奥运期间北京交通环境细颗粒物中多环芳烃特征研究

采用GC/MS测定了奥运空气质量保障措施实施期间(2008年8月)及非奥运时段(2008年6月、2009年8月)北京市北四环道路边PM2.5中12种优控PAHs含量,并应用特征化合物比值法对PAHs来源进行了识别.研究表明,奥运空气质量保障措施实施期问PAHs总浓度平均为4.77 ng·m-3,较非奥运时段下降了59%...     

接种混合功能细菌降低黑麦草体内菲和芘污染的机理初探

本研究通过批量降解试验,探讨了功能菌株Massilia sp. Pn2和Mycobacterium flavescens 033降解菲和芘的基本动力学过程和规律;重点采用温室盆栽试验,研究了接种混合菌株对黑麦草体内PAHs含量及多酚氧化酶(PPO)和过氧化物酶(POD)活性的影响.结果表明,菌株Pn2和033可以分别利用菲和芘作为碳源和能源进行生长;在30℃、pH=7.0条件下,菌株Pn2和033对100 mg·L~(-1)菲和50 mg·L~(-1)芘的降解率分别高达99.7%和98.3%,降解半衰期分别为0.34 d和0.95 d(R~20.98).与接种灭活混合菌株对比,接种混合菌株Pn2和033显著地降低了黑麦草体内菲和芘的含量和积累量(p0.05),并阻控菲和芘由黑麦草根向茎叶转移.同时,接种混合菌株Pn2和033显著地提高了黑麦草根和茎叶中POD(p0.05)活性,该酶能够促进黑麦草体内超氧自由基的清除,并保护细胞免受PAHs损伤,进而影响PAHs在黑麦草体内的代谢过程.研究结果为阐明接种混合功能菌降低植物体内PAHs污染的作用机理提供了一定的参考价值.     

Microbial community changes in aquifer sediment microcosm for anaerobic anthracene biodegradation under methanogenic condition

The widespread distribution of polycyclic aromatic hydrocarbons (PAHs) in groundwater has become an important environmental issue. Knowledge of microbial community changes could aid in identification of particular microorganisms that are capable of degrading PAHs in contaminated aquifers. Therefore, 16S rRNA gene clone library analysis was used to identify the archaeal and bacterial communities in an aquifer sediment microcosm used for anaerobic anthracene degradation under methanogenic conditions. A remarkable shift of the archaeal community structure occurred after anaerobic anthracene degradation, but the types of the abundant bacterial phyla did not change. However, a decrease of both archaeal and bacterial diversity was observed. Bacterial genera Bacillus, Rhodococcus and Herbaspirillum might have links with anaerobic anthracene degradation, suggesting a role of microbial consortia. This work might add some new information for understanding the mechanism of PAH degradation under methanogenic conditions.     

不同接种物对富集反硝化型甲烷厌氧氧化微生物的影响

在厌氧条件下,反硝化型甲烷厌氧氧化过程(Denitrifying anaerobic methane oxidation,DAMO)以CH_4为电子供体,以NO_3~-或NO_2~-作为电子受体,可同时实现甲烷氧化和废水中脱氮.本文利用两种电子受体(NO_3~-、NO_2~-)及不同接种污泥成功富集了4种DAMO培养物,研究了不同接种物对富集DAMO微生物的影响.结果表明,NO_3~-对富集DAMO古菌具有重要作用,而NO_2~-则对DAMO细菌的富集过程有较大影响.其次,在富集培养过程中,NH_4~+的存在会获得厌氧氨氧化(Anaerobic ammonium oxidation,Anammox)细菌与DAMO古菌的混培物,并形成协同关系,而DAMO细菌却因与Anammox细菌竞争而被淘汰.当NH_4~+不再加入,NO_3~-成为唯一氮源时,DAMO细菌重新出现并与DAMO古菌形成一种新的协同关系.此外,以淡水河道底泥、淡水湖泊底泥及水稻田土壤的混合物作为接种污泥而得到的DAMO富集培养物,其脱氮速率比以淡水河道底泥、活性污泥及厌氧消化污泥的混合物作为接种污泥的富集培养物高出3.3倍,但后者在驯化时间上缩短了36%.     

