不同CDPF贵金属负载量对柴油公交车VOCs组分排放影响

基于重型底盘测功机,利用质子转移反应质谱(PTR-MS)研究了柴油公交车在中国典型城市公交车循环(CCBC)下,不同CDPF贵金属负载量对尾气中挥发性有机物(VOCs)组分排放特性的影响.结果表明,柴油公交车VOCs主要组分为含氧有机物(OVOCs)、芳香烃和烯烃等,且OVOCs占比达50%以上;在贵金属成分、配比相同时,VOCs减排率随CDPF贵金属负载量增加而增加:贵金属负载量为15 g·ft~(-3)(A型后处理装置)、25 g·ft~(-3)(B型)和35 g·ft~(-3)(C型)时,VOCs总量的减排率依次为36.2%、40.1%和41.4%.C型后处理装置对烷烃全循环减排率高达70.2%,且对OVOCs的催化有微弱优势;对于不饱和烃类,3种不同贵金属负载量的后处理装置均有一定催化效果,但无明显差异;A型对含氮有机物减排率可达50.5%,但减排率随贵金属负载量增加而降低.采用DOC+CDPF后能较好地降低公交车VOCs排放量进而降低臭氧生成潜势(OFP).同时考虑不同方案减排效果与成本因素,当加权系数分别为0.8和0.2时,B型为最优方案.     

南京北郊黑碳气溶胶的来源解析

利用七波段黑碳仪对2015年1~12月南京北郊地区黑碳(black carbon,BC)气溶胶实时监测,并结合黑碳仪模型对该期间内BC进行来源解析,探讨化石燃料排放产生BC(BCff)与生物质燃烧产生BC(BCbb)各自的贡献大小.结果表明,观测期间BC的吸收波长指数(α)和生物质燃烧对BC的贡献百分比(BB)的变化范围都较大但趋势较为一致;冬季α值偏高而夏季α值较低,表明不同季节时间BC来源和强度的差异性.BCff在各季节BC总浓度中占比略有不同但均高于75%;BC、BCff和BCbb的日变化趋势均呈双峰特征,在07:00~09:00和18:00~21:00左右浓度有最大值;全天中,BCff对BC贡献最大,浓度值约为BCbb的3~5倍;夜晚BC浓度普遍高于白天,其平均浓度值是白天的1.2倍.由浓度权重轨迹分析的结果可知,影响南京北郊地区高浓度BC的源区主要集中在浙江、安徽以及江西和福建等地区.     

西大海湖沉积物营养盐垂直分布特征变化分析

通过对西大海湖心柱状沉积岩芯有机质(OM)、总氮(TN)、总磷(TP)、磷形态和粒度指标的测试和分析,探讨其垂向分布特征及影响因素.结果表明,营养盐中OM、TN和TP的含量分别为0.633%~2.756%、0.150%~0.429%和648.00~1 480.67 mg·kg-1.Ca-P是TP的主要部分,占TP含量66.04%.1843~1970年间,Ca-P、IP、OM含量变化较小,Fe/Al-P、OP、TP、TN含量波动较大;1970~1996年间,Ca-P、IP、TP含量变化均呈减小趋势,Fe/Al-P、OP、OM含量不同程度上先减少后增加,TN波动较大;1996~2009年营养元素含量相对波动较大,Fe/Al-P、OP和OM的平均含量是3个阶段中最高的.西大海湖沉积岩芯营养元素污染来源以工业废水、生活污水和化肥农药的流失为主.沉积物中C/N比值显示有机质主要来源于水生生物.沉积物粒度组成以黏土和细粉砂为主.相关性研究表明,Ca-P、IP与TP均呈显著的正相关关系,表明Ca-P对IP、TP的增长贡献大.     

Removal of perfluorinated surfactants from wastewater by adsorption and ion exchange——Influence of material properties,sorption mechanism and modeling

Perfluorooctane sulfonate(PFOS) has attracted increasing concern in recent years due to its world-wide distribution, persistence, bioaccumulation and potential toxicity. The influence of sorbent properties on the adsorptive elimination of PFOS from wastewater by activated carbons, polymer adsorbents and anion exchange resins was investigated with regard to their isotherms and kinetics. The batch and column tests were combined with physicochemical characterization methods, e.g., N_2 physisorption, mercury porosimetry, infrared spectroscopy, differential scanning calorimetry, titrations, as well as modeling. Sorption kinetics was successfully modelled applying the linear driving force(LDF) approach for surface diffusion after introducing a load dependency of the mass transfer coefficient βs.The big difference in the initial mass transfer coefficient βs,0, when non-functionalized adsorbents and ion-exchange resins are compared, suggests that the presence of functional groups impedes the intraparticle mass transport. The more functional groups a resin possesses and the longer the alkyl moieties are the bigger is the decrease in sorption rate.But the selectivity for PFOS sorption is increasing when the character of the functional groups becomes more hydrophobic. Accordingly, ion exchange and hydrophobic interaction were found to be involved in the sorption processes on resins, while PFOS is only physisorptively bound to activated carbons and polymer adsorbents. In agreement with the different adsorption mechanisms, resins possess higher total sorption capacities than adsorbents. Hence, the latter ones are rendered more effective in PFOS elimination at concentrations in the low μg/L range, due to a less pronounced convex curvature of the sorption isotherm in this concentration range.     

