利用单颗粒气溶胶质谱仪研究燃煤尘质谱特征

采用单颗粒气溶胶质谱仪(SPAMS)和再悬浮采样器联用的方式对燃煤电厂烟道气样品和下载灰样品的质谱特征进行测定,并使用颗粒物粒径分级采样仪ELPI测定其粒径分布特征.研究表明,SPAMS监测得到的粒径分布与ELPI结果差异较大,SPAMS对于500 nm以上粒径段检测效果较好;两个样品正谱图中有非常明显的锂、钙、钛、铝等金属组分信号和碳组分信号特征,负谱图中硅酸盐、硝酸盐和硫酸盐等信号比较明显,并且随着粒径的增加碳组分、硫酸盐和硝酸盐等组分对应的信号强度逐渐减弱,而硅酸盐、铝、钙和钛等组分对应的信号强度逐渐增强;对两个样品使用ART-2a聚类获得多个颗粒物类别,分析表明,它们均含有元素碳二次类(硫酸盐和硝酸盐缩写为二次Sec)、有机碳二次类、铝元素碳类、铝钙硅酸盐类和富硅酸盐类等颗粒物类别,并且随着粒径的增加金属硅酸盐颗粒出现频率增大,而含碳颗粒与硫酸盐出现频率降低.但烟道气样品和下载灰样品的质谱特征呈显著差异,下载灰样品更能代表燃煤源真实排放特征.建议在今后建立基于单颗粒质谱固定源成分谱时,应使用单颗粒气溶胶质谱仪在外场进行实测,并使用聚类的方法提取不同粒径段上的源质谱特征,可能会取得更好的效果.     

深圳冬季边界层大气中污染物垂直分布特征

为更好地掌握深圳城区近地边界层大气污染物的性质、来源及大气理化过程,2017年冬季利用深圳市356 m石岩梯度观测塔进行大气主要污染物的垂直观测,获得包括4个高度(60 m/70 m、110 m/120 m、210 m/220 m和325 m/335 m)的污染物浓度垂直分布廓线.分析了不同高度浓度的垂直廓线、相关性和日变化特征,并探讨了风向风速对其的影响.结果表明,SO_2浓度随高度升高先降低再升高,在高空存在明显的区域输送特征;NO_x、PM_(2.5)、PM_(10)浓度随高度升高而下降,70 m高度近地大气中NO_x和PM_(2.5)受局地源影响显著,白天存在由近地大气向上混合扩散的过程,而PM_(10)中的粗粒子部分在整个气层中显现出一个比较稳定的本底值;O_3浓度随高度升高而升高,主要由于夜间高空O_3缺乏NO的滴定反应而具有一个较高的背景值.     

城市热场剖面的分形维数计算及其意义研究——以上海中心城区为例

城市热环境是城市中建筑物的不断增加及人类活动、大气状况、地表热量传输等多种因素综合作用的结果,因此城市往往具有极为复杂的热表面。由于热量分配、传输具有一定的复杂性,传统的模型预测与定点观测方法在分析城市热表面空间结构及其形成机制方面存在一定的不足。随着空间信息科学的发展,卫星遥感技术为获取城市热场信息提供了可靠的手段。选用上海市2000年6月14日的Landsat ETM+热波段影像,首先反演城市地表温度,再引入剖面线分形的方法,在GIS的支持下,计算从人民广场出发的8个方向的分维数,并进一步探讨剖面线分形的意义,得到如下结论：城市热表面的剖面线具有明显的分形特征,8个方向的分维数为1.530 0～1.780 6,表征不同剖面线的复杂程度。热场表面剖面线的分维数揭示了3个方面的意义：首先不同的分维数反映热场不同方向上温度变化的复杂程度;其次,相对于城市中心,反映不同方向上城市边界形态的差异性;第三,进一步揭示不同方向上,下垫面土地利用类型空间组合变化的复杂程度。     