澳门南湾湖钻孔沉积物中自由态和束缚态的多环芳烃

研究自然条件下沉积物中有机污染物沉积后的环境行为,考察澳门南湾湖钻孔沉积物中自由态和束缚态PAHs的含量与分布.研究表明,自由态PAHs以4-环、6,7-环和5-环为主,其质量百分贡献分别为28.7%～40.6%、17.6%～29.6%和13.2%～28.2%;而束缚态PAHs则以4-环、3-环和2-环为主,质量百分贡献分别为42.3%～55.8%、20.2%～35.8%和7.8%～18.8%.说明低分子量PAHs比高分子量PAHs更容易进入沉积有机质的孔隙中.自由态PAHs的垂直分布特征受区域经济发展及环境治理进程的影响,束缚态PAHs的含量一方面受控于PAHs的输入量,另一方面与沉积有机质的结构(特别是聚合程度)有关,随着沉积埋藏时间的延长有利于各化合物从自由态向束缚态转变.     

洛阳市秋冬季PM2.5中多环芳烃的污染特征、来源解析及健康风险评价

本研究于2018年10月4日至2019年1月30日在洛阳市高新和林校2个采样点位同步连续采集秋冬季PM_2.5样品,使用气相色谱-质谱联用仪（GC-MS）对PM_2.5中优先控制的16种多环芳烃（polycyclic aromatic hydrocarbons,PAHs）进行了分析测定.对优良天和污染天PM_2.5中16种PAHs的质量浓度和组成分布特征进行了研究,利用特征比值法和主成分分析法对其主要来源进行了定性解析,并使用苯并［a］芘（BaP）毒性当量法和增量终生致癌风险模型评估了对人体的健康风险.结果表明在采样期内,高新和林校两个采样点的PM_2.5中16种PAHs质量浓度变化范围分别为24.33~90.26 ng·m^-3和23.81~76.99 ng·m^-3.随着PM_2.5污染程度的加重,PAHs浓度明显升高（污染天为优良天的1.3倍）,不同环数PAHs贡献顺序均为：4环（43%~48%） > 5~6环（32%~35%） > 2~3环（20%~22%）.大气中PAHs主要来自于燃烧源,包括燃煤、生物质燃烧以及机动车排放等,其中燃煤对PAHs污染贡献最大（优良天：49.28%~56.38%,污染天：49.44%~60.60%）.BaP毒性当量浓度表明,污染天存在更高的人体健康风险;增量终生致癌风险结果表明,污染天致癌风险高于优良天,成人呼吸暴露风险高于儿童,在研究区域内不同污染水平下健康风险属于可接受水平（<1×10^-6）.     

