我国中部地区大气CO2柱浓度时空分布

基于日本GOSAT及美国AIRS反演数据产品,对我国中部六省大气CO₂时空分布特征进行研究,结果表明：由GOSAT反演的中部地区2010~2013年大气CO₂年均柱浓度由389.36×10^-6增长到396.52×10^-6,年均绝对增长率达2.39×10^-6/a,呈现出冬春季高值、夏秋季低值的季节变化特征,其柱浓度年均值及去长期趋势后的月均值均略低于长三角地区,高于京津冀和东三省地区;其CO₂柱浓度高值区集中在湖南、江西及周边一带,年均绝对增长率为2.01×10^-6,其柱浓度年均值及去长期趋势后的月均值与长三角地区相当,略低于京津冀和东三省地区,由于受地面源汇影响较小,其与GOSAT反演结果相反,可能是由于AIRS反映了对流层中层大气状况,而GOSAT则更多地反映了近地面层大气CO₂变化.     

邻苯二甲酸二丁酯降解过程的单体同位素分析

研究对比了邻苯二甲酸二丁酯（DBP）在不同降解过程（水解、UV/H₂O₂光解、直接光解、过硫酸钾光氧化）中的碳、氢同位素组成变化、分馏特征及二维同位素（Δδ²H-Δδ¹³C）的相关性.水解反应中DBP分子产生了显著的碳同位素分馏,未发现氢同位素分馏,而且碳同位素富集因子ε_C为（-2.7±0.4）‰,表明DBP水解时发生C-O键断裂,氢原子不参与反应.而UV/H₂O₂光解和直接光解反应（pH值分别为2、7和10）中,DBP分子呈现了相似的二维同位素相关性Λ值[（9±2）~（11±2）],推测经历了相同的反应过程.过硫酸钾光氧化降解时,明显偏大的Λ值（31±3）说明反应可能发生C-H键断裂.结果表明：二维单体同位素分析（2D-CSIA）技术可以有效区分DBP的水解、光解、光氧化3种不同类型的降解过程,有助于分析其降解路径.     

兰州市南山季节性土壤微生物特征及影响因素

为了探究不同季节和不同植被类型对土壤微生物分布的影响,以兰州市南山不同海拔的两种植被类型为研究对象,采用稀释涂布平板法测定了土壤微生物的季节动态变化特征.结果表明：研究区内细菌数量占微生物总数的96.22%~99.80%,远高于真菌和放线菌数量.土壤微生物类群随季节变化呈现明显差异,其总数整体表现为夏季最高,为89.22×10⁶cfu/g soil,分别是春、秋、冬季的12.02、3.28、2.74倍,其中夏季细菌数量最高,真菌与放线菌数量均在春季达到最大值.人工林样地土壤微生物数量略低于荒坡,环境因子中土壤含水量和有机碳含量高于荒坡.随着海拔的升高,pH值逐渐上升,土壤温度、有机碳与全氮含量逐渐下降,土壤微生物总数则呈现先减少后增加的趋势.相关分析表明,不同季节各微生物类群与环境因子的相关系数各有不同,春季放线菌与有机碳,秋季真菌与有机碳、全氮均呈极显著正相关（P<0.01）.冗余分析表明,环境因子中有机碳与第一物种轴的相关系数最高,为0.520,说明土壤有机碳含量是影响土壤微生物类群分布的主导因素.     

