1990-2018年浙江省人为铅排放时空变化解析

随着工农业的高速发展,大量的人为铅排放到环境,引起了一系列的生态健康问题.本文以工农业集产区浙江省为案例,系统构建了18个铅排放源排放清单,其中新增添了纺织业、制革业、造纸业、秸秆利用、牲畜废物利用、化肥消费、农药消费等铅排放行业,估算了浙江省1990—2018年各污染源铅排放量,分析了其时空变异趋势.结果表明,浙江省前期（1990—2000）铅排放通量增长有限,其排放量仅约2500 t·a^-1,有色金属开采贡献了约55%;其后增长速度较快,到2014年以后达到较高的稳定值,约35000 t·a^-1,是1990年的14倍,铅酸蓄电池生产是其主要排放源,占比从14%增长到了80%.从排放的去向来看,98%左右的铅通过固废的形式进入环境,而进入大气和废水的只有2%和0.2%左右,其主要排放源分别为铅酸蓄电池生产、原煤燃烧、纺织业.而浙江省各个地区铅排放表现出较大的空间差异,各地区因工农业发展模式不一样,人为排放源也不一样.总体来看北部高于南部,尤其湖州、绍兴、舟山等地铅排放量较高.可见,浙江省人为铅排放形势仍然很严峻,控制好铅酸蓄电池生产固废资源化无害化处理是源头控制的重中之重,调整原煤燃烧将有利于降低大气铅排放,纺织业废水净化处理对缓解水体铅污染有重要意义.本研究不仅为浙江省铅污染治理提供了重要科学依据,同时也为铅污染源端防控提供了数据基础.     

Speciation and Seasonal Variations of Dissolved Inorganic Arsenic in Jiaozhou Bay,North China

The distributions and biogeochemical cycles of arsenic in the aquatic environment have captured the interest of geochemists due to arsenic’s multiple chemical forms, the toxicity of certain arsenic species and large anthropogenic input. Seasonal variations in the dissolved inorganic arsenic concentration and speciation in Jiaozhou Bay, which is located on the west coast of the Yellow Sea in northern China, are presented here. Three cruises were carried out in Jiaozhou Bay under varying tidal regimes, one at neap tide and one at spring tide in August and one at spring tide in October of 2001. In addition to the transect surveys, the main sources of dissolved inorganic arsenate and arsenite in Jiaozhou Bay, including riverine input from five major tributary rivers, atmospheric dry and wet depositions, and groundwater and wastewater input, were collected in different seasons to estimate arsenic transport through different sources. The mean concentrations of total dissolved inorganic arsenic (TDIAs, As (V+III)) in Jiaozhou Bay were statistically comparable between summer and autumn, with higher concentrations at the northwest and northeast parts of the bay, reflecting human activities. The As (III)/TDIAs ratio ranged between 0.045 and 0.68, with an average of 0.16, implying that arsenate was the dominating species in Jiaozhou Bay. A preliminary box model was established to estimate the water-mass balance and arsenic budgets for Jiaozhou Bay, which demonstrated that river inputs and atmospheric depositions were the main sources of arsenic into Jiaozhou Bay. The concentrations of dissolved inorganic arsenic in Jiaozhou Bay have decreased in the last two decades. Compared with other areas in the world, the concentration of arsenic in Jiaozhou Bay remains at the natural level and this region can be characterized as a less disturbed area.     

西安市大气中多溴联苯醚的季节变化特征及人体暴露评估

利用大流量主动采样器于2008年8月至2009年7月采集了西安城区气态和颗粒态大气样品,研究了大气中多溴联苯醚(PBDEs)的季节变化特征.结果表明,西安大气中总PBDEs(气相+颗粒相)浓度范围为21.38~161.84pg/m3,平均值为66.34pg/m3.大气中PBDEs在冬季污染最严重,颗粒相PBDEs季节变化趋势与总悬浮颗粒(TSP)较为相似,气相PBDEs的季节变化没有颗粒相明显.对PBDEs的总浓度、气相浓度、颗粒相浓度与采样期间气象因素做偏相关分析,发现总浓度和颗粒相浓度均与气压呈显著正相关,与温度呈显著负相关,表明西安大气中PBDEs浓度主要受气压和温度的影响.对西安普通人群的PBDEs吸入暴露量进行计算,并采用BDE-99的吸入量进行人体暴露评估,西安普通儿童和成人对BDE-99总摄入量低于De Winter-Sorkina提出的最大允许摄入量260pg/(kg·d).     

