基于机器学习和卫星遥感的PM2.5/10 空间连续分布反演方法研究

在过去的几十年里,快速的经济发展以及工业化、城镇化进程加速使得中国的资源环境承担的压力不断加大。作为影响空气质量的首要污染物,PM_2.5和PM₁₀（记为PM_2.5/10）直接影响着广大人民群众的身体健康。因此,针对PM_2.5/10浓度进行遥感反演研究,对环境监测和控制改善全国空气环境质量具有重要的意义。近些年来,随着对近地面PM_2.5/10浓度研究的不断深入,基于遥感影像数据进行PM_2.5/10浓度的反演方法也日益增多。本文利用Google Earth engine（GEE）平台获取了海量的Landsat 8 OLI遥感影像数据,并结合气象信息、空间特征等参数,采用机器学习中常用的多层映射反向传播神经网络构建了波段反射率与PM_2.5/10浓度之间的反演模型,以获得PM_2.5/10在研究区域的连续分布。为了提高基础PM_2.5/10反演模型的反演精度,还从影响因素和前溯时间两个维度出发,探寻了模型的最优化输入参数组合,并最终实现了对PM_2.5/10浓度的精准反演。以北京市地区为例,模型的PM_2.5和PM₁₀的反演精度R²分别达到0.814和0.796,均方根误差RMSE分别为19.21 μg?m^?3和28.31 μg?m^?3。鉴于该反演结果具有较高的准确性和可靠性,本文所建立的方法模型为研究PM_2.5/10在空间上的连续分布特征提供了新的思路和方法,具有较为重要的科研意义与广泛的应用价值。     

基于精细化观测的沙尘通量分布特征

研究沙尘随高度的变化特征对揭示沙尘物质在近地层分布特征具有重要意义。为揭示0—80 m沙尘通量的垂直分布规律,在野外实测的基础上,选取2008年7月20日、8月7日、8月19日、8月29日4次沙尘天气,对贴地层（0—0.05 m）、中间层（0.05—2 m）、近地层（2—80 m）的沙尘通量进行对比分析。结果表明：贴地层（0—0.05 m）,沙尘通量随着高度的增高呈增加趋势,最大值为1604.29 g?mm^?2。中间层（0.05—2 m）,沙尘通量随高度分布的关系为幂函数关系,且随着高度的升高沙尘通量减小,决定系数R²值均在0.9以上。近地层（2—80 m）,沙尘通量随高度增加呈分段函数分布,32 m、48 m处为沙尘通量的拐点高度。由此看出,研究沙尘通量对阐明沙尘输送机制非常重要,不仅可加强对沙尘输送的定量研究,还可为沙尘输送的数值模拟提供重要参数。     

雨水管道沉积物沉淀特性及主要污染物含量分布

为研究雨水管道沉积物的沉淀特性和污染物含量特征,在武汉市对建筑(包括住宅小区)、道路和绿地3种用地类型的雨水管道沉积物进行采样和分析.沉速测试结果表明,高沉速颗粒在沉积物中所占比例较大,建筑和道路中沉积物的沉速分布相对稳定,建筑、道路和绿地中沉速大于3.00 cm·s-1的颗粒占比依次递减.粒径分析结果显示,沉积物粒径分布范围较广,大多集中在13~628μm范围内,且同种用地类型沉积物粒径分布差别很大.按沉降速度将每份沉积物样品分为7组,分析化学需氧量(COD)、总氮(TN)和总磷(TP)含量与沉降速度之间的联系.结果表明,沉速大于3.00 cm·s-1和小于0.025cm·s-1的沉积物中污染物含量较低,但高沉速沉积物中污染物总量较多.对沉积物样品整体而言,各用地类型COD含量从高到低依次为:绿地道路建筑;道路雨水管道沉积物中氮含量较低,其余两种用地中含量接近;建筑区雨水管道沉积物中磷含量较高,其余两种用地中含量接近;COD∶TN在(51~89)∶1之间,COD∶TP的值在(102~186)∶1之间.     

Purification and molecular weight distribution of a key exopolysaccharide component of Bacillus megaterium TF10

Extracellular polymeric substances (EPS) are organic metabolic compounds excreted by microorganisms. They largely impact microbial aggregate structures and functions. Extracellular polysaccharides (EP) in EPS are responsible for the formation of microbial aggregates. In this work, we successfully separated and characterized EP from EPS of the bacterium Bacillus megaterium TF10. Extraction of EP from EPS was optimized using Sevag''s reagent. Chemical characteristics, functional groups, and molecular weight (MW) distribu-tion of EP were compared with the harvested EPS and soluble microbial products (SMP). We found that the polymers of lower MW and free proteins were successfully removed by Sevag''s reagent. The higher MW components of EPS were predominantly polysaccharides, while the polymers of lower MW tended to secrete to the supernatant and were described as SMP. A part of the proteins in the EP was polysaccharide-bonded. Our results can be further used in elucidating the complex flocculation mechanisms in which EP play a major role.     

