基于OMI数据的东南沿海大气臭氧浓度时空分布特征研究

基于臭氧监测仪(OMI)卫星反演数据,对2005—2018年东南沿海5省区域大气臭氧柱浓度数据进行提取及分析,探讨其时空分布格局及影响因素.结果表明:①在时间变化上,14年间,该区域大气臭氧柱浓度整体呈先上升后下降的趋势,2005—2013年臭氧柱浓度持续升高,最高值为324.52 DU,高值区不断向南部区域扩大;2013—2018年臭氧柱浓度呈下降趋势,最低值为228.27 DU,但在2017、2018年略有上升.②在空间分布上,臭氧柱浓度自北向南逐渐降低,高值区集中分布在江苏及浙江省北部;低值区集中于福建省南部及广东省大部分地区.③在季节变化上,大体呈现出春夏季高于秋冬季,高值区在春夏季交替出现,秋季略高于冬季,但差异不明显.④稳定性分析表明:研究区臭氧柱浓度整体呈现中部分散、南北部集聚、差异较显著的分布格局.⑤自然因素中,风向、气温均呈现显著正相关,江淮地区的梅雨季节(降水)及华南地区的台风和暴雨也起到显著作用.⑥人文因素中,臭氧柱浓度与地区生产总值、各产业生产总值及机动车保有量均表现出正相关,其中,臭氧柱浓度与第二产业的相关度最高.另外,臭氧柱浓度与NO_x排放量表现出显著相关性.VOC_s对臭氧柱浓度的影响中,工业源是主控因素,交通源和居民源次之,电厂源对臭氧柱浓度的影响最弱.这进一步说明臭氧浓度的变化受到了诸多因素的综合影响,但气温、NO_x及VOC_s的排放是臭氧浓度变化的主导因素.     

模拟土壤淋洗废液中重金属的选择性去除与淋洗液的回收研究

土壤淋洗废液中污染物的选择性去除是实现淋洗液回收的关键.本文以硫化钠（Na₂S）、乙基黄原酸钾（PEX）、二甲基二硫代氨基甲酸钠（DTC）作为重金属沉淀剂处理电子垃圾污染土壤模拟淋洗废液,在筛选出Na₂S作为理想重金属沉淀剂的基础上,研究初始pH值、反应温度、沉淀剂浓度等因素对Na₂S分离络合态重金属的影响,并通过软件模拟和产物表征等方式推测反应机理.结果表明：Na₂S对柠檬酸络合态重金属的分离顺序依次为Cu、Pb、Cd,符合硫化物溶度积原则;反应温度、初始pH值对Na₂S处理络合态重金属无显著影响,重金属去除率均保持在90%以上,柠檬酸的回收率约为95%;Visual MINTEQ模拟结果显示,S^2-投加前液相中重金属主要以H₂CA^-、HCA^2-和CA^3-结合形式存在,S^2-投加后液相中重金属则以HS^-和S^2-结合形式存在;扫描电镜及能谱（SEM-EDS）表明,S^2-与金属阳离子按物质的量比1：1生成硫化物沉淀物,沉淀主要呈团聚、成簇和圆片状存在;X射线衍射（XRD）分析结果表明,沉淀产物中存在CuS、CdS、PbS和CuPbS₂.本研究结果可为化学沉淀法处理重金属污染土壤淋洗废液提供技术参考.     

Mechanism and catalytic performance for direct dimethyl ether synthesis by CO2 hydrogenation over CuZnZr/ferrierite hybrid catalyst

Direct synthesis of dimethyl ether(DME) by CO_2 hydrogenation has been investigated over three hybrid catalysts prepared by different methods:co-precipitation,sol-gel,and solid grinding to produce mixed Cu,ZnO,ZrO_2 catalysts that were physically mixed with a commercial ferrierite(FER) zeolite.The catalysts were characterized by N_2 physisorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),temperature programmed desorption of CO_2(CO_2-TPD),temperature programmed desorption of NH_3(NH_3-TPD),and temperature programmed H2 reduction(H_2-TPR).The results demonstrate that smaller CuO and Cu crystallite sizes resulting in better dispersion of the active phases,higher surface area,and lower reduction temperature are all favorable for catalytic activity.The reaction mechanism has been studied using in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).Methanol appears to be formed via the bidentate-formate(b-HCOO) species undergoing stepwise hydrogenation,while DME formation occurs from methanol dehydration and reaction of two surface methoxy groups.     

