典型工业源VOCs治理现状及排放组成特征

基于长三角典型城市大气VOCs排放清单识别的8个VOCs主要排放行业,选择11家代表性企业,实测研究了VOCs治理装置、排放现状、排放组成特征,并计算相关行业排放的臭氧生成潜势.结果表明,不同净化技术对非甲烷总烃(NMHC)的去除效率差异大,存在净化后浓度增加的现象,目前的环保装置对废气的处理有待优化.本次采样的大部分企业存在NMHC、苯、甲苯、二甲苯超标现象,其中甲苯的超标情况最严重.对于筛选的8个主要行业,芳香烃和含氧VOCs,是最主要的排放化合物,芳香烃是对臭氧生成贡献最大的化合物.在不同行业中,VOCs组成存在显著差异,因此在制定VOCs减排控制措施时,应优先减排对臭氧生成贡献大的行业.     

我国淡水生物菲水质基准研究

菲是一种国内外水体中普遍检出的优控多环芳烃,会对水生生物产生有害影响.然而,由于本土物种生态毒理学数据匮乏等问题,关于菲的基准阈值研究鲜有报道.本研究以9种本土水生生物为研究对象,进行了9种水生生物的急性生态毒理学实验及3种慢性生态毒理学实验并推导了菲的基准阈值.此外,基于物种敏感性分布法(species sensitivity distribution,SSD)对本地和非本地物种之间的差异进行了比较,以期探究美国水生生物毒性数据在我国本土基准阈值推导过程中的可行性.结果显示,采用US EPA"指南"推荐的方法对菲本土水生生物急性基准阈值(CMC)和慢性基准阈值(CCC)进行了推导,分别为0.033 mg·L~(-1)和0.012 mg·L~(-1);另外,本土与美国物种敏感性分布不存在显著性差异,这表明存在使用美国水生生物毒性数据来推导我国菲水生生物基准阈值的可能性.     

Molecular characterization of effluent organic matter in secondary effluent and reclaimed water: Comparison to natural organic matter in source water

Municipal wastewater reclamation is becoming of increasing importance in the world to solve the problem of water scarcity. A better understanding of the molecular composition of effluent organic matter(Ef OM) in the treated effluents of municipal wastewater treatment plants(WWTPs) is crucial for ensuring the safety of water reuse. In this study, the molecular composition of Ef OM in the secondary effluent of a WWTP in Beijing and the reclaimed water further treated with a coagulation–sedimentation–ozonation process were characterized using a non-target Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS) method and compared to that of natural organic matter(NOM) in the local source water from a reservoir. It was found that the molecular composition of Ef OM in the secondary effluent and reclaimed water was dominated by CHOS formulas, while NOM in the source water was dominated by CHO formulas. The CHO formulas of the three samples had similar origins. Anthropogenic surfactants were responsible for the CHOS formulas in Ef OM of the secondary effluent and were not well removed by the coagulation-sedimentation-ozonation treatment process adopted.     

Concurrent catalytic removal of typical volatile organic compound mixtures over Au-Pd/α-MnO2 nanotubes

α-MnO_2 nanotubes and their supported Au-Pd alloy nanocatalysts were prepared using hydrothermal and polyvinyl alcohol-protected reduction methods, respectively. Their catalytic activity for the oxidation of toluene/m-xylene, acetone/ethyl acetate, acetone/m-xylene and ethyl acetate/m-xylene mixtures was evaluated. It was found that the interaction between Au-Pd alloy nanoparticles and α-MnO_2 nanotubes significantly improved the reactivity of lattice oxygen, and the 0.91 wt.% Au0.48 Pd/α-MnO_2 nanotube catalyst outperformed the α-MnO_2 nanotube catalyst in the oxidation of toluene, m-xylene, ethyl acetate and acetone. Over the0.91 wt.% Au0.48 Pd/α-MnO_2 nanotube catalyst,(i) toluene oxidation was greatly inhibited in the toluene/m-xylene mixture, while m-xylene oxidation was not influenced;(ii) acetone and ethyl acetate oxidation suffered a minor impact in the acetone/ethyl acetate mixture; and(iii) m-xylene oxidation was enhanced whereas the oxidation of the oxygenated VOCs(volatile organic compounds) was suppressed in the acetone/m-xylene or ethyl acetate/m-xylene mixtures. The competitive adsorption of these typical VOCs on the catalyst surface induced an inhibitive effect on their oxidation, and increasing the temperature favored the oxidation of the VOCs. The mixed VOCs could be completely oxidized into CO_2 and H_2 O below 320°C at a space velocity of 40,000 m L/(g·hr). The 0.91 wt.% Au0.48 Pd/α-MnO_2 nanotube catalyst exhibited high catalytic stability as well as good tolerance to water vapor and CO_2 in the oxidation of the VOC mixtures. Thus, the α-MnO_2 nanotube-supported noble metal alloy catalysts hold promise for the efficient elimination of VOC mixtures.     

