我国北方典型城市大气中VOCs的组成及分布特征

从2008年4月到2009年1月,利用前级浓缩-气相色谱/质谱法,对天津市和沈阳市大气中的挥发性有机物及浓度变化进行了采样研究.共监测了108种VOCs,包括卤代烷烃39种、苯系物16种、烯烃12种、烷烃30种、醛酯11种,在天津市检测到挥发性有机污染物中,醛酯56.9%,卤代烷烃13.4%,烷烃13.1%,苯系物12.9%,烯烃2.5%,卤代烯烃1.1%.沈阳市醛酯49.3%,卤代烷烃17.8%,烷烃11.8%,苯系物10.3%,卤代烯烃7.8%,烯烃2.9%.2市VOCs的含量季节变化都是春秋季节大于冬夏季节,在不同季节不同点位的VOCs的总量的变化趋势几乎一致,并且分析了天津市和沈阳市苯系物和卤代烃的的主要组成成分以及主要来源,苯系物的主要成分包括苯、甲苯、乙苯、二甲苯,苯系物的主要来源是汽车尾气,卤代烷烃的主要成分是二氯甲烷和氯乙烯,主要来自于汽车尾气和石油化工.     

A review of polybrominated diphenyl ethers and alternative brominated flame retardants in wildlife from China: Levels, trends, and bioaccumulation characteristics

Accelerated industrialization and urbanization, and unregulated disposal of waste of electric and electronic equipment (e-waste) in China have caused environmental pollution of brominated flame retardants (BFRs). This review summarized the levels, trends, and bioaccumulation characteristics of polybrominated diphenyl ethers (PBDEs) and other potential alternative BFRs including hexabromocyclododecanes (HBCDs), 1,2-bis(2,4,6-dibromophenoxy) ethane (BTBPE) and decabromodiphenylethane (DBDPE) in wildlife from China. PBDE levels in wildlife from China were generally higher than those from other parts in Asia, and were comparable to those from Europe but were lower than those from North America. However, wildlife from the e-waste recycling sites in South China and East China contained much higher PBDEs compared to other reports around the world, suggesting the heavy contamination of PBDEs in these regions. The alternative BFRs were also detected in wildlife, revealing that the animals are exposed to these chemicals, in addition to PBDEs. Temporal trends indicated by levels in marine mammals from South China suggested that PBDE levels increased from the beginning of 1990s to 2000s, but decreased from the middle of 2000s, followed by relatively steady levels. In contrast, HBCDs were found to be continuously increasing from 1997 to 2007, indicating the increasing usage of HBCDs in China in recent years. Compared to PBDE profiles found in other parts, aquatic species and birds from China contained relatively higher contributions of BDE-28 and 209, respectively, suggesting the possible different usage pattern of PBDEs. Future works including keeping monitoring at a reasonable scale and frequency to make sure levels near urban centers indicative of population do not increase are needed. Additionally, focus effort on e-waste recycling regions to look for impacts and to determine if regulation/controls are resulting in lower environmental contamination, and incorporation of sentinel species in monitoring efforts are recommended.     

Operating condition influences on PCDD/Fs emissions from sinter pot tests with hot flue gas recycling

This study was designed to clarify the influence of operating conditions on the formation and emissions of polychlorinated-pdibenzodioxins and dibenzofurans (PCDD/Fs) from a sintering process with hot flue gas recycling. A pilot scale sinter pot with simulated flue gas recycling was developed, and four key operational parameters, including temperature, oxygen content of the simulated waste flue gas, the coke rate of the sintering mixture, and the quicklime quality, were selected for exploring PCDD/Fs formation. The results showed that the temperature of the recycled flue gas had a major affect on PCDD/Fs formation, and a high temperature could significantly increase their formation during sintering. A clear linear correlation between the temperature of recycling flue gas and PCDD/Fs emission (r = 0.93) was found. PCDD/Fs could be reduced to a certain extent by decreasing the level of oxygen in the recycled flue gas, while sintering quality was unchanged. The coke rate had no significant influence on the formation of PCDD/Fs, but the quality of quicklime used in the sintering mixture could affect not only the amount of PCDD/Fs emissions but also the sintering productivity. Compared with a benchmark sinter pot test, PCDD/Fs emissions markedly decreased with improvements to quicklime quality. However, the reduction in PCDD/Fs emissions realized by using high-quality quicklime was limited by the temperature of the inlet gas. The highest reduction achieved was 51% compared with conventional quicklime when the temperature of the inlet gas was 150°C.     

