Influence of fuel moisture, charge size, feeding rate and air ventilation conditions on the emissions of PM, OC, EC, parent PAHs, and their derivatives from residential wood combustion

Controlled combustion experiments were conducted to investigate the influence of fuel charge size, moisture, air ventilation and feeding rate on the emission factors (EFs) of carbonaceous particulate matter, parent polycyclic aromatic hydrocarbons (pPAHs) and their derivatives from residential wood combustion in a typical brick cooking stove. Measured EFs were found to be independent of fuel charge size, but increased with increasing fuel moisture. Pollution emissions from the normal burning under an adequate air supply condition were the lowest for most pollutants, while more pollutants were emitted when an oxygen deficient atmosphere was formed in the stove chamber during fast burning. The impacts of these factors on the size distribution of emitted particles was also studied. Modified combustion efficiency and the four investigated factors explained 68%, 72%, and 64% of total variations in EFs of PM, organic carbon, and oxygenated PAHs, respectively, but only 36%, 38% and 42% of the total variations in EFs of elemental carbon, pPAHs and nitro-PAHs, respectively.     

电厂燃煤锅炉排放烟尘粒径和多环芳烃的分布及致突变特性

本文研究电厂UG-35/39-M型工业锅炉分别燃烧原煤和型煤时排放烟尘的径和多环芳烃的分布及其直接致突变特性.按粒径的大小将烟尘分成降尘、飘尘和烟气三部分收集,结果表明,多环芳烃主要分布在飘尘和烟气中,其中飘尘内集中了大部分高环的多环芳烃,烟气内集中了大部分低环的多环芳烃;飘尘和烟气的Ames试验致突变性之和比降尘高5—6倍,锅炉燃烧型煤排放烟尘的总量比烧原煤低50—60％,而且直接致突变性也比较低,由此看来,型煤燃烧技术是目前防治煤烟型大气污染的一种重要方法。     

添加剂对柴油机燃用乙醇柴油时排放颗粒特性的影响

为研究十六烷值改进剂和消烟剂对柴油机燃用乙醇柴油时颗粒排放特性的影响,在乙醇柴油中加入0.1%(以w计)、0.3%和0.5%的十六烷值改进剂或消烟剂,并在YZ4DB3柴油机上分别对这些燃料的排气烟度、颗粒比排放和粒径分布等进行研究. 结果表明:含添加剂的乙醇柴油颗粒物排放远低于0#柴油,降幅在50%以上;与0#柴油相比,添加0.3%十六烷值改进剂的乙醇柴油降低颗粒排放效果较显著,降幅高达64.2%,而添加0.1%消烟剂的乙醇柴油颗粒物排放降幅更高达84.0%,表明消烟剂的降颗粒效果更加显著. 柴油机燃用柴油时,排放颗粒的粒径呈双峰分布,峰值分别在0.56和0.18μm左右;但燃用含添加剂的乙醇柴油时,排放颗粒的粒径则呈单峰分布,其峰值均在>0.56~1.00μm粒径范围内. 柴油机燃用含添加剂的乙醇柴油后,0.18~0.32μm粒径范围内的排放颗粒显著减少,但在>0.32~1.00μm粒径范围内增加;同时,排放颗粒物中的积聚模态颗粒占排放颗粒总质量的比例降低,而粗粒子模态颗粒的所占比例相应增加. 排气烟度与积聚模态颗粒质量分布密切相关. 研究结果表明,柴油添加剂能够显著改善柴油机颗粒物排放特性,有利于改善大气质量.      

生物质露天焚烧及家庭燃用的多环芳烃排放特征研究

农村地区生物质燃烧排放是大气多环芳烃(PAHs)的重要来源之一.本研究利用建立的烟尘罩稀释通道采样系统,对我国典型的生物质燃烧方式—水稻、玉米、花生、大豆秸秆的家庭炉灶燃烧,并对水稻、玉米、花生秸秆以及荔枝树、大叶榕、小叶榕等落叶的露天焚烧进行实验室模拟,实测了秸秆野外焚烧、落叶野外焚烧、秸秆炉灶燃烧等3种典型生物质燃烧类型排放的气相及颗粒相PAHs的排放因子.结果表明,本研究生物质露天焚烧PAHs排放因子高于大部分已有实验结果,秸秆炉灶燃烧PAHs排放因子亦高于大部分排放清单采用值.3类燃料燃烧排放PAHs的谱分布相近,均以中低环PAHs为主,中高环(4~6环)PAHs比例为22.2%~28.8%.采用某单一数值作为某类源PAHs特征比的取值,并将其运用于大气PAHs的来源解析可能会造成偏差.     

