典型西南工业城市柳州市核心区大气污染物时空分布与气象因素研究

为研究柳州市核心区大气污染物浓度时空变化规律与气象因素之间的关系,统计分析了2018年全年研究区内6个自动监测站点PM_(2.5)、PM_(10)、SO_2、NO_2、O_3和CO的浓度监测数据和气象站气象数据,并对28次超标日污染物来源进行了解析.结果显示:①核心区颗粒污染物污染较为严重,且以PM_(2.5)为主的细颗粒污染物仍为柳州市主要的大气污染物;各污染物月均浓度季节差异显著,除NO_2外柳州大气污染物浓度下降明显,指示柳州市多项节能减排综合整治措施成效显著;PM_(2.5)、PM_(10)、CO受早晚高峰期影响,浓度日变化均呈双峰型;NO_2在不同季节峰型不同,作为O_3前体物其浓度日变化与O_3相反,呈现"早峰午谷"的变化趋势.②通过对污染物浓度插值发现,由于核心区主要工商业区位于西部且处于主导风向下风向,故PM_(2.5)和SO_2浓度西北高、东南低,PM_(10)、NO_2和CO浓度西南高、东北低;核心区东部的山区为O_3生成带来大量前体物,使O_3浓度东南高、西北低.③由于气候特征,核心区春、夏季主要气象因素均为降水量;秋季的主要气象因素是风速,风速与污染物的负相关关系表明了风的扩散效应;冬季大部分污染物与气象因素的相关性不显著,表明人为因素对污染物的影响大于气象因素;核心区大气污染物主要来源于局地排放和区域传输,且南北主导风向对大气污染影响最大.④HYSPLIT模型结果指示柳州超标日大气污染物主要来自于珠三角地区,且陆源颗粒物浓度普遍比海洋源高,来自南部的远距离输送气流颗粒物含量最低,表明远距离输送为影响颗粒物传播的主要原因.     

泗顶矿区6种土地利用类型土壤微生物群落结构特征

以广西柳州泗顶铅锌矿区的玉米地、菜地、灌木、尾矿库、森林和柑橘园6种不同利用类型土壤为研究对象,采用高通量测序技术,分析了不同土地利用类型土壤微生物群落结构特征及土壤环境因子对微生物群落结构的影响.结果表明,变形菌门（Proteobacteria）是6种土壤的优势菌门,所占比例为31.34%~53.47%,γ-变形菌纲（Gammaproteobacteria）为优势菌纲.冗余分析表明,在重金属含量最高的灌木区,厚壁菌门（Firmicutes）和拟杆菌门（Bacteroidetes）的丰度与土壤中铅、锌、镉、铜的含量呈现显著正相关;在土壤钠和钾含量较高的玉米地和菜地,浮霉菌门（Planctomycetes）的丰度有所增加,而厚壁菌门和拟杆菌门的丰度则有所下降.在土壤有机质含量较高而总氮、总磷含量较低的柑橘园,酸杆菌门（Acidobacteria）和疣微菌门（Verrucomicrobia）的丰度较高.芽单胞菌门（Gemmatimonadetes）和浮霉菌门的丰度与土壤pH值呈显著正相关.研究结果表明土地利用类型及土壤环境因子对土壤微生物群落结构多样性有显著的影响.     

节水灌溉措施下湘东北丘陵林-稻汇水区复合系统铅的迁移

铅通过食物链的迁移和积累对人类健康的毒害作用日益为社会所重视,而水稻是人类铅摄入的主要途径之一,因此,对稻田土壤铅的迁入途径及其过程特征的研究十分必要.为了探明湖南地区远离城镇、工矿区的丘陵稻区铅的输入、迁移、滞留机制,选择位于湘东北地域的汩罗市桃林林场的林地-山塘-稻田汇水区系统作为研究对象,在水稻大田生长期间,原位研究其大气沉降、岗地径流、山塘水、稻田水、水稻生长等过程的铅通量.结果表明：①输入系统的铅源是大气沉降,其中,在水稻生育前期通过东南季风输入的区域外源铅占90%;②山塘是大气沉降铅的主要集纳地貌单元,存留了大气沉降输入岗地和山塘总铅的66%;③林-稻汇水区系统岗地铅净留存28.8~57.7 g·hm^-2,山塘铅净留存604.3~961.9 g·hm^-2,稻田铅净留存89.6~90.9 g·hm^-2;而对照系统岗地铅净输出173.3 g·hm^-2,山塘净留存3427.6 g·hm^-2,稻田净留存87.1 g·hm^-2;④岗地和山塘对铅的截留量能够互补;⑤从岗地通过径流-山塘水过程迁移到稻田的大分子有机物能够增强稻田对铅的截留.综上所述,丘陵林-稻汇水区系统中铅的循环与大气沉降有关,系统内岗地森林类型、郁闭度、降水产流及泥沙、有机物的输出都会影响铅在系统中的迁移和分配.     

