南方林区2000~2016年林火释放污染物动态变化研究

以南方林区为研究区域,基于林业统计年鉴和MODIS卫星火点数据,结合相关文献中不同林型各类污染物的排放因子数据,估算2000~2016年间研究区域各省森林生物质燃烧及污染物排放总量,并分析其时空变化情况.结果表明,南方林区森林火灾总体呈先升后降的趋势,林火空间分布较为分散.2000~2016年南方林区森林生物质燃烧总量4.79×10⁴kt.其中,温带常绿针叶林、温带常绿阔叶林、温带落叶阔叶林、热带常绿阔叶林和灌木的燃烧比例分别为65.24%,17.45%,1.55%,1.10%和14.66%.CO、CO₂、NO_x、CH₄、VOCs和PM_2.5等主要污染物的排放总量均值依次为3.73×10³,5.87×10⁴,48.05,347.27,358.54和365.06kt.此外,各类污染物的时空分布差异性明显：福建、广东、广西全省,海南西部,以及江西和湖南南部是各类污染物网格排放高值区;江西和湖北各类污染物的排放呈显著下降,福建NO_x、VOCs和PM_2.5,以及广东CH₄和VOCs下降趋势显著,其余省份各类污染物排放下降但不显著.林火释放污染物占工业粉尘比例呈波动性上升,表明该地区森林火灾对大气环境的影响程度逐渐增加.     

有机物对SAD的影响及其数学模拟

通过血清瓶批式实验,研究了不同C/N下葡萄糖和乙酸钠对厌氧氨氧化耦合反硝化系统（SAD）污泥活性及脱氮性能的影响.耦合系统颗粒污泥为在亚硝态氮充足的UASB连续流反应器中培养得到,具有较高的厌氧氨氧化活性和反硝化活性.以葡萄糖为碳源,C/N分别为1,2,4时,厌氧氨氧化活性差异不大,反硝化活性逐渐增加,亚硝态氮最大降解速率分别为0.265,0.345,0.453kgN/（kgVSS·d）;以乙酸钠为碳源,C/N分别为1、2、4时,厌氧氨氧化活性和反硝化活性都无明显差别.相同C/N下,耦合系统以葡萄糖为碳源时的厌氧氨氧化活性较高,以乙酸钠为碳源时的反硝化活性较高.C/N分别为1,2,4时,以葡萄糖为有机物的氨氮最大降解速率分别为乙酸钠的1.15,1.19,1.58倍,以乙酸钠为有机物时反应的亚硝态氮最大降解速率分别为葡萄糖的1.89,1.48,1.15倍.实验的数学模拟结果表明,通过模型的模拟,能较为准确地预测实验过程中氮素的变化趋势,在C/N为1~4时耦合系统中颗粒污泥的厌氧氨氧化活性无较大变化.     

基于稳定碳同位素技术的干旱区绿洲土壤有机碳向无机碳的转移

应用稳定碳同位素技术测定土壤无机碳稳定碳同位素组成(soil inorganic carbonδ13C,SICδ13C),并对干旱区绿洲土壤无机碳进行区分,结合土壤有机碳(soil organic carbon,SOC)与SIC含量关系进一步探讨SOC向SIC转移的碳量.结果表明,4种类型土壤SICδ13C值差异性极显著(P0.01),风沙土SICδ13C值最高且为正,均值为(0.32±0.04)‰,随土层深度增加而增加,说明风沙土原生性碳酸盐占绝对优势;灌漠土、棕漠土和盐碱土SIC的δ13C均值分别(-0.30±0.24)‰、(-1.96±0.66)‰和(-1.24±0.49)‰,随土层变化均呈先降低后逐渐增大的趋势,说明灌漠土原生性碳酸盐占优势,棕漠土和盐碱土发生性碳酸盐相对前者占优势.风沙土、灌漠土、棕漠土和盐碱土的发生性碳酸盐占SIC比例均值分别为1.33%、4.72%、15.01%、35.71%,均小于50%,说明干旱区绿洲土壤发生性碳酸盐比例总体水平较低.风沙土、灌漠土、棕漠土和盐碱土在土壤发生性碳酸盐形成或重结晶过程中固定土壤CO2的量分别为0.30、2.44、4.96、12.40 g·kg~(-1),其中固定来自大气CO2量平均为0.18、0.79、1.45、8.67 g·kg~(-1),来自SOC氧化分解转化为CO2的量分别为0.06、0.83、1.62、1.86g·kg~(-1),说明盐碱土、棕漠土SOC的贡献相对较高,灌漠土、风沙土较低;对土壤固定CO2量的来源比较发现,风沙土、盐碱土固定土壤CO2的量来自大气CO2量较高,SOC的贡献较低,而灌漠土、棕漠土固定来自SOC氧化分解CO2的量较高,大气贡献较低.研究区整体SOC向SIC的碳转移量介于0.03~2.38 g·kg~(-1)之间,平均每千克土壤固定1.09 g的CO2,说明干旱区绿洲土壤发生性碳酸盐所占比例较低,SOC的贡献较少.     