蚊香燃烧产物中多环芳烃的分布规律及相关性研究

对蚊香燃烧后的烟气和灰烬样品进行采集,利用GC-MS方法分析其中16种优控多环芳烃(PAHs)的含量,并对烟气和灰烬中各PAHs组分及总量间的相关关系进行探讨.结果表明:蚊香烟气中16种PAHs均有检出,排放量较大的组分主要有萘、苊、二氢苊、菲和荧蒽,并以2～3环PAHs为主;灰烬中PAHs也以2～3环化合物为主,但排放总量仅为烟气中的4.7%～21.8%.通过与其他室内燃烧源PAHs排放量的对比发现,蚊香灰烬中总PAHs排放量低于卫生香源和木柴源,但比香烟源高一个数量级以上;烟气中总PAHs排放量低于燃煤源、木柴源和卫生香源,但明显高于烹调源.回归分析结果表明,烟气中总PAHs排放量与灰烬中的排放量表现出明显的线性关系(R2=0.9054).     

浙北地区PM2.5中多环芳烃特征

为了研究浙北地区PM_2.5中多环芳烃（PAHs）的季节性变化和它们的来源,于2014年11月~2015年11月收集了杭州和宁波2个城市中4个采样点的PM_2.5样品,利用气-质联用仪测定了17种PAHs浓度.结果表明,∑PAHs年平均浓度范围为24.1~51.9ng/m³,平均值为（35.5 ±12.3） ng/m³.2~3环PAHs在PM_2.5中的浓度较低（<1ng/m³）,而4~6环PAHs占总PAHs的77.0%.∑PAHs的浓度与PM_2.5呈相似的季节性变化特征,冬季浓度最高而夏季最低.惹烯作为软木燃烧的示踪物,冬季的浓度是夏季的4倍,表明在冬季软木燃烧的排放和对PM_2.5的贡献都有所增加.除了夏季的2个城区站点,其它季节和站点∑PAHs浓度和PM_2.5呈现一定的正相关性.特征PAHs比值显示,浙北地区气溶胶相关的多环芳烃主要来自燃烧和热解排放,如生物质燃烧和煤燃烧,而交通排放和石油挥发源的影响不大.     

Size distribution of particulate polycyclic aromatic hydrocarbons in fresh combustion smoke and ambient air: A review

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous in the atmosphere and they mostly stem from the imperfect combustion of fossil fuels and biofuels. PAHs are inherently associated with homogenous fine particles or distributed to different-sized particles during the aging of air masses. PAHs carried by fine particles undergo a long-range transport to remote areas while those adsorbed on coarse particles have a shorter lifetime in ambient air. More importantly, PAHs with higher molecular weights tend to be bound with finer particles and can deeply enter the lungs, posing severe health risks to humans. Thus, the environmental fate and health effects of particulate PAHs are strongly size-dependent. This review summarizes the size distributions of particulate PAHs freshly emitted from combustion sources as well as the distribution patterns of PAHs in ambient particles. It was found that PAHs from stationary sources are primarily bound to fine particles, which are slightly larger than particles to which PAHs from mobile sources are bound. In ambient air, particulate PAHs are distributed in larger size modes than those in the combustion fume, and the particle size decreases with PAH molecular weight increasing. The relevant mechanisms and influencing factors of particle size distribution changes are illustrated in this article, which are essentially attributed to combustion and ambient temperature as well as the physical and chemical properties of PAHs. Overall, the study on the particle size distribution of PAHs will contribute for a full understanding of the origin, atmospheric behaviors and health effects of particulate PAHs.     

Preliminary correlation of organic molecular tracers in residential wood smoke with the source of fuel

Polar cyclic di- and triterpenoids were analyzed in the extracts of residential wood combustion aerosols collected in suburban sections of Eugene, Oakridge and Corvallis, Oregon. Additional samples collected included alder wood, smoke from two wood stoves burning only alder or pine as fuel, soot from a stove burning alder and a fireplace where oak was the predominant fuel. Due to the relatively cooler temperatures present under the smoldering conditions of residential wood combustion, as compared to the active burning of forest fires and slash burns, incomplete combustion resulted in the preservation of high levels of the natural products.There were three distinct signatures which could be used to trace relative input from coniferous, alder and oak combustion products, i.e. diterpenoids, lupane-derived triterpenoids and friedelin, respectively. Conifer combustion products dominated the suburban smoke aerosols.     

