Catalytic hydrogenation of polyaromatic hydrocarbon (PAH) compounds in supercritical carbon dioxide over supported palladium

A series of supported palladium catalysts were evaluated for their ability to mediate the complete hydrogenation of polycyclic aromatic hydrocarbon (PAH) compounds. Benzo[a]pyrene (B[a]P) or phenanthrene (Phe) in hexane was merged with a hydrogen-carbon dioxide [5% (w/w) H(2)/CO(2)] stream and transferred to a flow through mini-reactor (capacity ca. 1 g) that was maintained at 90 degrees C under a back-pressure of 20.68 MPa. Effluent from the reactor trapped in hexane was monitored/quantified by gas chromatography-mass spectrometry. Catalyst formulations supported on iron powder, high density polyethylene (HDPE) or gamma-alumina were prepared and compared in terms of hydrogenation activity as measured by the quantity of substrate per unit time that could be perhydrogenated to toxicologically innocuous products. Both of the Pd preparations supported on gamma-alumina were more efficient than a commercial Pd(0) (5% w/w) on gamma-Al(2)O(3) formulation or preparations supported on HDPE or the iron powder. Bimetallic mixtures with Pd increased the hydrogenation activity when co-deposited with Cu or Ni but not with Ag or Co. However, increases in hydrogenation activity by increasing the loading of Pd (or bimetallic mixture) on this surface were limited. Despite using supercritical carbon dioxide (scCO(2)) to swell the surfaces of the polymer, the deposition of nanoparticles within the polyethylene formulation was appreciably less active than either the oxidic or the Fe(0) formulations.     

Sorption of organic contaminants by biopolymers: role of polarity, structure and domain spatial arrangement

Sorption behavior of hydrophobic organic contaminants (HOCs) (i.e., pyrene, phenanthrene and naphthalene) by native and chemically modified biopolymers (lignin, chitin and cellulose) was examined. Lignins (native and treated) showed nonlinear sorption for all compounds studied, emphasizing their glassy character. Chitins and celluloses had linear isotherms for phenanthrene and naphthalene, illustrating the dominance of partitioning, while pyrene yielded nonlinear isotherms. Sorption capacity (K(oc)) of HOCs was negatively correlated with the polarity [(O+N)/C] of the biopolymers. Aromatic and alkyl+aromatic C percentages, rather than alkyl C content, demonstrated a better correlation with K(oc) values, indicating the importance of aromatic structures for HOC affinity. Hydrophobicity (K(ow))-normalized K(oc) values decreased sharply with increasing percentage of O-alkyl C versus total aliphatic C (O-alkyl C/total aliphatic C) or with polar C/(alkyl+aromatic C) ratio of the biopolymers until their values reached 80% and 4, respectively, illustrating the effect of surrounding polar groups on reducing affinity for HOCs. Overall, the results of this study highlight the role of spatial arrangement of domains within biopolymers in sorption of HOCs, and point to sorbent properties, such as functionality, polarity and structure, jointly regulating the sorption of HOCs in biopolymers.     

Determining Sources of Fecal Bacteria in Waterways

The microbiological contamination of waterways by pathogenic microbes has been, and is still, a persistent public safety concern in the United States and in most countries of the world. As most enteric pathogens are transmitted through the fecal–oral route, fecal pollution is generally regarded as the major contributor of pathogens to waterways. Fecal pollution of waterways can originate from wastewater treatment facilities, septic tanks, domestic- and wild-animal feces, and pets. Because enteric pathogens are derived from human or animal sources, techniques capable of identifying and apportioning fecal sources have been intensively investigated for use in remediation efforts and to satisfy regulatory concerns. Pollution of human origin is of the most concern, since human feces is more likely to contain human-specific enteric pathogens. Fecal indicator bacteria have been used successfully as the primary tool for microbiologically based risk assessment. However measurement of fecal indicator bacteria does not define what pathogens are present, or define the sources of these bacteria. Microbial source tracking (MST) methods that have the ability to differentiate among sources of fecal pollution are currently under development. These methods will ultimately be useful for risk assessment purposes and to aid regulatory agencies in developing strategies to remediate microbiologically impaired waterways.     

苯并(a)芘对大弹涂鱼(Boleophthalmus pectinirostris)卵巢还原型谷胱甘肽含量的影响

分析了大弹涂鱼肌肉、鳃、肝脏、内脏 (不含肝脏 )以及卵巢等的GSH含量 ;并以GSH含量最高的卵巢为研究对象 ,在实验条件下 ,经 0 (CK) ,0 .0 5 ,0 .2和 0 .5mg/L等不同浓度的BaP暴露 7d ,分析其卵巢GSH含量变化的时间 -效应和剂量 -效应特征 ,结果显示 :0 .5mg/L浓度组的大弹涂鱼卵巢GSH含量迅速升高 ,暴露 12h即显著高于CK(P≤ 0 .0 5 ) ,但随暴露时间的延长 ,其GSH含量显著降低 ,7d的样品显著低于CK(P≤ 0 .0 5 ) ;在暴露 3d ,GSH水平与BaP浓度的剂量 -效应关系表现为正相关 ,而在 7d ,则呈负相关 ,这可能表明大弹涂鱼卵巢对BaP暴露由适应性反应到产生毒性效应的过程 .以上研究结果表明 ,卵巢GSH可对BaP暴露作出快速灵敏的反应 ,GSH水平有可能作为具氧化 -还原循环活性的污染物暴露的一种敏感的生物标记 .图 2表 2参 9     