固相微萃取模拟生物法用于养殖底泥多环芳烃污染监测的研究

本研究以养殖底泥中多环芳烃(PAHs)为研究对象,采用以聚二甲基硅氧烷(PDMS)为材料测定孔隙水中PAHs自由溶解态浓度(Cfree)的固相微萃取技术,以重要海水经济底栖生物菲律宾蛤仔(Ruditapes philippinarum)为参照生物,建立了PDMS中PAHs浓度与菲律宾蛤仔脂肪标化及底泥有机碳标化的PAHs浓度间的定量关系模型,进一步证明了基于固相微萃取的模拟生物法用于养殖区域中多环芳烃监测的可能性.结果表明,孔隙水中自由溶解态PAHs浓度(Cfree)显著低于孔隙水中总PAHs浓度(Cwater),且随着环数增加,两者间的差异越大,说明Cwater忽视了生物有效性,从而会高估孔隙水中PAHs的环境风险,因此,Cfree能更好地反映底泥孔隙水中PAHs的暴露水平;菲律宾蛤仔对PAHs的富集系数(BAF)及PDMS-水分配系数(KPDMS)均与辛醇-水分配系数(Kow)呈显著线性相关,且两者斜率相近,说明菲律宾蛤仔摄取PAHs的主要途径与PDMS相似,且PDMS中PAHs的浓度与生物体内PAHs的残留浓度和底泥有机碳标化的PAHs浓度间均呈现显著相关,说明当底泥孔隙水中和PDMS膜之间达到平衡时,固相微萃取模拟生物法可以用于计算底栖生物和沉积物中有机污染物,具有应用于养殖区域中多环芳烃监测的潜力,但有机污染物在生物体内转化和底泥性质对相关关系和监测应用的影响有待进一步研究.     

河北与京津地区非采暖期大气中的PAHs污染特征

对河北与京津地区42个样点非采暖期大气中多环芳烃(Polycyclic Aromatic Hydrocarbons,PAHs)的研究表明,该区域大气中的PAHs浓度水平较高.2～3环PAHs主要分布在气相当中,颗粒相(大气可吸入颗粒物,PM10)中PAHs以4～6环为主.PAHs的高浓度样点在石家庄、唐山和邯郸地区分布最为集中.县城样点与城市样点的PM10和PAHs污染水平相近.临近区域广泛存在的大气污染很可能对北京市的大气环境造成影响.     

Emission factors of polycyclic aromatic hydrocarbons from domestic coal combustion in China

Domestic coal stove is widely used in China, especially for countryside during heating period of winter, and polycyclic aromatic hydrocarbons （PAHs） are important in flue gas of the stove. By using dilution tunnel system, samples of both gaseous and particulate phases from domestic coal combustion were collected and 18 PAH species were analyzed by GC-MS. The average emission factors of total 18 PAH species was 171.73 mg/kg, ranging from 140.75 to 229.11 mg/kg for bituminous coals, while was 93.98 mg/kg, ranging from 58.48 to 129.47 mg/kg for anthracite coals. PAHs in gaseous phases occupied 95% of the total of PAHs emission of coal combustion. In particulate phase, 3-ring and 4- ring PAHs were the main components, accounting for 80% of the total particulate PAHs. The total toxicity potency evaluated by benzo[a]pyrene-equivalent carcinogenic power, sum of 7 carcinogenic PAH components and 2,3,7,8-tetrachlorodibenzodioxin had a similar tendency. And as a result, the toxic potential of bituminous coal was higher than that of anthracite coal. Efficient emission control should be conducted to reduce PAH emissions in order to protect ecosystem and human health.     

常州市大气PM2.5中PAHs污染特征及来源解析

2016年1~8月期间,在常州市采集到55个大气细颗粒物PM_(2.5)样品,采用气相色谱-质谱联用仪测定其中17种PAHs的含量.结果表明,冬、春、夏季PAHs的季均浓度分别为140.24、41.42和2.96 ng·m~(-3),冬季污染较严重,且以4~6环中高分子量化合物为主.Ba P日均浓度平均值3.64 ng·m~(-3),超标日占总采样天数的41%.PAHs浓度与气温(相关系数-0.643)和能见度(相关系数-0.466)显著负相关,与大气压呈显著正相关(相关系数0.544),而与风速、相对湿度相关性较差.受昼夜温差、大气层结和污染源变化等因素影响,夜间PAHs浓度高于白天.气团后向轨迹模型分析表明,常州PM_(2.5)中PAHs主要受当地排放源和短距离传输的影响,长距离传输影响小(仅占11%).特征比值法分析发现,PAHs主要来源于燃煤、机动车尾气和生物质燃烧.利用超额终生致癌风险(ILCR)模型评估PAHs通过呼吸暴露途径对人体健康的影响,结果表明:成人的ILCR值高于儿童,冬季和春季人群的ILCR值略高于风险阈值,夏季则不明显.     