2009年春季成都城区碳气溶胶污染特征及其来源初探

于2009年4月19日至5月17日在成都城区每天采集PM2.5样品,然后对样品进行8种碳组分、水溶性有机碳、左旋葡聚糖及水溶性离子分析,初步探讨了碳气溶胶的来源.结果发现：成都春季PM2.5日均值质量浓度为（133.2±55.5）μg·m^-3,TC、OC、EC和WSOC质量浓度分别为（26.4±7.2）,（20.7±...     

葫芦岛市生物质能燃料改善大气环境的探讨

分散在中小城市的小型洗浴锅炉,点多面广,锅炉燃料经历了原煤散烧、型煤、焦碳等不同阶段。虽然对其燃烧过程及其排放烟气进行了严格的管理、治理,但是燃烧产生的烟尘浓度、黑度、SO2经常超标排放,严重污染了大气环境质量。结合这种现状,通过改造锅炉结构,燃烧生物质颗粒燃料,实现了洗浴锅炉各种大气污染物达标排放,解决了市区四处冒黑烟的问题,改善了大气环境质量。     

民用燃料燃烧碳质组分及VOCs排放特征

选取北京市地区典型生物质燃料（玉米芯、玉米秆、黄豆秆、草梗、松木、栗树枝、桃树枝）以及民用煤（烟煤、蜂窝煤）在实验室内进行了模拟燃烧实验,对燃烧产生的颗粒物及气体样品进行采集,采用Model 2001A热/光碳分析仪对不同粒径段颗粒物中的有机碳、元素碳进行测定,采用AgilentGC-MS 5977/7890B气质联用仪对燃烧烟气中的挥发性有机物进行分析.研究表明：除蜂窝煤OC、EC的排放因子在2.5~10μm粒径范围内达到最大,其他8种固体燃料燃烧产生的OC、EC的排放因子最大值均在0~2.5μm粒径范围内.薪柴（栗树枝、桃树枝、松木）、秸秆（玉米芯、玉米秆、黄豆秆、草梗）和民用煤（蜂窝煤、烟煤）3类物质燃烧排放VOCs的物种分类差异较大.薪柴和民用煤燃烧排放的卤代烃以及含氧有机物的质量分数明显高于秸秆的质量分数;在同一类别中VOCs物质分布趋势一致.3种薪柴平均总VOCs的排放系数为2.02g/kg,4种秸秆平均总VOCs的排放系数为6.89g/kg,2种民用煤平均总VOCs的排放系数为2.03g/kg,秸秆类的排放因子最大.玉米芯、玉米秆、黄豆秆和草梗的臭氧生成潜势较高,而栗树枝、桃树枝、松木、烟煤以及蜂窝煤的臭氧生成潜势较低,且分布类似.烯烃类、烷烃类、芳香烃类是固体燃料燃烧臭氧生成潜势贡献较大的VOCs物质.     

昆明松华坝水库沉积物中PAHs垂直分布特征及其来源

为揭示昆明松华坝水库人类活动对PAHs（多环芳烃）的影响程度及其污染历史,研究了松华坝水库2根沉积柱（包括集水区人口较密集的1号柱和以山地为主的2号柱）中16种PAHs的垂直分布特征及其来源.结果表明:1号、2号柱中∑₁₆PAHs（16种PAHs总量）分布范围分别为155.9~471.3和100.7~316.3 ng/g,但1号柱污染程度高于2号柱,可能与其集水区较高的人为排放有关.1号柱中∑₁₆PAHs整体随采样深度的下降而降低,2号柱则随采样深度的下降而增长;这2根柱子PAHs的组成相似,沉积物中PAHs均以2环的Nap（萘）和3环的Phe（菲）为主（二者占比高于50%）,高致癌性的4~6环PAHs也有较大占比.分子比值法和正定矩阵因子分解法结果显示,1号柱中PAHs主要来源顺序为生物质燃烧源（38.8%）>石油源（34.7%）>煤炭燃烧源（13.4%）>石化燃料燃烧源（13.1%）,2号柱主要来源为石油源（44.4%）>生物质燃烧源（26.2%）>煤炭燃烧源（15.3%）>石化燃料燃烧源（14.1%）,反映了集水区人类活动方式与强度对沉积物中PAHs的控制作用.      

