compensated for by a concomitant increase in cellulose content. When antisense 4CL and sense coniferaldehyde 5-hydroxylase (CAld5H) genes were simultaneously transferred into aspen via Agrobacterium, transgenic trees expressing each one and both of the transgenes were produced. Lignin reductions up to 55% were achieved in antisense 4CL plants and up to 3-fold S/G increases were observed in sense CAld5H plants. These effects were independent but additive, with plants expressing both transgenes having less lignin and higher S/G ratio. Consistent with our previous results, lignin reduction has always resulted in an increase in cellulose content. These transgenics could be potentially valuable for pulp production. But more importantly, these benchmark transgenics are rich sources of information for functional genomics and metabolic engineering, allowing the generation of the ultimate raw materials for wood pulp production.