合肥市典型交通干道大气苯系物的特征分析

为研究合肥市交通干道大气苯系物污染状况,采用自主研制的差分吸收光谱(DOAS)系统,于2016年3月期间对合肥市交通主干道大气苯系物(苯、甲苯、间二甲苯和邻二甲苯)以及常规污染物NO_2、SO_2等进行了连续观测.观测结果显示,观测期间苯、甲苯、间二甲苯和邻二甲苯的平均浓度分别为:21.7、63.6、33.9和98.7μg·m~(-3).与国内外其它城市比较显示,合肥市交通干道大气苯和甲苯的污染处于中等水平,二甲苯的污染较为严重.结合观测期的间风速风向、T/B特征比值以及与CO等污染物的相关性,对上述苯系物来源进行了分析,结果显示观测期间T/B值为0.8~4.5,苯、甲苯与CO的相关性系数R分别为0.55和0.34.表明机动车尾气排放是观测区域苯和甲苯的主要排放源之一,同时也受到周边工业园区排放的影响,二甲苯的主要排放源为观测地点北偏东方向的涂料行业工业园区.苯和甲苯的夜间高浓度峰值分析结果表明,夜间的高浓度苯和甲苯可能主要来源于观测地点周边工业园区的排放.观测区域苯系物的臭氧生成潜势(OFP)表现为邻二甲苯间二甲苯甲苯苯,其中二甲苯的OFP占总OFP的85%,表明周边工业园区的排放对该地区臭氧生成的贡献较大.     

黄河干流宁蒙段溶解性有机物组分特征及其与金属离子的相关性

溶解性有机物(dissolved organic matter,DOM)是天然水体的重要组成部分,由于化学极性及所含的官能团不同,其在水体中的化学行为也不同.本研究以黄河干流宁蒙段为研究对象,于2015年4月采集了下河沿至头道拐沿程7个断面的水样,采用XAD系列树脂将DOM分为疏水性酸(hydrophobic acid,HOA)、疏水性碱(hydrophobic base,HOB)、弱疏水性酸(weak hydrophobic acid,WHOA)和亲水性物质(hydrophilic matter,HYI)这4个组分,探讨了DOM组分含量、荧光峰值及其与Pb、Zn、Cu、Cr、As这5种金属离子之间的相关性.结果表明,黄河宁蒙段DOM总量由下河沿至头道拐沿程逐渐增加.各断面DOM腐殖化程度较低,以亲水性的蛋白质类小分子物质(HYI)为主,疏水性酸(HOA)次之,这与黄河沿岸排污导致内源作用增强有关.三维荧光光谱中类腐殖质和类蛋白质荧光峰型显著,且类腐殖质峰沿程逐渐增强,进一步证实了内源污水输入的影响.SPSS相关性分析结果表明,DOM与5种金属离子呈现出不同程度的相关性,其中与Cu离子显著相关;4种组分中HYI与Cu离子的相关性最强,说明二者在迁移转化过程中存在显著相互作用.进一步研究发现,芳香蛋白类物质荧光峰强度随Cu离子浓度的升高而降低,这可能是Cu与亲水性组分中的芳香类蛋白质发生络合产生荧光淬灭效应,从而导致荧光强度降低.     

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.     

中国显示器件行业VOCs排放特征及控制对策

为掌握和了解我国电子行业VOCs的排放特征,以显示器件行业为研究对象,梳理和分析其生产工艺及排污环节;通过典型企业有机废气的实际排放监测,掌握其VOCs排放水平;利用排放因子法,核算了2011-2016年我国显示器件行业VOCs的排放量,分析其排放量的变化趋势及空间分布特征.结果表明:受产量和污染控制效率变化的双重影响,2011-2016年我国显示器件行业VOCs排放量（文中涉及"全国"的各要素范围均未包含港澳台地区）呈先增后降的趋势,2015年达到最大值（15 605 t）,此后在产量增长放缓和污染控制效率提高的作用下,2016年的排放量有所下降;从排放占比来看,显示器件行业无组织VOCs排放占比从2011年的45%升至2016年的53%,车间无组织VOCs逸散,以及废水处理过程、有机原辅料和有机废液储运等环节的VOCs无组织排放是行业污染控制的重点和难点.研究显示,我国显示器件行业VOCs无组织排放量占比逐年上升,为控制未来行业VOCs排放,企业应将无组织排放转化为有组织排放,之后再通过高效的末端处理装置来减少VOCs排放量.      