Pollution characteristics and health risk assessment of polycyclic aromatic hydrocarbons and nitrated polycyclic aromatic hydrocarbons during heating season in Beijing

Polycyclic aromatic hydrocarbons(PAHs) and their nitrated derivatives(NPAHs) attract continuous attention due to their outstanding carcinogenicity and mutagenicity. In order to investigate the diurnal variations, sources, formation mechanism, and health risk assessment of them in heating season, particulate matter(PM) were collected in Beijing urban area from December 26, 2017 to January 17, 2018. PAHs and NPAHs in PM were quantitatively analyzed via gas chromatography-mass spectrometry(GC-MS). ...     

薪柴和经济作物秸秆燃烧VOCs排放特征

薪柴及经济作物秸秆在中国农村地区仍普遍使用,其燃烧是挥发性有机物(VOCs)的重要排放源,当前对其排放特征研究仍比较薄弱.本研究选取了3种薪柴(白杨树、杉木和柑橘枝)和6种经济作物秸秆(黄豆秆、芝麻秆、玉米棒、棉花秆、花生秆和玉米秆),通过实验室模拟燃烧和稀释通道采样系统,采用Tedlar袋和Agilent 7820A/5977E气相色谱/质谱联用法采集和分析了烟气中102种VOCs组分组成,并对不同类型生物质燃烧排放VOCs的臭氧生成潜势进行分析.结果表明,不同类型的生物质燃烧排放的VOCs组分存在差异,乙烷(11.1%)、反-2-戊烯(15.4%)、乙烯(8.3%)和二氯甲烷(11.9%)是白杨树和杉木燃烧排放的主要VOCs组分;甲苯(49.8%)是柑橘枝燃烧排放的VOCs含量最丰富的物种;乙烯(11.8%～17.5%)和丙酮(9.2%～14.7%)是秸秆类燃料燃烧的主要VOCs组分.玉米秆、花生秆和柑橘枝具有相似的VOCs源成分谱,分歧系数小于0.1.本研究及已有报道中的生物质燃烧排放苯/甲苯比值范围是0.030～6.48,在开展源解析研究中,采用苯/甲苯比值大于1认定为受到生物质燃烧排放影响值得商榷.烯烃、含氧VOCs和芳香烃对生物质燃烧排放VOCs的臭氧生成潜势的贡献分别为30.6%～80.3%、 6.5%～21.0%和3.8%～56.5%,对臭氧生成潜势贡献比例超过10.0%的组分为乙烯、丙烯、反-2-戊烯、顺-2-戊烯、甲苯和丙醛.     

浅析燃木屑锅炉的消烟除尘改造

通过对燃木屑锅炉消烟除尘的改造 ,得出对于不同燃料结构的锅炉所采用的消烟除尘方法也应随烟尘的性质改变而改变的结论。在传统的燃煤锅炉单筒花岗岩水膜除尘器中心加装竖式喷淋管增加三级倒扣盆状水膜能解决密度小、颗粒细的木屑烟尘净化难题。     

Characterization and problems of indoor pollution due to cooking stove smoke

Findings from the five groups of matched houses, each using either cattle dung, wood, coal, kerosene or liquid petroleum gas (LPG) as cooking fuels are presented with emphasis on cross comparison of indoor pollution levels during the cooking period. The houses using LPG were considered as controls. The characterization of pollution was made by measurements of total suspended particulates (TSP), carbon monoxide, nitrogen dioxide, formaldehyde, sulfur dioxide and particle sizing of TSP, which were further analysed for the evaluation of levels of polycyclic aromatic hydrocarbons (PAHs). A correlation between the pollutants as a function of fuel type has also been looked for. The study revealed that 50–80% of the TSP emissions from biomass and coal-burning cooking stoves were in a respirable fraction of ≤2 μm size and that a large amount of the PAHs (> 75%) belonged to this fraction only. Air quality biomass-using houses was the worst among the users of the five aforementioned fuels and levels were relatively high. The findings stress that a conserted effort towards a solution should be made as a large fraction of the world's population regularly uses biomass as a prime domestic fuel. The problems associated with cooking stoves in India and immediate research needs are outlined.     