Application of nanoparticle tracking analysis for characterising the fate of engineered nanoparticles in sediment-water systems

Novel applications of nanotechnology may lead to the release of engineered nanoparticles (ENPs), which result in concerns over their potential environmental hazardous impact. It is essential for the research workers to be able to quantitatively characterise ENPs in the environment and subsequently to assist the risk assessment of the ENPs. This study hence explored the application of nanoparticle tracking system (NTA) to quantitatively describe the behaviour of the ENPs in natural sediment-water systems. The NTA allows the measurement of both particle number concentration (PNC) and particle size distribution (PSD) of the ENPs. The developed NTA method was applied to a range of gold and magnetite ENPs with a selection of surface properties. The results showed that the positively-charged ENPs interacted more strongly with the sediment than neutral and negatively-charged ENPs. It was also found that the citrate coated Au ENPs had a higher distribution percentage (53%) than 11-mercaptoundecanoic acid coated Au ENPs (20%) and citrate coated magnetite ENPs (21%). The principles of the electrostatic interactions between hard (and soft) acids and bases (HSAB) are used to explain such behaviours; the hard base coating (i.e. citrate ions) will interact more strongly with hard acid (i.e. magnetite) than soft acid (i.e. gold). The results indicate that NTA is a complementary method to existing approaches to characterise the fate and behaviour of ENPs in natural sediment.     

Characteristics of molecular weight distribution of dissolved organic matter in bromide-containing water and disinfection by-product formation properties during treatment processes

The characteristics of dissolved organic matter (DOM) and bromide ion concentration have a significant influence on the formation of disinfection by-products (DBPs). In order to identify the main DBP precursors, DOM was divided into five fractions based on molecular weight (MW), trihalomethane formation potential and haloacetic acid formation potential were determined for fractions, and the change in contents of different fractions and total DBPs during treatment processes (pre-chlorination, coagulation, sand filtration, disinfection) were studied. Moreover, the relationship between bromide concentration and DBP generation characteristics in processes was also analyzed. The results showed that the main DBP precursors were the fraction with MW < 1 kDa and fraction with MW 3−10 kDa, and the DBP''s generation ability of lower molecular weight DOM (< 10 kDa) was higher than that of higher molecular weight DOM. During different processes, pre-chlorination and disinfection had limited effect on removing organics but could alter the MW distribution, and coagulation and filtration could effectively remove organics with higher MW. For DBPs, trihalomethanes (THMs) were mainly generated in pre-chlorination and disinfection, while haloacetic acids (HAAs) were mostly generated during pre-chlorination; coagulation and sand filtration had little effect on THMs but resulted in a slight removal of HAAs. In addition, the results of ANOVA tests suggested that molecular sizes and treatment processes have significant influence on DBP formation. With increasing bromide concentration, the brominated DBPs significantly increased, but the bromine incorporation factor in the processes was basically consistent at each concentration.     

宜昌市天福庙水库沉积物磷形态分布特征及其释放通量估算

为揭示天福庙水库沉积物中磷的形态及空间分布特征,探讨沉积物-水界面磷的释放通量及其主要影响因素,在天福庙水库库区内设立了6个采样点,采用SMT（磷形态标准测试程序）法测量其沉积物中磷的形态组成,对沉积物磷空间分布、间隙水及上覆水PO₄3-质量浓度变化特征进行了分析,估算了磷释放通量.结果表明:①库区沉积物中TP主要由Ca-P（钙磷）构成,TP在水库库尾和支流入库处具有较高的质量分数,分别为4 904.6、5 015.2 mg/kg.TP、IP（无机磷）、Ca-P时空动态具有一致性,磷矿石灰污染是重要原因.②孔隙水中PO₄3-质量浓度在沉积物表层1~3 cm内存在很高的峰值,达11.3 mg/L,各采样点均高于上覆水中PO₄3-质量浓度,存在向上覆水释放PO₄3-的风险,孔隙水中PO₄3-质量浓度与TP质量分数及磷形态相关.③采用孔隙水扩散模型法估算PO₄3-在沉积物-上覆水界面上的释放通量,库区沉积物磷释放通量范围为0.13~3.08 mg/（m2·d）,平均值为1.03 mg/（m2·d）,处于较高水平.研究显示,磷矿开采是干流沉积物磷来源和形态组成的重要原因,库区磷释放通量与水流扰动密切相关,坝前、支流交汇处、库尾是库区内源磷污染的主要区域.      

