基于车载测试的重型柴油车尾气典型烷烃排放特征

本文采用车载排放测试系统对11辆国Ⅰ~国Ⅳ标准重型柴油车进行实际道路测试,利用GC-MS对样品中典型烷烃进行定量分析,解析重型柴油车尾气典型烷烃排放特征及规律.结果表明,排放标准对重型柴油车尾气中正构烷烃、藿烷类有机物排放有显著影响,总体呈现随排放标准的加严而降低的趋势,相比于国Ⅰ测试车辆,国Ⅳ测试车辆正构烷烃、17α(H),21β(H)-C30藿烷(C30-藿烷)、22S-和22R-17α(H),21β(H)-C31升藿烷(22S-C31升藿烷;22R-C31升藿烷)总排放因子分别降低了72.23%,64.95%,70.78%和74.68%.气相正构烷烃呈双峰前锋型,以C17~C18为主峰碳,固相呈单峰前锋型,以C18~C21为主峰碳.藿烷类有机物其22S-C31升藿烷/(22S-C31升藿烷+22R-C31升藿烷)的比值在0.46~0.56之间,平均值为0.50,符合石油中藿烷的分布特征.正构烷烃总排放因子与17α(H),21β(H)-C30藿烷总排放因子呈现出一定的线性关系,其R~2为0.926 8.此外,行驶工况对测试车辆正构烷烃及藿烷类有机物排放有较大影响,非高速工况下排放因子是高速工况的1.69~2.42倍.     

西安市重污染与清洁天PM2.5组分及其活性氧物质对比

针对重霾污染,在西安市冬季重污染日(2015-11-30~2015-12-09)和清洁日(2016-01-13~2016-01-22)各进行了为期10d的PM_(2.5)采集,测量其中的有机碳、元素碳,及NH_4~+、NO_3~-、SO_4~(2-)等无机水溶性离子,探讨两种污染条件下的组分特征及其成因.结果表明:观测期,重霾日和清洁日PM_(2.5)质量浓度分别为(170±47.5)μg·m~(-3)和(48.6±17.9)μg·m~(-3),且重霾日伴随低能见度、高湿静风等多种不利气象条件;重霾日二次无机离子(NH_4~+、NO_3~-、SO_4~(2-))组分占PM_(2.5)质量浓度的49.8%±13.1%,而清洁日为19.4%±5.95%,并且重霾日硫氧化速率(sulfur oxidation ratio,SOR)和氮氧化速率(nitrogen oxidation ratio,NOR)分别为0.282±0.157和0.269±0.124,远高于清洁日(SOR和NOR分别为0.189±0.057和0.077±0.046),重霾日二次有机组分浓度[(6.22±3.87)μg·m~(-3)]是清洁日[(1.44±1.63)μg·m~(-3)]的5倍,表明二次污染及不利气象条件是造成重霾期间相关组分浓度升高的重要原因.最后,通过二氯荧光黄双乙酸盐(2',7'-DCFH)化学荧光分析法测定了其中活性氧物质(reactive oxygen species,ROS)的浓度,探讨其对于二次无机组分形成的影响,结果表明观测期ROS平均浓度(以H_2O_2计)分别为(4.99±1.54)nmol·m~(-3)(重霾期),(0.492±0.356)nmol·m~(-3)(清洁期),二次反应及积累效应可能是西安重霾条件下ROS浓度升高的主要原因.NO_3~-、SO_4~(2-)与ROS均呈现正相关(P0.05),表明ROS可能通过二次氧化过程参与到二次无机组分形成过程中.     

泉州市大气PM2.5镧系元素组成特征及来源解析

2014年3月、4月和7月分别采集了泉州市5个采样点共49个PM_(2.5)样品,采用电感耦合等离子体质谱(ICP-MS)测定样品镧系元素(Loid)及其他微量金属元素浓度水平.分析了PM_(2.5)镧系元素组成特征和配分模式,利用La-Ce-V三元图和化学质量平衡(CMB)受体模型解析了泉州市大气PM_(2.5)污染来源.结果表明:(1)泉州市大气PM_(2.5)总镧系元素(Σ Loid)浓度为2.490~5.708 ng·m~(-3)(含量65.682~126.529μg·g~(-1)),轻重镧系元素比值(L/H)为12.086~14.319;(2)PM_(2.5)镧系元素配分模式与福建土壤相似,PM_(2.5)中Ce元素表现为正异常,而Eu元素表现为负异常;(3)城市扬尘、燃煤尘、汽车尾气尘和垃圾焚烧飞灰是泉州市大气PM_(2.5)的主要来源,贡献率分别为18.9%、10.9%、30.6%和30.2%.     