Characterizing the optimal operation of photocatalytic degradation of BDE-209 by nano-sized TiO2

Brominated flame retardants have been widely used in industry. There is a rapid growing public concern for their availabilities in the environment. Advanced oxidation process (AOP) is a promising and efficient technology which may be used to remove emerging chemicals such as brominated flame retardants. This project aims at investigating optimal operational conditions for the removal of BDE-209 using nano-scaled titanium(IV) oxide. The residual PBDE congeners after photocatalytical degradation of BDE-209 by TiO₂ were analysed by gas chromatography-mass spectrometry (GC-MS). It was found that the degradability of BDE-209 by TiO₂ was attributed to its photocatalytic activity but not the small size of the particles. The half-life of removing BDE-209 by TiO₂ was 3.05 days under visible light. Tetra- and penta-BDEs were the major degraded products of BDE-209. Optimum conditions for photocatalytical degradation of BDE-209 was found to be at pH 12 (93% ± 1%), 5, 10, 20 mg/L (93.0% ± 1.70%, 91.6% ± 3.21%, 91.9% ± 0.952%, respectively), respectively of humic acid and in the form of anatase/rutile TiO₂ (82% ± 3%). Hence, the efficiency of removing BDE-209 can be maximized while being cost effective at the said operating conditions.     

Occurrence of selected aliphatic amines in source water of major cities in China

The formation of toxic nitrogenous disinfection byproducts (N-DBPs), such as nitrosamines, halonitromethanes and haloacetonitriles, from reactions between chlorine/chloramine and dissolved organic nitrogen in drinking water has caused great concern with regarding public health. This study revealed the occurrence of 17 aliphatic amines, some of which have been confirmed to be the precursors of N-DBPs, in source water across China. A sensitive method based on benzenesulfonyl chloride derivatization and liquid-liquid extraction followed by GC-MS analysis was established for the simultaneous analysis of the selected amines in aqueous samples. In total, 37 source water samples from the capital cities of 20 provinces were collected for the survey. Among the 17 amines, 14 were detected with an average frequency of detection of 36%. The most relevant amines in terms of frequency and maximum concentrations detected were dimethylamine (100%, 24.82 μg/L), methylamine (78%, 0.92 μg/L), N-methylethylamine (70%, 8.84 μg/L), propylamine (59%, 10.69 μg/L), diethylamine (54%, 3.76 μg/L), N-methylbutylamine (35%, 3.07 μg/L), N-ethylpropylamine (35%, 0.52 μg/L), and piperidine (32%, 2.35 μg/L). This is the first large scale survey of the aliphatic amines occurrence in source water in the world. The wide presence of nitrosamine precursors like dimethylamine, N-methylethylamine and diethylamine, and the precursors of haloacetonitriles and halonitromethanes like methylamine and propylamine suggests that better source water management is required to ensure the safety of drinking water.     

Pb2+对城市污水处理厂污泥中苏云金芽孢杆菌发酵的影响

以城市污水处理厂污泥为培养基,研究了添加Pb2+对Bt(Bacillus thuringiensis,苏云金芽孢杆菌)生长和晶体蛋白合成的影响,同时分析了Bt发酵过程中有效态Pb含量(以ρ计)的变化,并采用FTIR(傅立叶红外光谱)和XPS(X射线光电子能谱),初步探讨了Pb2+在Bt表面的作用机制.结果表明:污泥培养基在支持Bt生长代谢和降低重金属有效态含量方面均优于商用培养基,当初始ρ(Pb2+)高达400 mg/L时,与未添加Pb2+相比,污泥培养基中Bt活菌数与晶体蛋白产量约分别下降48%和54%,而商用培养基中约分别下降82%和75%,证实了污泥作为Bt发酵培养基的可行性;Bt对Pb2+有较好的耐受性,当ρ(有效态Pb)在80 mg/L以下时,Bt生长代谢不会受到显著影响.光谱学分析表明,Bt对Pb2+有少量吸附,从而降低Bt发酵过程中Pb的生物有效性,吸附位点主要为羟基,部分C O和S O也参与了吸附反应.     