滇黔桂岩溶区河漫滩土壤重金属含量、来源及潜在生态风险

利用全国地球化学基准计划在滇黔桂岩溶区35个点位采集的70件河漫滩表、深层土壤样品,分析了As、Cd、Cr、Cu、Hg、Ni、Pb和Zn 8种重金属元素含量特征,探究了重金属来源、污染状况及潜在生态风险.结果表明,8种重金属元素含量大部分均高于全国土壤背景值,在滇东南地区含量最高,桂西北地区最低.表层土壤Cd、Hg明显富集,As、Cr、Cu、Ni与深层土壤含量相当;As、Cd、Hg、Pb、Zn在农田、菜地中明显高于深层土壤,Cr、Cu和Ni在各类土地中与深层土壤相当.因子分析结果显示,表层土壤中Cd、Cr、Cu、Ni受地质背景控制,As、Pb、Zn既与地质背景有关,也受人为活动影响,Hg受人为活动影响较严重;深层土壤中Cd、Cr、Cu、Ni、Cr、Zn继承了区域母岩特征,As、Hg和Pb受地质背景和人为活动双重影响.地累积指数法和富集因子法污染评价结果表明,研究区河漫滩表层土壤中Cd、Hg污染较重,As、Cr、Cu、Ni、Pb、Zn大部分为轻度污染或无污染.各重金属潜在生态风险指数高低顺序依次为Hg > Cd > As > Cu > Ni > Pb > Cr > Zn,Cd和Hg的生态风险指数之和占综合指数的82.43%,生态风险最高;滇东南地区重金属潜在风险综合指数最高,具重度生态风险.     

Density functional theory (DFT) studies of vanadium-titanium based selective catalytic reduction (SCR) catalysts

Based on density functional theory (DFT) and basic structure models, the chemical reactions on the surface of vanadium-titanium based selective catalytic reduction (SCR) denitrification catalysts were summarized. Reasonable structural models (non-periodic and periodic structural models) are the basis of density functional calculations. A periodic structure model was more appropriate to represent the catalyst surface, and its theoretical calculation results were more comparable with the experimental results than a non-periodic model. It is generally believed that the SCR mechanism where NH₃ and NO react to produce N₂ and H₂O follows an Eley-Rideal type mechanism. NH₂NO was found to be an important intermediate in the SCR reaction, with multiple production routes. Simultaneously, the effects of H₂O, SO₂ and metal on SCR catalysts were also summarized.     

Recent advances in catalytic decomposition of ozone

Ozone (O₃), as a harmful air pollutant, has been of wide concern. Safe, efficient, and economical O₃ removal methods urgently need to be developed. Catalytic decomposition is the most promising method for O₃ removal, especially at room temperature or even subzero temperatures. Great efforts have been made to develop high-efficiency catalysts for O₃ decomposition that can operate at low temperatures, high space velocity and high humidity. First, this review describes the general reaction mechanism of O₃ decomposition on noble metal and transition metal oxide catalysts. Then, progress on the O₃ decomposition performance of various catalysts in the past 30 years is summarized in detail. The main focus is the O₃ decomposition performance of manganese oxides, which are divided into supported manganese oxides and non-supported manganese oxides. Methods to improve the activity, stability, and humidity resistance of manganese oxide catalysts for O₃ decomposition are also summarized. The deactivation mechanisms of manganese oxides under dry and humid conditions are discussed. The O₃ decomposition performance of monolithic catalysts is also summarized from the perspective of industrial applications. Finally, the future development directions and prospects of O₃ catalytic decomposition technology are put forward.     