Universally improving effect of mixed electron donors on the CO2 fixing efficiency of nonphotosynthetic microbial communities from marine environments

The universality of improved CO2 fixing upon the addition of mixed electron donors（MEDs）composed of Na2 S,NO2-,and S2O32-to non-photosynthetic microbial communities（NPMCs）obtained from 12 locations in four oceans of the world was validated. The CO2 fixing efficiencies of NPMCs were universally enhanced by MED compared with those obtained using H2 alone as electron donor,with average increase of about 276%. An increase in microbial inoculation concentration could increase the net amount of CO2 fixing to853.34 mg/L in the presence of MED. NO2-and S2O32-may play the roles of both electron acceptor and electron donor under aerobic conditions,which may improve the energy utilization efficiency of NPMC and enhance the CO2 fixation efficiency. The sequence determination of 16 S ribosomal deoxyribonucleic acid（rDNA） from 150 bacteria of NPMC showed that more than 50% of the bacteria were symbiotic and there were many heterotrophic bacteria such as Vibrio natriegens. These results indicate that NPMC acts as a symbiotic CO2 fixing system. The interaction between autotrophic and heterotrophic bacteria may be a crucial factor supporting ladder utilization and recycling of energy/carbon source.     

长江水系武汉段沉积物再悬浮过程中PAHs的释放动力学

采用沉积物再悬浮模拟装置进行了再悬浮过程中多环芳烃（PAHs）的释放动力学实验,研究了长江水系武汉段7种沉积物中PAHs的释放动力学特征,并考察了沉积物组成对PAHs释放动力学的影响.结果表明,不同剪应力作用下的沉积物再悬浮过程中,不同性质沉积物中PAHs向上覆水体的释放均符合一级动力学方程,且释放过程分为两个阶段,第...     

二级热脱附结合气相色谱-质谱联用分析大气细颗粒物中多环芳烃类污染物

化学组分是影响大气细颗粒物(即PM_(2.5))健康危害的重要因素,但目前流行病学研究对于颗粒物组分的暴露评价受到了传统分析方法的限制.为探索高效的颗粒物组分测定方法,本研究建立并优化了二级热脱附结合气相色谱-质谱联用(TD-GC-MS)方法,以多环芳烃(PAHs)为目标污染物开展研究.结果表明,该方法具有极高的灵敏度,当使用0.28 m~3PM_(2.5)样品时,该方法的检出限为0.018~0.26 ng·m~(-3).对于标准参考物质的测量显示,该方法具有较好的准确性和精密度.同时,分析了北京2012年3月—2013年3月PM_(2.5)样品并与索氏提取结果进行对比,发现两种方法测量3~5环PAHs的一致性较好;部分物种的差异较大,热脱附因减少前处理步骤,结果可能更为准确.北京PM_(2.5)中∑_(12)PAHs浓度为4.27~340 ng·m~(-3),采暖季比非采暖季高一个数量级.基于正矩阵因子分解法(PMF)的源解析显示,燃煤是采暖季的主要污染源,非采暖季则为交通排放.最后,估算了成年北京居民暴露于PAHs的终生致癌风险,结果表明,可重点控制交通源及煤炭源以降低其潜在危害.     

Comparison of polycyclic aromatic hydrocarbon pollution in Chinese and Japanese residential air

Comparative studies on polycyclic aromatic hydrocarbon (PAH) pollution in residential air of Hangzhou (China) and Shizuoka (Japan) were conducted in summer (August, 2006) and winter (January, 2007). Total concentrations of 8 PAHs ranged from 7.1 to 320 ng/m³ and 0.15 to 35 ng/m³ in residential air of Hangzhou and Shizuoka, respectively. Air PAH concentrations in smoking houses were higher than that in nonsmoking houses. In nonsmoking houses, mothball emission and cooking practice were the emission sources of 2- and 3-ring PAHs in Hangzhou, respectively. The 2- and 3-ring PAHs were from use of insect repellent, kerosene heating and outdoor environment in nonsmoking houses in Shizuoka. The 5- and 6-ring PAHs in residential air were mainly from outdoor environment in both cities. Toxicity potencies of PAHs in residential air of Hangzhou were much higher than that in Shizuoka.     