环境管理、规划管理与项目管理

文章从深入分析环境管理的内涵出发,进而提出树立项目管理意识,强化项目管理的概念,说明项目管理在环境管理中的地位和作用,从这个意义上讨论环境管理与项目管理的关系,简述环境保护项目管理的主要环节,达到提高环境管理效能的途径的目的。     

湖北农村降水中SO_4~(2-)浓度变化研究

在湖北农村 10个地点 ,利用澳大利亚集雨器自 1996年 1月至 1998年 6月 ,按季度采集大气降水样品测定SO2 - 4浓度 ,并对数据进行统计分析。研究结果表明 ,各地 1997年降水中SO2 - 4浓度年均值比 1996年显著升高 ;大多数地点 1996、1997、1998年 1季度和 2季度降水中SO2 - 4浓度呈逐年升高趋势 ;大多数地点每年 1、4季度降水中SO2 - 4浓度高 ,2、3季度降水中SO2 - 4浓度低 ,说明湖北农村降水中的硫对秋冬作物影响比对春夏作物影响大 ;湖北农村降水中SO2 - 4浓度近两年不仅有时间变化规律 ,而且同一季度内的地区差异也很明显 ,在 1996年和 1997年 8个季度 10个点的降水SO2 - 4浓度最大值中 ,有 4个最大值出现在襄樊 ,它是目前湖北继宜昌市区、恩施市区之后又一个酸雨发展较快的地区     

石墨相氮化碳协同UV-H_2O_2光催化降解亚甲基蓝

以三聚氰胺为前驱体,经热解—回流法制备了石墨相氮化碳(g-C3N4),采用XRD、FTIR、SEM、EDS、PL等技术对g-C_3N_4进行了表征。研究了g-C_3N_4在UV-H_2O_2体系中对废水中亚甲基蓝(MB)的光降解效果。实验结果表明,UV+g-C_3N_4催化剂+H_2O_2体系能协同降解MB,在初始MB质量浓度为20 mg/L、初始废水p H为5、废水体积为250 mL、g-C_3N_4加入量为0.10 g、H_2O_2浓度为0.4 mmol/L、反应温度为25℃的优化工艺条件下,紫外光照射70 min时MB脱色率达98.32%。g-C_3N_4催化剂具有较好的重复使用性能,使用5次后MB脱色率仍保持在95.10%。     

Combination of biochar amendment and phytoremediation for hydrocarbon removal in petroleum-contaminated soil

Remediation of soils contaminated with petroleum is a challenging task. Four different bioremediation strategies, including natural attenuation, biochar amendment, phytoremediation with ryegrass, and a combination of biochar and ryegrass, were investigated with greenhouse pot experiments over a 90-day period. The results showed that planting ryegrass in soil can significantly improve the removal rate of total petroleum hydrocarbons (TPHs) and the number of microorganisms. Within TPHs, the removal rate of total n-alkanes (45.83 %) was higher than that of polycyclic aromatic hydrocarbons (30.34 %). The amendment of biochar did not result in significant improvement of TPH removal. In contrast, it showed a clear negative impact on the growth of ryegrass and the removal of TPHs by ryegrass. The removal rate of TPHs was significantly lower after the amendment of biochar. The results indicated that planting ryegrass is an effective remediation strategy, while the amendment of biochar may not be suitable for the phytoremediation of soil contaminated with petroleum hydrocarbons.     

三峡库区重庆段土壤保持服务时空分布格局研究

土壤保持是生态系统服务与功能的重要组成,在防止土壤侵蚀、减少径流泥沙与农业面源污染等方面具有至关重要的作用。以对国家生态安全具有重要作用的土壤保持生态功能区——三峡库区重庆段为研究区域,研究得到了2000~2013年时间序列区域土壤保持服务"流量"结果,结果表明:(1)三峡库区重庆段多年平均土壤保持量为604.39 t/hm~2·a,沿长江干流自西向东逐渐增强,区域差异显著;(2)三峡库区的土壤保持服务存在明显的垂直分异特征,随着高程的增加,以300 m与900 m为节点,出现递减-递增-递减的分段规律,与人类活动存在明显的相关关系;(3)增加森林覆被面积是改善区域土壤保持、减少水土流失的重要举措。同时,在三峡库区开展坡改梯工程,减少坡耕地的数量能够有效控制区域水土流失;     

Fe~(3+)和Cu~(2+)对饮用水氯消毒副产物三卤甲烷形成的影响

为了研究水中存在Br-的情况下,Fe3+和Cu2+对三卤甲烷(THMs)的生成及CHCl3、CHBr Cl2、CHBr2Cl、CHBr34种消毒副产物相对分布的影响,以腐殖酸模拟氯消毒过程中的前体物进行实验。结果表明,在p H为6、7和9 3种条件下,Fe3+抑制了THMs的生成,p H=6时只有CHCl3生成量随着Fe3+浓度的增加逐渐减少,其余3种消毒副产物均在增加,p H=7时4种消毒副产物浓度均减小并在Fe3+浓度为2 mg/L时生成量最低,p H=9时的生成趋势与p H=6时类似。Cu2+能促进THMs的生成,在p H为6、7和9时,当加入0.5 mg/L Cu2+时,THMs总量分别增加了16.7%、22.6%和2.5%,随着p H增加,THMs总量增加。在3种p H环境中,Cu2+对THMs生成的影响大于Fe3+,在偏酸性环境中,Fe3+影响THMs生成,产生的致癌风险高,当金属离子浓度为2.5 mg/L时,致癌风险相差最高为15%,在中性和偏碱性环境中,Cu2+影响THMs生成,产生的致癌风险高。