Advanced molecular-fingerprinting analysis of dissolved organic sulfur by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry using optimal spray solvent

Molecular level characterization of dissolved organic sulfur (DOS) by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR MS) is necessary for further understanding of the role of DOS in the environment. Here, ESI spray solvent, a key parameter for ion production during ESI process, was investigated for its effect on the molecular characterization of DOS by ESI-FTICR MS. 100% MeOH as spray solvent was found for the first time to remarkably enhance the ionization efficiency of the majority of CHOS-molecules in NOM, which facilitated a total of 1473 CHOS-molecular formulas with one sulfur atom to be detected. The number of CHOS-molecular formulas obtained using 100%MeOH as spray solvent increased notably over 740 in comparison with those using 50% MeOH aqueous solution (731) or 50% ACN aqueous solution (653). Moreover, due to the enhancement of ionization efficiency of DOS during ESI processes, the tandem mass spectra of the NOM CHOS-molecules could be easily obtained using 100% MeOH as spray solvent, which were hardly obtained using 50% MeOH aqueous solution as spray solvent. The results of the tandem mass spectra suggested the first discovery of organosulfates or sulfonic acids in Suwannee River NOM sample. A simple method based on 100% MeOH as ESI spray solvent for advanced molecular characterization of DOS by ESI-FTICR MS was proposed and applied, and the results revealed more molecular information of DOS in sea DOM samples.     

On-going nitrification in chloraminated drinking water distribution system (DWDS) is conditioned by hydraulics and disinfection strategies

Within the drinking water distribution system (DWDS) using chloramine as disinfectant, nitrification caused by nitrifying bacteria is increasingly becoming a concern as it poses a great challenge for maintaining water quality. To investigate efficient control strategies, operational conditions including hydraulic regimes and disinfectant scenarios were controlled within a flow cell experimental facility. Two test phases were conducted to investigate the effects on the extent of nitrification of three flow rates (Q = 2, 6, and 10 L/min) and four disinfection scenarios (total Cl₂=1 mg/L, Cl₂/NH₃-N=3:1; total Cl₂=1 mg/L, Cl₂/NH₃-N=5:1; total Cl₂=5 mg/L, Cl₂/NH₃-N=3:1; and total Cl₂=5 mg/L, Cl₂/NH₃-N=5:1). Physico-chemical parameters and nitrification indicators were monitored during the tests. The characteristics of biofilm extracellular polymetric substance (EPS) were evaluated after the experiment. The main results from the study indicate that nitrification is affected by hydraulic conditions and the process tends to be severe when the fluid flow transforms from laminar to turbulent (2300<Re<4000). Increasing disinfectant concentration and optimizing Cl₂/NH₃-N mass ratio were found to inhibit nitrification to some extend when the system was running at turbulent condition (Q = 10 L/min, Re = 5535). EPS extracted from biofilm that was established at the flow rate of 6 L/min had greater carbohydrate/protein ratio. Furthermore, several nitrification indicators were evaluated for their prediction efficiency and the results suggest that the change of nitrite, together with total organic carbon (TOC) and turbidity can indicate nitrification potential efficiently.     

Concentrations and chemical compositions of PM10 during hazy and non-hazy days in Beijing