Performance and microbial community of a membrane bioreactor system——Treating wastewater from ethanol fermentation of food waste

In this study, a lab-scale biological anaerobic/anaerobic/anoxic/membrane bioreactor(A_-~3MBR) was designed to treat wastewater from the ethanol fermentation of food waste,a promising way for the disposal of food waste and reclamation of resources. The 454 pyrosequencing technique was used to investigate the composition of the microbial community in the treatment system. The system yielded a stable effluent concentration of chemical oxygen demand(202 ± 23 mg/L), total nitrogen(62.1 ± 7.1 mg/L), ammonia(0.3 ±0.13 mg/L) and total phosphorus(8.3 ± 0.9 mg/L), and the reactors played different roles in specific pollutant removal. The exploration of the microbial community in the system revealed that:(1) the microbial diversity of anaerobic reactors A_1 and A_2, in which organic pollutants were massively degraded, was much higher than that in anoxic A_3 and aerobic MBR;(2) although the community composition in each reactor was quite different, bacteria assigned to the classes Clostridia, Bacteroidia, and Synergistia were important and common microorganisms for organic pollutant degradation in the anaerobic units, and bacteria from Alphaproteobacteria and Betaproteobacteria were the dominant microbial population in A_3 and MBR;(3) the taxon identification indicated that Arcobacter in the anaerobic reactors and Thauera in the anoxic reactor were two representative genera in the biological process. Our results proved that the biological A_-~3MBR process is an alternative technique for treating wastewater from food waste.     

Simultaneous removal of Cu(II) and Cr(VI) by Mg–Al–Cl layered double hydroxide and mechanism insight

Mg–Al–Cl layered double hydroxide (Cl-LDH) was prepared to simultaneously remove Cu(II) and Cr(VI) from aqueous solution. The coexisting Cu(II) (20 mg/L) and Cr(VI) (40 mg/L) were completely removed within 30 min by Cl-LDH in a dosage of 2.0 g/L; the removal rate of Cu(II) was accelerated in the presence of Cr(VI). Moreover, compared with the adsorption of single Cu(II) or Cr(VI), the adsorption capacities of Cl-LDH for Cu(II) and Cr(VI) can be improved by 81.05% and 49.56%, respectively, in the case of coexisting Cu(II) (200 mg/L) and Cr(VI) (400 mg/L). The affecting factors (such as solution initial pH, adsorbent dosage, and contact time) have been systematically investigated. Besides, the changes of pH values and the concentrations of Mg²⁺ and Al³⁺ in relevant solutions were monitored. To get the underlying mechanism, the Cl-LDH samples before and after adsorption were thoroughly characterized by X-ray powder diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. On the basis of these analyses, a possible mechanism was proposed. The coadsorption process involves anion exchange of Cr(VI) with Cl⁻ in Cl-LDH interlayer, isomorphic substitution of Mg²⁺ with Cu²⁺, formation of Cu₂Cl(OH)₃ precipitation, and the adsorption of Cr(VI) by Cu₂Cl(OH)₃. This work provides a new insight into simultaneous removal of heavy metal cations and anions from wastewater by Cl-LDH.     

Simulated reaction of formaldehyde and ambient atmospheric particulate matter using a chamber

The reaction of HCHO with Beijing winter's real ambient particulate matter(PM) inside a 3.3 m~3 Teflon Chamber was conducted in this study. NO_2, O_3 and H_2O gases were removed from the ambient aerosol before entering into the chamber. The decays of HCHO were monitored(acetylacetone spectrophotometry method) during the reactions at different PM number concentrations(N_a) and relative humidities(RHs), and the formed particulate formate was detected by IC and XPS techniques. The results showed that when RH was10%–15%, the decay rate of HCHO in the chamber was higher with the existence of PM from relatively clean days(with number concentration(N_a) 200,000 particle/L, 0.35–22.5 μm)compared to dirty days(N_a 200,000 particle/L, 0.35–22.5 μm). When RH increased to 30%–45%, PM can hardly have significant influences on the decay of HCHO. The formations of formate on the reacted PM were consistent with the HCHO decay rates at different ambient PM N_aand RH conditions. This is a first study related to the "real" ambient PM reacted with HCHO and suggested that in the clean and low RH days, PM could be an effective medium for the conversion of HCHO to formate.     

北京市郊区夏季臭氧重污染特征及生成效率

为研究北京郊区夏季O₃(臭氧)重污染过程特征及O₃生成的光化学敏感性,基于2016年夏季在北京郊区开展的针对O₃及其相关污染物的强化观测试验(7月23日—8月31日,共计40 d),分析了观测期间O₃浓度[以φ(O₃)计]变化特征、O₃重污染过程主控因素与O₃敏感性化学特征.结果表明:观测期间φ(O₃)超标时有发生,最大小时φ(O₃)为151.1×10-9,其中有15 d的φ(O₃)最大8 h滑动平均值(O₃-max-8h)超过了GB 3095—2012《环境空气质量标准》二级标准限值,占观测天数的37.5%;不同O₃重污染过程成因有所不同,城市烟羽传输的污染物对郊区O₃重污染过程影响显著(观测期间臭氧重污染过程:过程1,7月27—29日;过程3,8月9—11日;过程4,8月16日;过程5,8月21—24日),区域光化学污染对郊区O₃重污染过程也有贡献(观测期间O₃重污染过程2:8月4—6日);结合后向气流轨迹进一步辅助说明了不同重污染过程中O₃的来源不同.研究还发现,观测区域存在反“周末效应”现象,说明观测区域周末受人为影响较为明显;基于观测数据计算的OPE(O₃生成效率)分析了O₃光化学敏感性表明,在有OPE值的22 d内NO_x控制区和VOCs控制区出现的概率(41%)相等,即观测区域O₃对NO_x和VOCs均敏感;此外还发现,在O₃重污染过程中光化学敏感性会随其反应进程发生改变,由NO_x控制区逐渐转变为VOCs控制区.      