深圳湾生态系统多环芳烃（PAHs）特征及其生态危害

2004年在深圳湾海域采集海水、悬浮物、表层沉积物和柱状沉积物样品,并分析其中15种多环芳烃的含量及其相关参数,同时采用210Pb法测定柱状沉积物的年龄.结果表明,海水、悬浮物、表层沉积物和柱状沉积物中总的PAHs含量分别为(69.4±24.7)ng·L-1、(429.1±231.8)ng·g-1、(353.8±128.1)ng·g-1和(321.1±134.6)ng·g-1,各介质优势组分均为菲、荧蒽和芘;1948～2004年期间,深圳湾柱状沉积物中PAH各单体的浓度总体上一直在增加,PAHs的平均沉积通量为89.9ng/(cm2·a);PAH各单体在沉积物/海水中的分配系数(Koc)与其相应的辛醇/水比(Kow)存在明显的正相关性,即可用PAH的Kow值来预测深圳湾海域PAH的Koc.目前,水体与沉积物中PAH含量对该海域的水生生物尚未构成威胁.     

松针生理性质对其富集多环芳烃行为的影响

测定了雪松(Cedrus deodar)和黑松(Pinus thunbergii)松针的脂含量、气孔密度和比表面积等生理性质及松针中多环芳烃 (PAHs)浓度,考察了松针生理性质对其富集PAHs行为的影响.结果表明,雪松松针中PAHs浓度高于黑松,其平均总浓度(ΣPAHs)分别为(1101±692)ng/g和(518±339)ng/g,2种松针对PAHs的富集能力有较大差异,脂含量是决定松针富集PAHs量的首要因素.2种松针中PAHs组成均以3环和4环PAHs为主,分别占ΣPAHs的56%和31%以上.松针对于3环PAHs的富集能力强于4环PAHs,两者浓度差异约为2倍左右;对于5、6环PAHs,未发现其浓度与脂含量之间的相关关系.由于雪松和黑松松针的脂含量随比表面积具有不同的变化趋势,2种松针中PAHs浓度随比表面积的变化趋势相反.对于5、6环PAHs,松针比表面积和气孔密度对其浓度有显著影响.     

混合电子供体对好氧非光合微生物菌群固碳效率影响的析因实验分析

通过混合电子供体析因实验,定量描述了Na2S、NaNO2、Na2S2O3 3种无机物的用量和比例与非光合微生物固碳量之间的关系,并分析了3种电子供体之间的两两交互作用.最后,通过16S rDNA V3区DGGE图谱分析,研究了不同混合电子供体对固碳微生物群落结构的影响.结果表明,电子供体析因实验的模型具有较好的拟合度,...     

Use of Fe/Al drinking water treatment residuals as amendments for enhancing the retention capacity of glyphosate in agricultural soils