Spatial and temporal variations of water quality in Cao-E River of eastern China

Evaluation and analysis of water quality variations were performed with integrated consideration of water quality parameters, hydrological-meteorologic and anthropogenic factors in Cao-E River, Zhejiang Province of China. Cao-E River system has been polluted and the water quality of some reaches are inferior to Grade V according to National Surface Water Quality Standard of China （GB2002）. However, mainly polluted indices of each tributary and mainstream are different. Total nitrogen （TN） and total phosphorus （TP） in the water are the main polluted indices for mainstream that varies from 1.52 to 45.85 mg/L and 0.02 to 4.02 mg/L, respectively. TN is the main polluted indices for Sub-watershed Ⅰ, Ⅱ, Ⅳ and Ⅴ（0.76 to 18.27 mg/L）. BOD5 （0.36 to 289.5 mg/L）, CODMn （0.47 to 78.86 mg/L）, TN （0.74 to 31.09 mg/L） and TP （0 to 3.75 mg/L） are the main polluted indices for Sub-watershed Ⅲ. There are tow pollution types along the river including nonpoint source pollution and point source pollution types. Remarkably temporal variations with a few spatial variations occur in nonpoint pollution type reaches （including mainstream, Sub-watershed Ⅰ and Ⅱ） that mainly drained by arable field and/or dispersive rural dwelling district, and the maximum pollutant concentration appears in flooding seasons. It implied that the runoff increases the pollutant concentration of the water in the nonpoint pollution type reaches. On the other hand, remarkably spatial variations occur in the point pollution type reaches （include Sub-watershed Ⅲ, Ⅳ and Ⅴ） and the maximum pollutant concentration appears in urban reaches. The runoff always decreases the pollutant concentration of the river water in the seriously polluted reaches that drained by industrial point sewage. But for the point pollution reaches resulted from centralized town domestic sewage pipeline and from frequent shipping and digging sands, rainfall always increased the concentration of pollutant （TN） in the river water too. Pollution controls were respectively suggested for these tow types according to different pollution causes.     

青藏高原纳木错湖水主要化学离子的时空变化特征

为揭示青藏高原纳木错湖水化学离子的时空变化特征、来源以及主要控制因子,于2006～2010年连续定点(30°47.27’N,90°58.53’E,4 718 m a.s.l.)采集近岸表层湖水样品;于2009年8月采集湖心区剖面样品;于2010年10月采集湖心区剖面样品及表层湖水样品;对其主要化学离子进行分析.结果表明,纳木错湖水中主要阳离子为Na+,主要阴离子为HCO3-.绝大多数离子浓度在季风期较高(6～9月),而非季风期尤其是封冻期(1～4月)偏低;Ca2+浓度的变化则相反,即封冻期较高,而非封冻期较低且变化较小.对垂直剖面湖水分析表明,在湖水垂直结构稳定的非季风期(如10月),除Ca2+浓度随深度无显著变化外,其他离子浓度随深度增加而增大.纳木错湖水主要离子来源于入湖河水的贡献;影响离子时空变化的因素包括蒸发、降水、pH值等,其中蒸发是最主要的影响因素,它造成湖水Na+浓度不断升高而Ca2+浓度降低.     

Secondary organic aerosols in Jinan, an urban site in North China: Significant anthropogenic contributions to heavy pollution

Secondary organic aerosols(SOAs) are an important component of particulates, but whether biogenic SOAs(BSOAs) or anthropogenic SOAs(ASOAs) are the dominant contributors to haze pollution remains poorly characterized. In this study, particulate samples were collected from September 2014 to August 2015 at an urban site in Jinan, which is the capital of Shandong Province and a typical city in the North China Plain. The PM2.5 samples were analyzed for BSOA(isoprene(SOAI) and monoterpenes(SOAM)) and ASOA(aromatic(SOAA)) tracers. The concentrations of the SOAAtracer(1.1 ± 1.0 ng/m3) were lowest, and those of SOAItracers(41.8 ± 86.2 ng/m3) were highest, with the concentrations of SOAMtracers(19.4 ± 9.9 ng/m3) being intermediate. The SOAItracers were more abundant in the summer and less abundant in the winter. Both SOAIand SOAMincreased with increasing ozone level but decreased with increasing NOx level. Correlation analysis revealed a good correlation between 2,3-dihydroxy-4-oxopentanoic acid and levoglucosan levels in three seasons. These results suggested that biomass burning activities occurring in the NCP can enhance the emissions of aromatics and should be controlled, especially in the autumn and winter. SOA tracers were classified according to pollution degree, and the results showed that as pollution increases, the contributions of SOAAincrease. These results indicate that reducing anthropogenic emissions is necessary to prevent SOA pollution, especially during heavy pollution episodes.     

黄渤海气溶胶中砷的分布特征和季节变化

于2017~2018年冬、春和夏季,在黄渤海海域走航采样,采集总悬浮颗粒物（TSP）样品,分析总砷（As）、As （Ⅴ）、As （Ⅲ）以及水溶性离子,讨论了As在黄渤海气溶胶中浓度、空间分布以及季节变化,估算了As的干沉降通量.气溶胶中As含量冬季（6.6 ng·m^-3） > 夏季（5.5 ng·m^-3） > 春季（4.4 ng·m^-3）,渤海和北黄海远大于南黄海.冬、夏季As（Ⅲ）/As（Ⅴ）比值分别为0.41和0.21.冬、春和夏季As/TSP平均值分别为95.4、83.9和81.4 μg·g^-1,冬季明显高于春季和夏季.冬季在冬季风主导下,携带了环渤海地区排放的污染物导致砷含量最高,夏季受东南季风携带的东部沿海地区污染物的影响也较大,而春季受西伯利亚陆地气团和东南远海海洋性气团的共同影响,浓度最小.冬季K⁺/TSP与As/TSP存在显著正相关（r=0.78,P<0.05）,说明受陆地生物质燃烧排放的As的影响明显,而夏季两者相关性不显著,说明来源不同.冬、春和夏季黄渤海大气气溶胶As的干沉降通量分别为1.15、0.77和0.97 μg·（m²·d）^-1,年平均为0.95 μg·（m²·d）^-1.     