Simultaneous removal of ammonia and N-nitrosamine precursors from high ammonia water by zeolite and powdered activated carbon

When adding sufficient chlorine to achieve breakpoint chlorination to source water containing high concentration of ammonia during drinking water treatment, high concentrations of disinfection by-products(DBPs) may form. If N-nitrosamine precursors are present, highly toxic N-nitrosamines, primarily N-nitrosodimethylamine(NDMA), may also form. Removing their precursors before disinfection should be a more effective way to minimize these DBPs formation. In this study, zeolites and activated carbon were examined for ammonia and N-nitrosamine precursor removal when incorporated into drinking water treatment processes.The test results indicate that Mordenite zeolite can remove ammonia and five of seven N-nitrosamine precursors efficiently by single step adsorption test. The practical applicability was evaluated by simulation of typical drinking water treatment processes using six-gang stirring system. The Mordenite zeolite was applied at the steps of lime softening, alum coagulation, and alum coagulation with powdered activated carbon(PAC) sorption. While the lime softening process resulted in poor zeolite performance, alum coagulation did not impact ammonia and N-nitrosamine precursor removal. During alum coagulation, more than67% ammonia and 70%–100% N-nitrosamine precursors were removed by Mordenite zeolite(except 3-(dimethylaminomethyl)indole(DMAI) and 4-dimethylaminoantipyrine(DMAP)). PAC effectively removed DMAI and DMAP when added during alum coagulation. A combination of the zeolite and PAC selected efficiently removed ammonia and all tested seven N-nitrosamine precursors(dimethylamine(DMA), ethylmethylamine(EMA), diethylamine(DEA), dipropylamine(DPA), trimethylamine(TMA), DMAP, and DMAI) during the alum coagulation process.     

中国生态用地及生态系统服务价值变化研究

生态用地具有重要的生态系统服务功能,在维护生态平衡、保障国土生态安全、应对全球气候变化中具有特殊地位。论文在总结国内研究学者有关生态用地研究成果的基础上,从生态系统服务功能入手,界定了生态用地的概念,根据生态干扰度构建了生态用地分类体系,并将生态用地分类与土地利用分类进行衔接,对全国生态用地的生态系统服务价值进行了评估,分析其特征及规律。研究表明：1）广义的生态用地是指能发挥供给、调节、支持生态系统服务功能,以及对维持区域生态平衡和调节全球气候具有重要作用的土地类型;2）依据“生态干扰度”构建了生态用地分类体系,将生态用地分为3个一级地类、5个二级地类和31个三级地类;3）2012年全国生态用地的生态系统服务价值为280 483.80亿元,呈现“西高、中次、东低”空间格局。2009—2012年全国生态用地的生态系统服务价值整体呈下降趋势,变化幅度空间分布差异较大,呈现“中增、东西减”的格局特点;2009—2012年全国生态用地各项生态系统服务功能受到损失,呈下降趋势,生态系统稳定性不容乐观。     

基于遥感影像的江西省水体资源和水产养殖结构空间异质性分析

为系统掌握江西省水体资源结构和水产养殖基本特征,论文通过遥感技术获取了2012年各县域的水体面积,并划分为不同的水体类型。通过全局和局域空间自相关,分析了89个县（市）水产养殖典型要素的空间异质性以及空间差异程度。针对空间关联及非均质性的现象,运用地理加权回归揭示了水体资源大小、养殖方式、平均单产水平和渔业专业养殖人员数量对养殖产量的影响程度。结果表明：江西省水体资源类型以大水面为主,占总面积的70%,其次为水库山塘,占21.26%,小型池塘面积占9%。水资源结构地区差异明显,北部区域以大水面为主,南部以山塘水库为主。养殖产量和面积表现出空间集聚分布特征（P<0.01）,但各县域的聚集性分布也表现出不同的模式,彭泽县、都昌县、鄱阳县、南昌市辖区、南昌县、丰城市、进贤县和余干县8个县域,均为高-高分布类型,养殖面积和产量分别占到总量的34.55%、35.42%。从养殖品种结构上,特种养殖产量主要集中在上饶市、九江市、南昌市和宜春市,占69.84%,但特种养殖产量所占比例与水体资源大小的相关性下降,水资源较少的东部山区丘陵地带依据区位特征发展鳖、蛙产业,特种养殖比例较高。从水产养殖驱动力分析,水体面积对养殖产量的影响程度最大（中位值为0.46）,其次是小型池塘面积（中位值为0.36）、专业养殖人口数量（中位值为0.26）,3个因素与养殖产量均为正相关,其中水体面积和小型池塘面积对养殖产量的影响程度从南向北递减,专业养殖人口对养殖产量的影响程度从南向北递增。影响程度的空间异质性变化可能与养殖方式和品种结构有关。平均单产水平对养殖产量的贡献较弱（中位值为 -0.003）,各地区影响强度差别不明显。分析结果有助于系统了解江西省水体资源分布和养殖结构,对优化产业规划布局有重要的指导意义。     