不同来源生物质废弃物高温堆肥过程的物理化学及微生物性质研究

采用实验室小型堆肥系统对3种典型废弃物牛粪、食物残渣及污泥堆肥过程的物理化学及微生物特性进行了研究和比较.研究表明不同原料堆肥pH都能升到8以上,C/N在堆肥过程中有降低的趋势。不同水分调整材料稻秸(RS)、蛭石(V)、废纸(WP)及锯屑(SD)对堆肥过程的影响与不同堆肥原料相比要小的多.在3种不同原料中,食物残渣堆肥活性最高,14 d有机物降解率为47.2%～56.8%,代表微生物量的醌含量在堆肥后期可增加到359.7～472.3 μmol·kg^-1,但微生物群体的多样性较低,醌多样性指数DQ在堆肥后期增加到6.1～6.7.牛粪堆肥只在初始阶段活性较高,之后很快降低,其醌含量较低.在堆肥中期达到最大值为36.3～117.0 μmol·kg^-1,醌多样性指数DQ初始期为10.3～12.8,堆肥过程中逐渐升高至后期达18.1～22.7.污泥堆肥的各项特性介于食物残渣和牛粪之间.堆肥过程的不同主要是由于原料中各种有机成分的不同而导致.根据研究结果提出了对堆肥过程进行合理控制的建议.     

北京市典型溶剂使用行业VOCs成分谱

基于北京市挥发性有机物(VOCs)排放清单和下一阶段VOCs减排的需求,针对汽车整车制造、木质家具制造和出版物印刷这3个主要溶剂使用行业,分别选取典型企业作为研究对象,采用负压法对重点排放环节进行采样,以GC-MS/FID系统测定样品中VOCs组分构成,从而获取了北京市典型溶剂使用行业VOCs成分谱.结果表明,汽车整车制造主要排放环节排放的VOCs组分存在明显差异,色漆涂装工序以含氧VOCs和芳香烃为主,分别占比71. 26%和27. 14%,罩光工序芳香烃达到84. 10%;木质家具制造业不同排放环节的VOCs组分差异不大,均以含氧VOCs和芳香烃为主,分别占55. 08%和18. 98%;出版物印刷业不同排放环节无法单独监测,其混合废气VOCs组分以烷烃和含氧VOCs为主,分别占比47. 29%和44. 57%.     

六类餐饮源排放PM2.5化学成分谱

大气颗粒物源成分谱可以表征源排放颗粒物的理化特征,为受体模型开展来源解析研究提供基础数据.餐饮油烟排放是室内外环境大气污染的来源之一,当前餐饮源排放PM_2.5的化学成分谱仍然缺乏.该研究分别在成都市、武汉市和天津市采集了29组6种餐饮源（居民烹饪、火锅店、烧烤店、职工食堂、中餐馆、商场综合餐饮）排放的PM_2.5样品,分析无机元素、离子、碳、多环芳烃（PAHs）等化学组分,并构建了餐饮源排放颗粒物化学成分谱.结果表明:①餐饮源排放PM_2.5化学成分中的主要组分为OC（有机碳）、EC（元素碳）、Ca、Al、Fe、NH₄+、SO₄2-、NO₃-、Na+、K+、Mg2+和Cl-,其中w（OC）最高,为41.67%~57.91%.②餐饮源排放PM_2.5的PAHs中,3环和4环占比较高,其中芴（Flu）、菲（Phe）、荧蒽（Fla）、芘（Pyr）的质量分数相对其他物质较高.研究显示:餐饮源排放PM_2.5中OC/EC约为15.99~67.61,在一定程度上可以用来表征餐饮源排放;Fla/（Fla+Pyr）和InP/（InP+BghiP）多集中在0.45~0.55之间,或可作为标识餐饮源的特征比值.      