北京冬春和夏初季节大气O3浓度的垂直分布特征

为探究北京地区不同季节大气O₃浓度垂直分布特征,于2010年12月1日—2011年3月31日（冬春季）和2011年5月7日—6月9日（夏初）,在北京北部地区的中国环境科学研究院内,利用第三代移动式大气环境激光雷达系统,对$\varphi $（SO₂）、$\varphi $（NO₂）以及$\varphi $（O₃）和气溶胶后向散射系数垂直方向和垂直剖面进行试验观测,并结合天气要素的变化进行了分析研究.结果表明:①$\varphi $（O₃）存在明显的季节变化,表现为夏季>春季>冬季,同时晴天、微风、逆温条件等气象背景是O₃污染过程出现的主要气象因素,在微风和南风的情况下,会出现高$\varphi $（O₃）带,在北风影响情况下,$\varphi $（O₃）相对较低,雨水冲洗的作用对$\varphi $（O₃）分布也有明显的影响;②$\varphi $（O₃）的日变化曲线呈单峰单谷型,$\varphi $（O₃）峰值一般出现在14:00—18:00之间,谷值则出现在22:00—翌日09:00之间;③$\varphi $（O₃）垂直分布呈现单峰、双峰、多峰型分布等多种垂直分布特征,10 km以上高空这3种分布特征均有出现,但是在5 km以下的近地面$\varphi $（O₃）垂直和斜程分布基本呈现多峰型,斜程方向上$\varphi $（O₃）的高低与下垫面及其所排放的O₃前体物有密切的关系;④$\varphi $（O₃）垂直分布呈现一定的不均匀性,其数值范围浮动比较小,最大值之间相差30×10-9.研究显示,$\varphi $（O₃）垂直规律主要表现出两种分布特征,一种是在3~5 km处有高浓度的堆积区,另一种则没有明显高值堆积区.      

FeCl3改性MOFs在低温下对Hg0的吸附性能

为提高吸附剂对Hg0（零价汞）的吸附效率,利用MOFs（金属有机框架）材料发达的孔隙结构和高比表面积（1 997.010 0 m2/g）,采用FeCl₃溶液浸渍改性,制备了吸附剂FeCl₃@MIL-101（Cr）用于脱除Hg0.在小型固定床反应器上考察了浸渍浓度、反应温度、氧含量等对Hg0去除的影响.结果表明:FeCl₃@MIL-101（Cr）在进口ρ（Hg0）为2×10-3 mg/L,c（FeCl₃）为0.2 mol/L,反应温度60℃,气体流速400 mL/min,φ（O₂）为1%的条件下,吸附穿透时间长达62 h,相应的吸附容量为14.27 mg/g.在此基础上,进一步利用BET（比表面积测试）、SEM（扫描电镜）-EDX（能量色散X射线光谱）、XRD（X射线衍射）、XPS（X射线光电子能谱）等常用表征手段研究了改性前后吸附剂的物理化学特性,证明了吸附剂FeCl₃@MIL-101（Cr）吸附零价汞是物理吸附与化学吸附共同作用的结果,含氯官能团在吸附Hg0过程中也发挥了相当大的作用,并且氧气可促进其吸附效果.最后,分析了其吸附机理.研究显示,该种吸附剂在低温条件下具有较为优良的脱汞性能,应用前景良好.      

厌氧条件下可溶性有机质对汞的还原与氧化作用

在沉积物、湿地和淹水的水稻土中天然可溶性有机质(DOM),如胡敏酸(HA)和富里酸(FA)处于还原状态,其介导Hg(Ⅱ)的还原,影响汞的转化及地球化学循环.本文通过模拟黑暗厌氧环境,研究还原态HA与FA对Hg(Ⅱ)的还原.结果表明,还原态HA与FA的还原容量高于对照氧化态HA与FA.还原态HA与FA对Hg(Ⅱ)的还原最佳浓度分别是0. 2mg·L~(-1)和1. 5 mg·L~(-1).而高于最佳浓度时,由于发生巯基竞争性络合作用,抑制Hg(Ⅱ)的还原;特别是还原态HA大于5mg·L~(-1)时,不能还原Hg(Ⅱ)为Hg(0).还原态HA与FA对Hg(Ⅱ)的还原反应动力学表明:有机碳(DOC)与Hg(Ⅱ)摩尔比DOC∶Hg(Ⅱ)=400∶1时,还原反应速率IHSS-HA FRC-HA FRC-FA;高摩尔比[DOC∶Hg(Ⅱ)=10 000∶1]时,还原态HA对Hg(Ⅱ)的还原反应停止,甚至向相反方向进行.还原态HA与FA对Hg(0)氧化结果表明,当还原态HA与FA浓度分别增加至5 mg·L~(-1)和10 mg·L~(-1)时,样品中检测不到Hg(0),还原态HA与FA对Hg(0)发生诱导性氧化络合作用.在汞的氧化还原与络合作用中,还原态DOM扮演双重角色,影响活性汞的可利用性,进而影响微生物汞的甲基化.