底泥原位洗脱过程中氮磷含量与形态变化特征

随着城市化进程的不断推进,城市河流底泥中内源氮磷污染问题日益突出.为研究原位洗脱技术对污染底泥中氮、磷物质和成分的作用效果,以北京市凉水河作为研究对象,分别比较了现场试验洗脱与对照组0~30 cm分层底泥以及实验室模拟洗脱处理前后0~10 cm底泥中pH、E_h（氧化还原电位）、容重、含水率、OM（有机质）、TN、TP和氮、磷形态分布的变化特征.结果表明:①现场洗脱对0~5 cm厚度底泥的处理和模拟洗脱处理均对底泥中pH、E_h、含水率的改变以及其中TN、TP的去除效果表现显著,其中,现场试验洗脱组0~5 cm范围底泥中w（TN）、w（TP）分别较对照组降低了66.4%±17.4%、40.8%±24.4%,模拟洗脱处理对底泥中OM、TN、TP的去除率分别达70.1%±4.8%、66.8%±2.0%、43.1%±3.1%.②原位洗脱技术对底泥中TN的去除主要通过对PON（颗粒态有机氮）的去除来实现,现场和模拟试验过程中PON对TN去除的贡献率分别达55.0%和73.6%.③原位洗脱对底泥中TP的去除主要通过对Al-P（铝结合态磷）、OP（有机磷）的去除来实现,现场和模拟试验中Al-P、OP对TP去除的贡献率分别达37.0%、66.2%和31.3%、43.7%.研究显示,原位洗脱技术可有效去除城市河流底泥处理层中的氮磷物质,并以有机氮、磷物质的去除为主.      

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.     

海绵城市地块汇水区颗粒污染物的传输

目前我国海绵工程建设多集中在地块汇水区单元内开展,通过多个低影响开发(LID)设施协同完成地表径流水质水量的调控,但基于地块汇水区尺度下城市面源污染的产生和控制效果鲜有报道.本研究比较分析了不同硬化率地块汇水单元内的面源颗粒污染物晴天累积、降雨冲刷、地表径流及径流输出负荷状况.结果表明,地块汇水单元内硬质路面是面源颗粒污染物贡献的最主要的下垫面类型,中硬化率(61.1%)地块和高硬化率(73.6%)地块路面街尘累积量分别约占汇水区单元的88.4%(2.22～12.51 g·m~(-2))和90.1%(4.99～33.43 g·m~(-2)),对径流SS的输出贡献比率分别约为91.7%(0.97～7.34 g·m~(-2))和90.5%(0.92～18.77 g·m~(-2)),降雨径流SS污染负荷占比分别约为95.2%和83.1%,经LID设施处理后输出径流污染负荷约为地表径流的24.0%和40.2%.硬质路面的街尘晴天累积及降雨冲刷以150μm为主,地表径流及输出径流则以50μm粒径段为主,同时地块不透水比例的增加,细粒径(105μm)颗粒物的累积及冲刷分布增大(24.4%和106.4%),而粒径50μm的颗粒物在路面径流中的分布减小(12.4%).屋面的街尘累积、冲刷及降雨径流的粒径分布状况与硬质路面大致相似,但中硬化率地块(1 000μm)和高硬化率地块(250～450μm、45μm)在3个粒径段范围的颗粒物累积和冲刷相较于路面街尘粒径分布明显增加(1 000μm:58.1%和108.5%; 250～450μm:72.9%和41.8%;45μm:59.2%和64.8%).以上结果揭示了颗粒污染物在地块汇水区尺度下的污染全过程(累积-冲刷-输出)分布及LID设施对地块整体SS污染负荷的控制效果,可为地块汇水单元内LID设施工程绩效的科学评估提供重要参考.     

汶川地震重灾区泥石流灾损土地利用及生态修复模式——以北川县都坝河小流域为例

汶川地震诱发了大量泥石流灾害,灾损土地利用和生态修复是灾区产业重建面临的重要课题。以北川县都坝河小流域为研究对象,通过调查灾损土地禀赋、灾害特征、土地需求,采取多因素耦合和关键因子限制分析法,探讨灾害胁迫条件下的经济活动与生态修复之间的互馈作用,结果表明：（1）流域新增土地供给源主要为泥石流灾损土地,土地资源化利用受灾害、聚落和产业结构控制;（2）灾损土地根据成因划分为沟口堆积型、沟道冲淤型以及岸坡侵蚀型,三者的肥力、安全性及交通条件等特征具有显著差异;（3）基于“因灾分区、耕地优先、产业共建、美居造景”的原则,建立了灾损土地的利用方式和生态修复模式,并选取杨家沟进行验证,沟域灾损土地利用方式为生态林地、产业林地及优质耕地,分别占比28.5%、56.3%、15.2%,生态修复措施主要为提高土地安全度、提升植被覆盖率和增强水保功能。该研究建立的震区土地利用和生态修复模式可有力协调人地矛盾、发展绿色经济和提升人居环境。