Impact of microbial communities from tropical soils on the mobilization of trace metals during dissolution of cinnabar ore

Biodissolution experiments on cinnabar ore(mercury sulphide and other sulphide minerals,such as pyrite) were performed with microorganisms extracted directly from soil. These experiments were carried out in closed systems under aerobic and anaerobic conditions with 2 different soils sampled in French Guyana. The two main objectives of this study were(1) to quantify the ability of microorganisms to mobilize metals(Fe, Al, Hg) during the dissolution of cinnabar ore, and(2) to identify the links between the type and chemical properties of soils, environmental parameters such as season and the strategies developed by indigenous microorganisms extracted from tropical natural soils to mobilize metals.Results indicate that microbial communities extracted directly from various soils are able to(1) survive in the presence of cinnabar ore, as indicated by consumption of carbon sources and,(2) leach Hg from cinnabar in oxic and anoxic dissolution experiments via the acidification of the medium and the production of low molecular mass organic acids(LMMOAs). The dissolution rate of cinnabar in aerobic conditions with microbial communities ranged from 4.8 × 10~(-4) to 2.6 × 10~(-3) μmol/m~2/day and was independent of the metabolites released by the microorganisms. In addition, these results suggest an indirect action by the microorganisms in the cinnabar dissolution. Additionally, because iron is a key element in the dynamics of Hg, microbes were stimulated by the presence of this metal,and microbes released LMMOAs that leached iron from iron-bearing minerals, such as pyrite and oxy-hydroxide of iron, in the mixed cinnabar ore.     

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.     

重庆市夏秋季VOCs对臭氧和二次有机气溶胶生成潜势的估算

为估算重庆市夏秋季VOCs（挥发性有机物）对O₃和SOA（二次有机气溶胶）的生成潜势,利用在线GC-MS/FID在2015年8月22日-9月23日对重庆市区点和郊区点VOCs开展了为期一个月的实时观测,获得市区点和郊区点$ \varphi $（TVOCs）（总挥发性有机物）分别为41.35×10-9和22.72×10-9,其中市区点以烷烃（35.2%）和烯炔烃（25.2%）为主,郊区点以含氧挥发性有机物（oxygenated volatile organic compounds,OVOCs）（30.6%）和烷烃（26.0%）为主.结合最大增量反应活性量化市区点和郊区点VOCs的OFPs（臭氧生成潜势）分别为149.11×10-9和71.09×10-9,市区点OFPs最大的是乙烯、丙烯、甲苯、C8和C9的芳香烃等,郊区点OFPs最大的VOCs是丙烯醛、异戊二烯和甲基乙烯基酮.结合气溶胶生成系数量化郊区点和市区点VOCs对SOA的生成贡献分别为0.36和1.26 μg/m3,相比国内其余城市VOCs的SOAP（二次有机气溶胶生成潜势）较小,主要以甲基环己烷、正壬烷、正葵烷和十一烷等高碳烷烃,以及甲苯、苯、二甲苯和乙苯等芳香烃的SOAP为主.研究显示,控制烯炔烃和芳香烃的浓度有助于控制重庆市O₃的生成,控制高碳烷烃和芳香烃则有助于控制重庆市SOA的生成.      

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.      

人为干扰对小兴安岭森林湿地土壤碳组分和酶活性的影响

以小兴安岭落叶林沼泽湿地为研究对象,对比研究皆伐地、火烧地和落叶松湿地土壤碳组分和酶活性.结果表明:(1)3种湿地类型土壤SOC含量表现为对照地显著高于皆伐地和火烧地(p0.05),在0~10 cm土层中皆伐地与对照地相比降低了58.38%,火烧地与对照地相比降低了61.96%.皆伐地与火烧地在不同土层的土壤中SOC含量差异不显著(p0.05);DOC含量对照地显著高于皆伐地和火烧地(p0.05).在0~10cm土层中火烧地DOC含量是皆伐地的1.99倍,两者差异不显著(p0.05);不同干扰方式对土壤MBC含量影响的差异主要表现在0~10 cm的土层土壤,对照地分别比皆伐地和火烧地高23.13%和95.79%(p0.05).在不同的土层中皆伐地MBC含量均大于火烧地,与SOC含量的变化趋势一致.(2)与对照地相比,皆伐地与火烧地0~10 cm土层的土壤蔗糖酶活性分别降低了45.59%和36.76%,脲酶活性显著降低了18.22%和55.69%(p0.05),蛋白酶活性降低了19.65%和17.34%,淀粉酶活性降低了6.29%和10.69%.土壤碳组分和酶活性在垂直方向上均表现为随着土层深度增加而减小.皆伐和火烧造成森林湿地土壤碳组分和酶活性降低.     

Ti/SnO_2-Sb阳极-空气阴极电催化降解染料废水

为解决电化学法处理高盐染料废水存在的能耗大、成本高等问题,分别采用溶胶-凝胶法和辊压法制备Ti/SnO_2-Sb阳极和空气阴极,构建了Ti/SnO_2-Sb阳极-空气阴极双极体系(TSSA-ADC)。甲基橙(MO)作为高盐染料废水的典型污染物,考察了电流强度、MO浓度、电解液浓度和初始p H对TSSA-ADC体系和TSSA单阳极体系降解MO的影响。结果表明:与TSSA单阳极体系相比,TSSA-ADC体系具有更好的抗有机负荷冲击、抗盐分冲击、抗酸碱波动能力,能够维护酸碱平衡防止硬度离子结垢。最佳反应条件为电流强度为0.030 A,电解液浓度为3%,MO浓度为100 mg/L,初始pH=6。以MO去除率达到98%为基准,TSSA-ADC体系比TSSA体系可节能74.26%。