Distribution of polychlorinated dibenzo-p-dioxins and dibenzofurans in ambient air of different regions in China

Levels of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) were determined in fourteen ambient air samples collected in twelve cities of five provinces and one large municipality in China. The PCDD/F concentrations varied from 2.6 to 120 pg m⁻³ (or from 0.04 to 1.93 pg I-TEQ m⁻³). Generally, TCDF was the dominant homologue group and as a rule the homologue concentration of PCDF decreased with rising chlorine substitution number of PCDF. In all cases 2,3,4,7,8-PeCDF was the most important contributor to the I-TEQ value, accounting for 35–57% of the total I-TEQ value. Higher PCDD/F levels in ambient air were found during winter. The highest PCDD/F levels were found in Chengdu, Sichuan Province. In general, the PCDD/F levels in this study were in the same range as in other studies in China.     

Pu/Cs ratios in the water column of the North Pacific: a proxy of biogeochemical processes

Anthropogenic radionuclides in seawater have been used as transient tracers of processes in the marine environment. Especially, plutonium in seawater is considered to be a valuable tracer of biogeochemical processes due to its particle-reactive properties. However, its behavior in the ocean is also affected by physical processes such as advection, mixing and diffusion. Here we introduce Pu/¹³⁷Cs ratio as a proxy of biogeochemical processes and discuss its trends in the water column of the North Pacific Ocean. We observed that the ^239,240Pu/¹³⁷Cs ratio in seawater exponentially increased with increasing depth (depth range: 100–1000 m). This finding suggests that the profiles of the ^239,240Pu/¹³⁷Cs ratios in shallower waters directly reflect biogeochemical processes in the water column. A half-regeneration depth deduced from the curve fitting the observed data, showed latitudinal and longitudinal distributions, also related to biogeochemical processes in the water column.     

Determining floodplain sedimentation rates using Cs in a low fallout environment dominated by channel- and cultivation-derived sediment inputs, central Queensland, Australia

Fallout ¹³⁷Cs has been widely used to determine floodplain sedimentation rates in temperate environments, particularly in the northern hemisphere. Its application in low fallout, tropical environments in the southern hemisphere has been limited. In this study we assess the utility of ¹³⁷Cs for determining rates of floodplain sedimentation in a dry-tropical catchment in central Queensland, Australia. Floodplain and reference site cores were analysed in two centimetre increments, depth profiles were produced and total ¹³⁷Cs inventories calculated from the detailed profile data. Information on the rates of ¹³⁷Cs migration through local soils was obtained from the reference site soil cores. This data was used in an advection–diffusion model to account of ¹³⁷Cs mobility in floodplain sediment cores. This allowed sedimentation rates to be determined without the first year of detection for ¹³⁷Cs being known and without having to assume that ¹³⁷Cs remains immobile following deposition. Caesium-137 depth profiles in this environment are demonstrated to be an effective way of determining floodplain sedimentation rates. The total ¹³⁷Cs inventory approach was found to be less successful, with only one of the three sites analysed being in unequivocal agreement with the depth profile results. The input of sediment from catchment sources that have little, or no, ¹³⁷Cs attached results in true depositional sites having total inventories that are not significantly different from those of undisturbed reference sites.     

Carbofuran degradation in soil profiles

Abstract

Two soils, Puyallup fine sandy loam from Puyallup, WA, and Ellzey fine sand from Hastings, FL, each with a prior history of carbofiiran exposure but with different pedological and climatological characteristics, were found to exhibit enhanced degradation toward carbofiiran in surface and subsurface soil layers. The treated Puyallup and Ellzey soils exhibited higher mineralization rates for both the carbonyl and the aromatic ring of carbofiiran when compared to untreated soils. Disappearance rates of [¹⁴C‐URL (uniformly ring labeled)] carbofiiran in the treated Ellzey soil was faster than in untreated soil, and also faster in surface soil than in subsurface soil. Initial degradation patterns in the treated Ellzey soil were also different from those in the untreated soil. The treated Ellzey soil degraded carbofuran mainly through biological hydrolysis, while untreated soil degraded carbofuran through both oxidative and hydrolytic processes.