In order to study the concentrations of major components,characteristics and comparison in hazy and non-hazy days of PM_(10) in Beijing,aerosol samples were collected at urban site in Beijing from December 29,2014 to January 22,2015.Heavy metals like Zn,Pb,Mn,Cu,As,V,Cr and Cd were deeply studied considering their toxic effects on human being;nine water-soluble inorganic ions(SO_4~(2-),NO_3~-,NH_4~+,Na~+,K~+,Cl~-,Ca~(2+) and Mg~(2+)) and carbon fractions(OC and EC) were also analyzed.The concentrations of heavy metals were 1.03–1.98 times higher in hazy days than those in non-hazy days,mainly due to biomass burning and coal burning.The trends in total heavy metals concentrations were basically consistent with the trends in PM concentrations except for two obvious periods(12.29–12.30;1.14–1.15);but when air masses accumulated locally or around Beijing,trends in PM concentrations and heavy metals were opposite.The proportion for NO_3~-/SO_4~(2-) indicated that mobile sources such as automobiles were important reasons for haze in Beijing.Correlation between OC and EC during non-hazy days was strong(R~2= 0.95) but it was low(R~2= 0.67) during hazy days,and large variations for OC/EC values occurred in hazy days.The calculated mass concentration of SOC is 2.58 μg/m~3,which only accounted for 10.1% of the OC concentration.When air masses from the far north-west,they decreased PM concentration in Beijing and they were relatively clean;however,those from the near east,south-east and south of the mainland increased PM concentration and they were dirty.     

典型西南工业城市春冬季PM2.5来源与潜在源区分析——以柳州市为例

为了揭示柳州城区春冬季PM_2.5的来源及其潜在源区分布和贡献,利用2018年24h自动监测数据和气象数据对柳州市大气污染物浓度变化特征进行了分析,并且使用后向轨迹模型（HYSPLIT）对春冬季柳州市PM_2.5逐日72h气流后向轨迹和前向轨迹进行聚类分析,同时结合潜在源贡献因子分析法（WPSCF）和轨迹浓度权重法（WCWT）对其潜在源区和浓度贡献进行了分析.结果显示,（1）在研究期内,不利的主导风向和工业区布局导致研究区PM_2.5在春冬季污染较严重,且工业源和交通源是其主要本地来源;（2）春冬季PM_2.5高值主要来源于西北和东南方向,其中,西北向PM_2.5主要来源于本地排放,且浓度在空间上呈现西高东低的趋势;（3）春季后向轨迹PM_2.5浓度整体大于冬季,春冬季中对柳州市PM_2.5影响最大轨迹均来自东部的短距离输送,而来自西北的气流轨迹输对PM_2.5贡献最低.春冬季柳州市大气PM_2.5通过气流传输对贵州地区大气环境有较大影响;（4）春季,柳州市PM_2.5的主要潜在源区分布在广西东南部、广东中西部、南海沿岸海域、湖南中部、江西西北部、湖北东部及安徽西北部;冬季,主要分布在广西东南部、广东西南部和南海沿岸海域.     

Heterogeneity in the relationship between carbon emission performance and urbanization: evidence from China

Mitigation and Adaptation Strategies for Global Change - Global change caused by carbon emissions alone has become a common challenge for all countries. However, current debates about urbanization...     

一种模拟动力学边界条件的环境振动试验方法研究

目的提高环境振动试验的可靠性。方法以某典型钛合金蜂窝夹芯壁板试验件为例,提出一种模拟试验件动力学边界条件的试验方法,在试验件周围引入弹性连接件,再通过刚性转接工装与振动台台面连接,以试验件在试验安装状态下的共振频率及振型节线位置为优化目标,以弹性连接件的外形尺寸及厚度为优化变量,对弹性连接件进行优化设计,从而模拟试验件真实的动力学边界条件。结果弹性连接件的优化设计使得试验件在试验安装状态下前两阶共振频率与试验要求相差小于8%,而且振型节线位置与试验要求基本重合,达到了模拟试验件真实动力学边界条件的设计目标。结论对于壁板类试验件,在传统刚性夹具的基础上引入弹性连接件的试验方法,可以较好地模拟试验件真实动力学边界条件,提高环境振动试验的可靠性,并且这种方法对试验费用及试验周期影响较小,具有良好的工程应用前景。     

乌鲁木齐市汽车尾气污染状况调查

对乌鲁木齐市主要街道受汽车尾气污染的调查和综合分析得到CO、NOx、HC的污染规律,主要街道路中心空气中CO、NOx日均值已超出国家大气环境质量二级标准,市区主要街道的人行道空气中NOx含量已超出二级标准,Ⅱ、Ⅲ类道路人行道空气中CO含量已超标;在三类街道中,Ⅰ类街道车流量最大,Ⅱ类次之,Ⅲ类最少,而汽车排放尾气对街道空气污染状况为Ⅲ类最重、Ⅱ类次之、Ⅰ类最轻。