天津市区夏季碳气溶胶特征及改进的二次有机碳估算方法

为更加准确地估算环境受体PM_2.5中SOC（二次有机碳）的质量浓度,于2015年6-8月利用在线监测仪器同步采集小时分辨率的PM_2.5及OC（有机碳）和EC（元素碳）样品数据,分析碳气溶胶的变化特征,并尝试运用改进的EC示踪法估算ρ（SOC）.结果表明:天津市区夏季ρ（PM_2.5）为（70.9±46.0）μg/m3,ρ（OC）和ρ（EC）分别为（7.6±3.1）（2.2±1.5）μg/m3,占ρ（PM_2.5）的11.8%±4.6%和3.1%±1.4%,OC/EC（质量浓度之比,下同）的平均值为4.0±2.0.ρ（OC）与ρ（EC）之间的Pearson相关系数（R）仅为0.66,说明OC和EC的来源较为复杂,SOC的产生可能是重要影响因素.ρ（NO₂）与OC/EC呈显著负相关（R=-0.47,P < 0.01）,并且OC/EC（4.0）相对较低,说明天津市区机动车可能对碳气溶胶具有重要影响.ρ（SO₂）与ρ（OC）、ρ（EC）的相关性较低（R均为0.33,P均小于0.01）,说明天津市区碳气溶胶可能受燃煤源的影响较低.改进的EC示踪法主要是利用O₃和CO、EC作为光化学反应和一次源排放的指标,并结合ρ（OC）、ρ（EC）和OC/EC的变化特征,逐步筛选一次排放源主导的时间段的ρ（OC）和ρ（EC）数据,然后利用最小二乘法拟合获得ρ（OC）和ρ（EC）的线性方程,最后进行ρ（SOC）和ρ（POC）（POC为一次有机碳）的估算.天津市区夏季ρ（SOC）的平均值为（2.5±2.0）μg/m3,分别占ρ（OC）和ρ（PM_2.5）的28.8%±15.0%和3.7%±3.6%;ρ（POC）的平均值为（5.2±1.7）μg/m3,分别占ρ（OC）和ρ（PM_2.5）的71.2%±15.0%和8.1%±5.2%,说明天津市区夏季有机碳的主要来源是一次排放源.研究显示,相比于EC示踪法,改进的EC示踪法估算的ρ（SOC）明显降低,ρ（POC）明显升高.AT（大气温度）对ρ（SOC）的影响较为显著,而WS（风速）对ρ（POC）的影响较为显著.      

Investigating missing sources of glyoxal over China using a regional air quality model (RAMS-CMAQ)

Currently, modeling studies tend to significantly underestimate observed space-based glyoxal(CHOCHO) vertical column densities(VCDs), implying the existence of missing sources of glyoxal. Several recent studies suggest that the emissions of aromatic compounds and molar yields of glyoxal in the chemical mechanisms may both be underestimated, which can affect the simulated glyoxal concentrations. In this study, the influences of these two factors on glyoxal amounts over China were investigated using the RAMS-CMAQ modeling system for January and July 2014. Four sensitivity simulations were performed, and the results were compared to satellite observations. These results demonstrated significant impacts on glyoxal concentrations from these two factors.In case 1, where the emissions of aromatic compounds were increased three-fold,improvements to glyoxal VCDs were seen in high anthropogenic emissions regions. In case 2, where molar yields of glyoxal from isoprene were increased five-fold, the resulted concentrations in July were 3–5-fold higher, achieving closer agreement between the modeled and measured glyoxal VCDs. The combined changes from both cases 1 and 2 were applied in case 3, and the model succeeded in further reducing the underestimations of glyoxal VCDs. However, the results over most of the regions with pronounced anthropogenic emissions were still underestimated. So the molar yields of glyoxal from anthropogenic precursors were considered in case 4. With these additional mole yield changes(a two-fold increase), the improved concentrations agreed better with the measurements in regions of the lower reaches of the Yangtze River and Yellow River in January but not in July.     

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.