同步脱氮除磷系统中两种颜色好氧颗粒污泥的微生物群落特征

为研究同步脱氮除磷系统中出现的WG（白色好氧颗粒污泥）外形特点及微生物群落特征,探究其成因,利用SEM（扫描电子显微镜）表征了系统中的WG与YG（黄色好氧颗粒污泥）的微观形态,并采用Illumina HiSeq 2500高通量测序平台对两种好氧颗粒污泥中细菌与真菌的群落组成进行研究.结果表明:WG结构疏松外形不规则,颗粒表面分布大量杆菌;而YG饱满紧实轮廓清晰,颗粒表面分布大量球菌.WG与YG的细菌群落组成相似,但真菌组成差异较大.与YG相比,WG具有更高的细菌和真菌多样性.变形菌门（Proteobacteria）和拟杆菌门（Bacteroidetes）为WG和YG中的细菌优势门,其在WG中的相对丰度分别为68.85%和26.61%,在YG中的相对丰度分别为82.52%和12.30%.Candidatus competibacter、Candidatus accumulibacter和Chiayiivirga为WG中的优势属,相对丰度分别为22.13%、8.95%和7.37%;Candidatus competibacter、Chiayiivirga和Xanthomonas为YG中的优势属,相对丰度分别为47.94%、6.95%和7.06%.子囊菌门（Ascomycota）和Rozellomycota分别为WG与YG中真菌优势门,其在两个样品中的相对丰度分别为50.10%和81.77%.在属水平,WG中存在大量青霉属（Penicillium）和假丝酵母属（Candida）等丝状真菌,为WG的形成提供了框架.研究显示,当YG破碎成为小菌胶团后,附着在真菌框架上,造成了WG的快速形成,同时WG中Candidatus competibacter的相对丰度较低,使其外形疏松、透光性较好,呈现出白色.      

Capability of cation exchange technology to remove proven N-nitrosodimethylamine precursors

N-nitrosodimethylamine(NDMA) precursors consist of a positively charged dimethylamine group and a non-polar moiety, which inspired us to develop a targeted cation exchange technology to remove NDMA precursors. In this study, we tested the removal of two representative NDMA precursors, dimethylamine(DMA) and ranitidine(RNTD), by strong acidic cation exchange resin. The results showed that pH greatly affected the exchange efficiency, with high removal(DMA 78% and RNTD 94%) observed at pH pk_a-1 when the molar ratio of exchange capacity to precursor was 4. The exchange order was obtained as follows: Ca~(2+) Mg~(2+) RNTD~+ K~+ DMA~+ NH_4~+ Na~+. The partition coefficient of DMA~+to Na~+was 1.41 ± 0.26, while that of RNTD~+to Na~+was 12.1 ± 1.9. The pseudo second-order equation fitted the cation exchange kinetics well. Bivalent inorganic cations such as Ca~(2+)were found to have a notable effect on NA precursor removal in softening column test. Besides DMA and RNTD, cation exchange process also worked well for removing other 7 model NDMA precursors. Overall, NDMA precursor removal can be an added benefit of making use of cation exchange water softening processes.     

覆盖金属氧化物对湖泊沉积物溶解性有机质特征的影响

为揭示不同金属氧化物对湖泊沉积物DOM（溶解性有机质）影响机制,通过室内模拟试验,在沉积物表层分别覆盖Fe、Al、Mn氧化物及湖沙后培养1 a,并利用三维荧光和紫外光谱方法进行表征.结果表明:① 覆盖Al、Fe、Mn氧化物和湖沙主要降低了0~3 cm沉积物的w（DOC）,降幅分别为8.61%、6.27%、22.38%和0.44%. ② 沉积物中DOM的类络氨酸峰（peak B₁）和类色氨酸峰（peak T₂）均产生较大变化.其中三种氧化物均显著降低了上层沉积物中DOM的peak T₂,使底层DOM的peakT₂显著增加. Mn氧化物使DOM的peak B₁降低,Fe和Al氧化物使DOM的peak B₁增加,湖沙则使两类峰均降低. ③ 覆盖金属氧化物改变了沉积物DOM结构特征,其中覆盖Fe氧化物增强了其芳香性,而覆盖Mn氧化物和Al氧化却降低其芳香性,但三者均使DOM腐质化程度及官能团数量增加,并使FI（Fluorescence Index,荧光指数）增大,表明DOM向生物源转化.研究显示,沉积物表层覆盖金属氧化物影响了沉积物中DOM迁移和转化,并促进了其降解,导致其分子量和腐殖化程度增加.