Fe/Al drinking water treatment residuals (WTRs), ubiquitous and non-hazardous by-products of drinking water purification, are cost-effective adsorbents for glyphosate. Given that repeated glyphosate applications could significantly decrease glyphosate retention by soils and that the adsorbed glyphosate is potentially mobile, high sorption capacity and stability of glyphosate in agricultural soils are needed to prevent pollution of water by glyphosate. Therefore, we investigated the feasibility of reusing Fe/Al WTR as a soil amendment to enhance the retention capacity of glyphosate in two agricultural soils. The results of batch experiments showed that the Fe/Al WTR amendment significantly enhanced the glyphosate sorption capacity of both soils (p < 0.001). Up to 30% of the previously adsorbed glyphosate desorbed from the non-amended soils, and the Fe/Al WTR amendment effectively decreased the proportion of glyphosate desorbed. Fractionation analyses further demonstrated that glyphosate adsorbed to non-amended soils was primarily retained in the readily labile fraction (NaHCO₃-glyphosate). The WTR amendment significantly increased the relative proportion of the moderately labile fraction (HCl-glyphosate) and concomitantly reduced that of the NaHCO₃-glyphosate, hence reducing the potential for the release of soil-adsorbed glyphosate into the aqueous phase. Furthermore, Fe/Al WTR amendment minimized the inhibitory effect of increasing solution pH on glyphosate sorption by soils and mitigated the effects of increasing solution ionic strength. The present results indicate that Fe/Al WTR is suitable for use as a soil amendment to prevent glyphosate pollution of aquatic ecosystems by enhancing the glyphosate retention capacity in soils.     

滦河流域多环芳烃的污染特征、风险评价与来源辨析

在滦河上、中、下游和河口地区布设了15个采样点,对滦河流域的河水和表层沉积物中多环芳烃(PAHs)进行了分析.结果表明,水中PAHs总量为9.8～310ng.L-1,表层沉积物中PAHs总量最高达478ng.g-1.城市地区河段中PAHs的浓度高于农村河段中PAHs的浓度,河口地区相对中游地区污染较轻.就组成特征而言,水中PAHs以3环(40.9%)、4环(56.2%)为主,表层沉积物中PAHs以3环(30.0%)、4环(39.3%)、5环(15.8%)为主.总的来讲,3环、4环PAHs是滦河流域PAHs最主要的成分.地表水健康风险评价结果显示,韩家营、瀑河口两个采样点苯并[a]芘(BaP)毒性当量值(EBaP)分别为11.8、11.4ng.L-1,超出中国国家环境保护部(CEPA)制定的EBaP=2.8ng.L-1的国家标准,存在不利的健康风险.表层沉积物生态风险评价结果显示,韩家营、上板城、乌龙矶地区的PAHs可能存在着对生物的潜在危害,剩余研究区域不存在生态风险.滦河水和表层沉积物PAHs主要表现为以草、木柴和煤燃烧来源为主的特征,部分样点存在燃油与木柴、煤燃烧的混合来源特征.瀑河口、大黑汀受石油源污染影响明显.     

基于硝酸盐缓释-功能微生物协同的污染底泥原位修复技术研究

重污染底泥原位修复常需外加大量电子受体,但大量实践表明电子受体直接投加存在作用时效短、微生物利用效率低等问题.针对该问题,开发了电子受体缓释-功能微生物协同的复合环境功能材料,并探讨了功能材料对底泥原位修复效果.结果表明:①复合功能材料〔以Ca（NO₃）₂计,下同〕仅投加5.7 g/kg时,底泥中ORP（氧化还原电位）提升了60.17%~73.96%,AVS（酸可挥发性硫化物）去除率高达90%,是其他传统原位修复材料的1倍.②相较于单独投加Ca（NO₃）₂的修复方式,复合功能材料最大可去除上覆水中33.78%的ρ（TN）,而且ρ（NH₄+-N）也降低了27.90%.③复合功能材料同时促进上覆水中TP和COD_Cr的去除,其去除率分别在78%和30%以上.④从经济成本和对环境影响的角度出发,在工程应用上宜用电子受体:固定剂:促凝剂:发泡剂:塑形剂:复合微生物菌剂:水的质量比为1:5:0.5:0.5:0.1:1:1的复合功能材料.研究显示,硝酸盐缓释-功能微生物复合材料是一种高效的重污染底泥原位修复材料,能显著提升底泥和上覆水中污染物去除效率,降低ρ（NH₄+-N）、ρ（COD_Cr）,避免上覆水体受到二次污染.