近10年中国三大经济区太阳总辐射特征及其与O3、PM2.5的关系

采用中国地面气象观测站网2007~2016年的辐射日值数据集和中国空气质量在线监测平台2014~2016年逐日观测数据,分析了京津冀、长三角和珠三角近10a太阳总辐射年际和季节变化,近3a臭氧日最大8h平均（O_{3_8h_max}）和细颗粒物（PM_2.5）的污染过程频次变化,通过不同因子及其不同强度等级的分型统计,探讨PM_2.5、O_{3_8h_max}与太阳总辐射的关系.结果表明：京津冀近10a太阳总辐射显著上升,京津冀春季和珠三角夏季太阳总辐射显著上升.三大经济区PM_2.5污染过程年频次均呈现逐年递减,且从北到南递减;O₃污染过程年频次时间上呈现先减后增,空间上京津冀多于长三角和珠三角.三大经济区O_{3_8h_max}与太阳总辐射相关系数均在0.71以上,有较强的正相关;而PM_2.5与太阳总辐射的相关性具有区域差异性.三大经济区不同季节不同太阳总辐射下O_{3_8h_max}与PM_2.5的相关关系差异显著,其中京津冀春夏秋三季O_{3_8h_max}与PM_2.5在强太阳总辐射下有较好的正相关,冬季则存在一定的负相关;长三角四季两者相关性均较弱;珠三角夏季两者正相关最为显著;不同PM_2.5浓度下O_{3_8h_max}与太阳总辐射的线性拟合效果较好,体现出较强的正相关关系,各经济区拟合曲线的倾向率均随PM_2.5升高而增大.PM_2.5>75μg/m³时拟合优度均达到最大.     

考虑边界条件不确定性的地下水污染风险分析

为分析边界条件不确定性对地下水污染质运移数值模拟模型输出结果的影响,运用Monte Carlo方法对一算例进行阐明,并从污染风险预报方面对模拟结果进行分析.为减少重复调用模拟模型产生的大量计算负荷,将边界条件（第一类边界条件-水头值）作为随机变量,建立地下水污染质运移数值模拟模型的Kriging替代模型,在保证较高精度的同时,实现了Monte Carlo模拟.结果表明：边界条件的不确定性,对地下水污染质运移数值模拟模型预报的结果有很大影响,考虑与未考虑边界条件不确定性得到的研究区污染羽分布差别较大.对地下水污染质运移数值模拟模型的Monte Carlo模拟结果进行统计与分析,可以评估研究区观测井1,2,3污染物浓度预报结果的可靠程度,并且可以预报出研究区观测井1,2,3遭受不同程度污染的风险.     

应用S-T模型对沉积物中PAHs的生态风险分级评价

本文构建S-T模型,运用集对分析理论（set pair analysis）构建基本模型,采用层次分析法并参考毒性当量因子确定各指标权重,应用三角模糊数（triangular fuzzy number）对差异度系数进行改进,基于加拿大沉积物环境质量标准,对沉积物中多环芳烃进行生态风险分级评价.结果表明,该模型考虑到化合物之间的相互作用因素并做模糊处理,对差异度系数进行改进体现沉积物中多环芳烃生态风险等级标准的模糊性,为持久性有机污染物生态风险分级评价提供了一种简便客观有效的方法.     

Nanoencapsulation of hexavalent chromium with nanoscale zero-valent iron: High resolution chemical mapping of the passivation layer

Solid phase reactions of Cr(Ⅵ) with Fe(0) were investigated with spherical-aberration-corrected scanning transmission electron microscopy(Cs-STEM) integrated with X-ray energy-dispersive spectroscopy(XEDS). Near-atomic resolution elemental mappings of Cr(Ⅵ)–Fe(0) reactions were acquired. Experimental results show that rate and extent of Cr(Ⅵ) encapsulation are strongly dependent on the initial concentration of Cr(Ⅵ) in solution. Low Cr loading in nZⅥ(1.0 wt%) promotes the electrochemical oxidation and continuous corrosion of n ZⅥ while high Cr loading(1.0 wt%) can quickly shut down the Cr uptake. With the progress of iron oxidation and dissolution, elements of Cr and O counter-diffuse into the nanoparticles and accumulate in the core region at low levels of Cr(Ⅵ)(e.g., 10 mg/L). Whereas the reacted n ZⅥ is quickly coated with a newly-formed layer of 2–4 nm in the presence of concentrated Cr(Ⅵ)(e.g., 100 mg/L). The passivation structure is stable over a wide range of pH unless pH is low enough to dissolve the passivation layer. X-ray photoelectron spectroscopy(XPS) depth profiling reconfirms that the composition of the newly-formed surface layer consists of Fe(Ⅲ)–Cr(Ⅲ)(oxy)hydroxides with Cr(Ⅵ) adsorbed on the outside surface. The insoluble and insulating Fe(Ⅲ)–Cr(Ⅲ)(oxy)hydroxide layer can completely cover the n ZⅥ surface above the critical Cr loading and shield the electron transfer. Thus, the fast passivation of nZⅥ in high Cr(Ⅵ) solution is detrimental to the performance of nZⅥ for Cr(Ⅵ) treatment and remediation.     