黄土高原地区生态脆弱性时空变化及其驱动因子分析

黄土高原是我国生态系统最脆弱的地区之一,科学评估其生态脆弱性是制定有效环境保护和管理措施的前提.然而,过去研究多关注某一小区域的生态脆弱性,不能反映该地区生态脆弱性的整体特征.基于"暴露-敏感性-适应力"模型框架,结合层次分析、空间主成分分析和地理探测器等方法评估了黄土高原地区2000~2015年生态脆弱性的时空变化特征及其驱动因子.结果表明,黄土高原地区生态脆弱性整体较高,并呈现出从东南到西北递增的趋势,且不同土地利用类型脆弱性差异大;2000~2015年生态脆弱性呈先增后降趋势,整体呈微弱降低趋势,其中约64%地区的脆弱性发生了变化;植被覆盖度和降水是控制生态脆弱性时空变化的主要因子,且所有指标因子间均存在明显的交互作用.说明气候变化和人类活动可能有助于降低黄土高原地区的生态脆弱性,但其作用有限.     

珠江流域水化学组成的时空变化特征及对岩石风化碳汇估算的意义

基于水-岩-气-生相互作用的碳酸盐风化碳汇模型表明,陆地碳酸盐风化碳汇是大气CO_2汇的重要组成部分;然而,碳酸盐风化碳汇的过程、机制和控制因素仍有待进一步的研究。本文采用野外监测、现场滴定和样品室内测试相结合的方法,对珠江流域支干流分旱季和雨季进行了4次野外监测取样,研究其水化学组成的时空变化特征。结果表明:珠江流域支干流的水化学组成受流域岩石风化、气候和水生光合作用的共同影响,并具有明显的时空变化特征。空间上,南盘江下游双江口段至红水河上游蔗香段,水流较慢,水质清澈,水生光合作用强烈,电导率、[HCO_3~-]和[Ca~(2+)]的空间变化主要受水生光合作用控制;从红水河上游蔗香段至肇庆西江大桥监测点,反映的是流域岩石风化对水化学空间变化的影响。季节变化上,西江的电导率、[HCO_3~-]和[Ca~(2+)]呈现出夏季低、冬春季高的特征,主要反映稀释效应的控制。西江干流河水的溶解氧具有明显的季节变化,在上述南盘江下游双江口段至红水河上游蔗香段,DO是夏季高冬季低,其他监测点是冬季高而夏季低;DO的季节变化受水生光合作用强度的控制。在南盘江下游双江口段至红水河上游蔗香段,温度是光合作用强度的限制因子,而其他监测点的光合作用限制因子为浊度影响的光照。造成上述差异的原因是监测点的水文环境不同。通过对梧州水文站流量和[HCO_3~-]变化的分析发现,[HCO_3~-]的季节变化幅度相对流量小得多,显示在西江流域中,HCO_3~-也存在化学稳定性行为。因此在西江流域中,流量变化是岩溶碳汇通量变化的主控因子。研究还发现,西江流域中具有强烈的生物碳泵效应,由内源有机碳形成的碳汇通量约占传统计算模式碳汇(溶解无机碳-DIC)通量的40%。因此,在估算珠江流域碳酸盐风化碳汇时,必须考虑水生生态系统光合生物对DIC的利用形成的有机碳的贡献。     

韶关市3座供水水库蓝藻种群及微囊藻毒素的季节变化

为了解供水水库的蓝藻种群和微囊藻毒素的季节变化,于2012年1—12月对韶关的苍村、瀑布和花山3座供水水库进行了采样分析。结果表明,3座水库为中营养型水库,监测蓝藻共9属(种),优势种为鱼腥藻和微囊藻,蓝藻最高丰度为5.67×107L-1;降水导致营养盐物质带入水库和水体不稳定性是蓝藻种群和优势种在夏秋两季季节变化和占优势的主要影响因子。3座水库ρ(微囊藻毒素)为0.1~0.9μg/L,最高值接近世界卫生组织对饮用水中MC-LR的指导性限制值(1μg/L)标准。微囊藻与微囊藻毒素呈显著正相关性(R=0.871,P0.01),表明产微囊藻毒素的蓝藻主要为微囊藻,当水库发生微囊藻水华时有发生微囊藻毒素的风险。