某危险废物填埋场地下水污染预测及控制模拟

以某危险废物填埋场为研究对象,在收集其水文地质资料基础上,运用Visual Modflow建立填埋场地下水水流和溶质运移耦合模型,对填埋场防渗层发生渗漏后,渗滤液中Cr6+在地下水中的运移过程以及地面硬化、防渗墙和排水沟3种污染控制措施对污染羽阻隔效果进行模拟预测.结果表明,Cr6+随地下水流方向运移形成污染羽,10 a后污染羽到达水塘边界,运移距离约为1 450 m,但随后10～20 a之间污染羽扩散范围没有明显扩大;地表硬化后,20 a内污染羽未扩散至水塘边界;防渗墙设置到上层含水层底部时,监测井Cr6+浓度高于未设置防渗墙时浓度,设置到下层含水层底部时,Cr6+浓度与设置于上层含水层时监测结果相反;排水沟日排水量达到2 642 m3时能有效控制污染羽扩散,20 a后污染羽尚未污染监测井;地表硬化与排水沟组合控制污染物扩散,效果最佳,同时排水沟日排水量可减少为1 878 m3.因此,当填埋场发生渗漏时,建议采用设置排水沟与周边地表硬化组合的地下水污染控制措施.     

全国大气扩散输送模态与区划研究

基于NCEP再分析气象资料,使用HYSPLIT模式对我国大陆区域进行了一整年的连续轨迹计算.轨迹以1°×1°的网格化经纬度分辨率进行计算.考虑气候、地理及经济因素,将全国计算区域分为10个大区,分别统计各大区出发的轨迹在全国的分布频率.根据全年和各季的轨迹统计结果,分析我国不同区域的大气输送扩散特征以及区域间大气环境的相互影响潜势.结果表明,全国10个大区的大气扩散输送模态可分为特性不同的7大类,其中以西北方向的3个大区为一类,西南高原的2个大区为另一类,其它各区自成一类.10个大区大气扩散物质的累积效应差异显著且季节变化特征各异.全国以西南区(XN)东部大气累积效应最强,东北区(DB)累积效应最弱.     

近17年鄱阳湖区生态系统健康时空变化研究

以遥感影像和社会统计数据为基础,构建基于压力-状态-响应(P-S-R)概念模型的鄱阳湖区生态系统健康评价指标体系,并建立湖区生态系统健康评价模型,通过对生态系统健康指数的计算与分析,揭示鄱阳湖区生态系统健康的时空变化特征.研究结果表明,在人类生产活动的影响下,近17年鄱阳湖区生态系统结构渐趋不合理,生态系统功能有所减弱,虽然湖区生态系统健康总体处于一般水平,但人类活动干扰的不断加强,导致湖区生态系统健康正逐步向着恶化方向发展.湖区生态系统健康在空间分布上呈现出南北分异的特点,南部工业化、城镇化水平较高的地区生态系统健康状况较差,经济发展水平较低的北部地区,生态系统健康状况则相对较好.     

长白山温带森林挥发性有机物的排放通量

2010年夏季,在长白山温带森林开展了挥发性有机物(VOC)排放通量以及气象参数、PAR的综合测量.VOC排放通量采用松弛涡度积累(RelaxedEddyAccumulation)技术在森林冠层上进行测量.初步发现长白山阔叶林主要排放α-蒎烯、β-蒎烯、莰烯、香桧烯、月桂烯、蒈烯、柠檬烯、罗勒烯、松油烯、繖花烃、萜品油烯、三环烯等.研究表明,长白山阔叶混交林VOC排放有明显的日变化——早晚较低和中午前后较高.2010年夏季,单萜烯总排放通量的平均值为0.242mg·m·h-2-1,其变化范围为0.005～1.668mg·m·h-2-1;各成分排放通量的平均值(和最大值)分别为α-蒎烯0.072(0.234)、莰烯0.028(0.356)、月桂烯0.027(0.433)、蒈烯0.023(0.173)、柠檬烯0.037(0.197)、罗勒烯0.016(0.168)、萜品油烯0.053(0.320)、繖花烃0.067(0.755)mg·m·h-2-1.研究还发现VOC排放通量与气温之间存在一定的联系.