1970—2013年西北干旱区空中水汽含量时空变化与降水量的关系

论文基于1970—2013年西北干旱区高空和地面气象资料,采用多种统计学方法,分析了西北干旱区空中水汽含量的时空变化特征及其与降水量的关系。结果表明：1）1970—2002年,西北干旱区空中水汽含量呈显著的增加趋势,速率为0.835 mm/10 a（P<0.01）,其中以夏季增速最高（1.709 mm/10 a,P<0.01）;而降水效率基本稳定,仅春、冬季节略增。在空间上,1970—2002年水汽含量变化速率大小依次为北疆>南疆>河西走廊,其中冬、春季节以北疆水汽增速最大,夏、秋季节以南疆水汽增速最高。2）2003—2013年,西北干旱区水汽含量呈不显著下降趋势（-2.061 mm/10 a）;而降水效率明显增加,速率为0.136%/10 a,这说明近年来空中水汽转化为降水的效率明显提升。同时,北疆降水效率增加幅度明显高于其他地区。3）西北干旱区各季节的降水效率与降水量均呈显著正相关性,而水汽含量与降水量的相关性则表现出明显的季节性差异：春季>夏季>秋季>冬季。另外,新疆降水变化与水汽含量和降水效率均呈显著正相关性,而河西走廊降水量与降水效率的关系更为密切。     

Long-term observations of tropospheric NO2, SO2 and HCHO by MAX-DOAS in Yangtze River Delta area, China

Yangtze River Delta(YRD) area is one of the important economic zones in China. However,this area faces increasing environmental problems. In this study, we use ground-based multi-axis differential optical absorption spectroscopy(MAX-DOAS) network in Eastern China to retrieve variations of NO_2, SO_2, and formaldehyde(HCHO) in the YRD area. Three cities of YRD(Hefei, Nanjing, and Shanghai) were selected for long-term observations. This paper presents technical performance and characteristics of instruments, their distribution in YRD, and results of vertical column densities(VCDs) and profiles of NO_2, SO_2, and HCHO.Average diurnal variations of tropospheric NO_2 and SO_2 in different seasons over the three stations yielded minimum values at noon or in the early afternoon, whereas tropospheric HCHO reached the maximum during midday hours. Slight reduction of the pollutants in weekends occurred in all the three sites. In general trace gas concentrations gradually reduced from Shanghai to Hefei. Tropospheric VCDs of NO_2, SO_2, and HCHO were compared with those from Ozone Monitoring Instrument(OMI) satellite observations, resulting in R~2 of 0.606, 0.5432, and 0.5566, respectively. According to analysis of regional transports of pollutants, pollution process happened in YRD under the north wind with the pollution dissipating in the southeast wind. The feature is significant in exploring transport of tropospheric trace gas pollution in YRD, and provides basis for satellite and model validation.     

Insights into the formation of secondary organic carbon in the summertime in urban Shanghai

To investigate formation mechanisms of secondary organic carbon(SOC) in Eastern China,measurements were conducted in an urban site in Shanghai in the summer of 2015. A period of high O_3 concentrations(daily peak 120 ppb) was observed, during which daily maximum SOC concentrations exceeding 9.0 μg/(C·m~3). Diurnal variations of SOC concentration and SOC/organic carbon(OC) ratio exhibited both daytime and nighttime peaks. The SOC concentrations correlated well with O_x(= O_3+ NO_2) and relative humidity in the daytime and nighttime, respectively, suggesting that secondary organic aerosol formation in Shanghai is driven by both photochemical production and aqueous phase reactions. Single particle mass spectrometry was used to examine the formation pathways of SOC. Along with the daytime increase of SOC, the number fraction of elemental carbon(EC) particles coated with OC quickly increased from 38.1% to 61.9% in the size range of 250–2000 nm, which was likely due to gas-to-particle partitioning of photochemically generated semi-volatile organic compounds onto EC particles. In the nighttime, particles rich in OC components were highly hygroscopic, and number fraction of these particles correlated well with relative humidity and SOC/OC nocturnal peaks. Meanwhile, as an aqueous-phase SOC tracer, particles that contained oxalate-Fe(III) complex also peaked at night. These observations suggested that aqueous-phase processes had an important contribution to the SOC nighttime formation. The influence of aerosol acidity on SOC formation was studied by both bulk and single particle level measurements, suggesting that the aqueous-phase formation of SOC was enhanced by particle acidity.