有机气溶胶的来源与形成研究现状

介绍了有机气溶胶来源与形成的研究现状,从有机气溶胶的化学组成特征、一次有机气溶胶的来源和二次有机气溶胶的形成机制论述其研究进展.一次有机气溶胶主要来源于烹调油烟、机动车排放、生物质燃烧、工业或民用燃油锅炉释放出的有机物,还有道路扬尘、沥青、刹车尘、轮胎屑、室外香烟烟雾、以及高等植物蜡、细菌活动和草本植物等.大气中的半挥发性有机物可通过物理和化学吸附形成二次有机气溶胶,一些挥发性有机物可通过气相化学反应转化为低挥发性的物质并形成二次有机气溶胶,其主要前体物是芳香族化合物,如苯、甲苯、二甲苯,以及烯烃、烷烃、环烷烃、萜烯和生物排放的非饱和氧化物.     

Characteristics of particulate-bound polycyclic aromatic hydrocarbons emitted from industrial grade biomass boilers

Polycyclic aromatic hydrocarbons(PAHs) are carcinogenic or mutagenic and are important toxic pollutants in the flue gas of boilers. Two industrial grade biomass boilers were selected to investigate the characteristics of particulate-bound PAHs: one biomass boiler retro-fitted from an oil boiler(BB1) and one specially designed(BB2) biomass boiler. One coal-fired boiler was also selected for comparison. By using a dilution tunnel system, particulate samples from boilers were collected and 10 PAH species were analyzed by gas chromatography–mass spectrometry(GC–MS). The total emission factors(EFs) of PAHs ranged from 0.0064 to0.0380 mg/kg, with an average of 0.0225 mg/kg, for the biomass boiler emission samples. The total PAH EFs for the tested coal-fired boiler were 1.8 times lower than the average value of the biomass boilers. The PAH diagnostic ratios for wood pellets and straw pellets were similar.The ratio of indeno(1,2,3-cd)pyrene/[indeno(1,2,3-cd)pyrene + benzo(g,h,i)perylene] for the two biomass boilers was lower than those of the reference data for other burning devices, which can probably be used as an indicator to distinguish the emission of biomass boilers from that of industrial coal-fired boilers and residential stoves. The toxic potential of the emission from wood pellet burning was higher than that from straw pellet burning, however both of them were much lower than residential stove exhausts.     

天津地区典型家用生物质颗粒采暖炉污染物排放分析

为调查研究天津市家用生物质颗粒采暖炉的污染物排放性状,同时为政府的政策制定提供技术依据,研究了天津地区生物质燃料成分和采暖炉不同运行负荷对污染物排放的影响.结果表明：稻杆和棉杆两种成型燃料在同一采暖炉的相同工况下燃烧时,稻杆灰分含量较棉杆高,造成较高的烟尘和CO排放,同时稻杆较棉杆S元素含量低,导致SO₂排放较低.棉杆成型燃料在同一容量的采暖炉上燃烧时,随着燃烧器负荷的增加,CO和SO₂的排放增加,NO_x的排放减少.两种生物质成型燃料在该采暖炉上燃烧排放的挥发性有机物的主要种类均依次为酮类、苯系物、醛类.本工作试验用家用生物质颗粒采暖炉运行过程中NO_x、CO、SO₂、烟尘的平均排放值分别为672.70,2297.94,124.00,109.35mg/m³,存在污染物排放超标的现象,可通过增添水浴除尘设施,合理调节不同燃烧负荷下的风机送风量,维持适宜过量空气系数,以降低污染物排放.同时还需制定合理的标准和政策加强对家用采暖炉和成型燃料质量的监管.     

南京北郊重金属气溶胶粒子来源分析

通过2013年1~12月使用在线单颗粒气溶胶质谱仪(SPAMS)在南京北郊对含有Cu、As、Pb、Cd、V、Co、Cr、Zn、Ni、Ba和Hg这11种重金属气溶胶粒子进行连续观测,并结合自适应共振理论神经网络算法(ART-2a)对其化学特征进行了分析,结果表明,南京北郊重金属气溶胶粒子来源按照化学组成特征可分为5类:工业排放(35.7%)、生物质燃烧(34.45%)、交通排放(13.6%)、化石燃料燃烧(11.03%)和矿尘(4.07%),其中,含Pb、Cd和Cr气溶胶粒子主要来源于工业排放,含Cu、Co和Hg气溶胶粒子主要来源于生物质燃烧,含V、Zn和Ba气溶胶粒子主要来源于交通排放,含As和Ni气溶胶粒子主要来源于化石燃料燃烧.