Mercury flows in large-scale gold production and implications for Hg pollution control

Large-scale gold production(LSGP) is one of the five convention-related atmospheric mercury(Hg) emission sources in the Minamata Convention on Mercury. However, field experiments on Hg flows of the whole process of LSGP are limited. To identify the atmospheric Hg emission points and understand Hg emission characteristics of LSGP, Hg flows in two gold smelters were studied. Overall atmospheric Hg emissions accounted for 10%–17% of total Hg outputs and the Hg emission factors for all processes were 7.6–9.6 kg/ton. There were three dominant atmospheric Hg emission points in the studied gold smelters, including the exhaust gas of the roasting process, exhaust gas from the environmental fog collection stack and exhaust gas from the converter of the refining process. Atmospheric Hg emissions from the roasting process only accounted for 16%–29% of total emissions and the rest were emitted from the refining process. The overall Hg speciation profile(gaseous elemental Hg/gaseous oxidized Hg/particulate-bound Hg) for LSGP was 34.1/57.1/8.8. The dominant Hg output byproducts included waste acid, sulfuric acid and cyanide leaching residue. Total Hg outputs from these three byproducts were 80% in smelter A and 84% in smelter B. Our study indicated that previous atmospheric Hg emissions from large-scale gold production might have been overestimated.Hg emission control in LSGP is not especially urgent in China compared to other significant emission sources(e.g., cement plants). Instead, LSGP is a potential Hg release source due to the high Hg output proportions to acid and sludge.     

Relationship between PM10 and PM2.5 levels in high-traffic area determined using path analysis and linear regression

The objective of this study was to determine the relationship between PM_(10) and PM_(2.5) levels as related to meteorological conditions and traffic flow using both a linear regression analysis and a path analysis. The Particulate matter(PM) samples were collected from Sukhumvit road, Bangkok, Thailand, at both open(104 samples) and covered(92 samples)areas along the road. Fifteen percent of all samples were separated before the statistical models were run and used for model validation. The results from the path analysis were more elaborate than those from the linear regression, thus indicating that meteorological conditions had a direct effect on the particulate levels and that the effects of traffic flow were more variable in open areas. The model also indicated that meteorological conditions had an indirect effect and that traffic flow had a direct effect on particulate levels in covered areas. The model validation results indicated that for open areas, the R~2 values were not very different between the path analysis and the linear regression model, but that the path analysis was more accurate than the linear regression model at very low PM concentrations. At high PM concentrations, the path analysis model also had a better fit than did the linear regression, so the predictions from the path analysis model were more accurate than those from the linear regression.     

Seasonal variation and size distribution of biogenic secondary organic aerosols at urban and continental background sites of China

Size-resolved biogenic secondary organic aerosols(BSOA) derived from isoprene and monoterpene photooxidation in Qinghai Lake, Tibetan Plateau(a continental background site) and five cities of China were measured using gas chromatography/mass spectrometry(GC/MS). Concentrations of the determined BSOA are higher in the cities than in the background and are also higher in summer than in winter. Moreover, strong positive correlations(R2= 0.44–0.90) between BSOA and sulfate were found at the six sites,suggesting that anthropogenic pollution(i.e., sulfate) could enhance SOA formation,because sulfate provides a surface favorable for acid-catalyzed formation of BSOA. Size distribution measurements showed that most of the determined SOA tracers are enriched in the fine mode( 3.3 μm) except for cis-pinic and cis-pinonic acids, both presented a comparable mass in the fine and coarse( 3.3 μm) modes, respectively. Mass ratio of oxidation products derived from isoprene to those from monoterpene in the five urban regions during summer are much less than those in Qinghai Lake region. In addition, in the five urban regions relative abundances of monoterpene oxidation products to SOA are much higher than those of isoprene. Such phenomena suggest that BSOA derived from monoterpenes are more abundant than those from isoprene in Chinese urban areas.