Emissions of parent, nitrated, and oxygenated polycyclic aromatic hydrocarbons from indoor corn straw burning in normal and controlled combustion conditions

Emission factors （EFs） of parent polycyclic aromatic hydrocarbons （pPAHs）, nitrated PAHs （nPAHs）, and oxygenated PAHs （oPAHs） were measured for indoor corn straw burned in a brick cooking stove under different burning conditions. The EFs of total 28 pPAHs, 6 nPAHs and 4 oPAHs were （7.9 ±3.4）, （6.5 ±1.6）×10^-3, and （6.1 ±1.4）×10^-1mg/kg, respectively. Fuel charge size had insignificant influence on the pollutant emissions. Measured EFs increased significantly in a fast burning due to the oxygen deficient atmosphere formed in the stove chamber. In both restricted and enhanced air supply conditions, the EFs of pPAHs, nPAHs and oPAHs were significantly higher than those measured in normal burning conditions. Though EFs varied among different burning conditions, the composition profiles and calculated isomer ratios were similar, without significant differences. The results from the stepwise regression model showed that fuel burning rate, air supply amount, and modified combustion efficiency were the three most significant influencing factors, explaining 72%-85% of the total variations.     

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.     

Air pollution and inhalation exposure to particulate matter of different sizes in rural households using improved stoves in central China

Household air pollution is considered to be among the top environmental risks in China.To examine the performance of improved stoves for reduction of indoor particulate matter(PM) emission and exposure in rural households, individual inhalation exposure to size-resolved PM was investigated using personal portable samplers carried by residents using wood gasifier stoves or improved coal stoves in a rural county in Central China.Concentrations of PM with different sizes in stationary indoor and outdoor air were also monitored at paired sites. The stationary concentrations of size-resolved PM in indoor air were greater than those in outdoor air, especially finer particles PM0.25. The daily averaged exposure concentrations of PM0.25, PM1.0, PM2.5 and total suspended particle for all the surveyed residents were 74.4 ± 41.1, 159.3 ± 74.3, 176.7 ± 78.1 and 217.9 ± 78.1 μg/m3,respectively. Even using the improved stoves, the individual exposure to indoor PM far exceeded the air quality guideline by WHO at 25 μg/m3. Submicron particles PM1.0 were the dominant PM fraction for personal exposure and indoor and outdoor air. Personal exposure exhibited a closer correlation with indoor PM concentrations than that for outdoor concentrations. Both inhalation exposure and indoor air PM concentrations in the rural households with gasifier firewood stoves were evidently lower than the reported results using traditional firewood stoves. However, local governments in the studied rural areas should exercise caution when widely and hastily promoting gasifier firewood stoves in place of improved coal stoves, due to the higher PM levels in indoor and outdoor air and personal inhaled exposure.     

Field assessment of straw pellet combustion in improved heating stoves in rural Northeast China

Straw pellets are widely promoted and expected to be a cleaner alternative fuel to unprocessed crop residues and raw coal in rural China.However,the effectiveness of these dissemination programs is not well evaluated.In this?eld study,emission characteristics of burning straw pellets,raw coal,and unprocessed corn cobs in heating stoves were investigated in a pilot village in Northeast China.Emission measurements covering the whole combustion cycle (ignition,?aming,and smoldering phases) shows th...     

Atmospheric pollution of agriculture-oriented cities in Northeast China: A case in Suihua

Agriculture-oriented cities in Northeastern China have experienced frequent atmospheric pollution events. Deeper understandings of the pollution characteristics, haze causes and effects of management on local air quality are crucial for conducting integrated management approaches for the sustainable development of agriculture-oriented cities. Taking a typical agriculture-dominant city (i.e., Suihua) in Northeast China, we analyzed in detail the characteristics and causes of atmospheric pollution and evaluated the straw-burning prohibition using multisource data. The results showed a clear temporal pattern of air quality index (AQI) on an annual scale (i.e., 2015-April 2019), with two typical pollution periods occurring in late autumn and early spring. The large areas of concentrated straw burning at local and regional scales accounted for the first period (i.e., October and November), while dust emissions and farming disturbances comprised the second period. The interannual variation in pollution periods among these years was large, showing similar trends from 2015 to 2017 and the postponed late-autumn pollution period in 2018. Our evaluation has shown that the prohibition effect of straw burning significantly improved air quality in 2018, with a reduction of 59% ± 88% in the PM_2.5 concentrations in October and November compared to 2015–2017. However, From October to April of the following year, the improvement effect was not significant due to postponement of straw burning to February or March. Our analysis also highlighted the roles of meteorological conditions, Therefore, combined with the promotion of straw utilization, scientifically prescribed burning considering the burning amount and location, meteorological conditions and regional transportation should be implemented.     

Photochemical properties and source of pollutants during continuous pollution episodes in Beijing, October, 2011

Beijing sufered from serious air pollution in October, 2011 with the occurrence of three continuous episodes. Here we analyze the pollution status of particulate matter, the relationship between the gaseous pollutants, physical and chemical properties of single particles, and the profile of watersoluble ions in PM2.5during the three episodes. Regional and photochemically aged air masses, which were characterized as having high values of O3and SO2, were hypothesized to have played a dominant role in the first episode. After mixing local air masses with freshly-emitted primary pollutants, the concentration of NOx continued to increase and the size of SO4 2, NO3 and NH4 +in the particle population continued to become smaller. The amount of elemental carbon-rich and organic carbonrich particles in the scaled single particles(0.2–2 μm) and water-soluble K+in PM2.5also increased in the episodes. All the available information suggests that the biomass or fuel burning sources in or around Beijing may have had a huge impact on the last two episodes.     

Investigation on emission factors of particulate matter and gaseous pollutants from crop residue burning

Emission factors of particulate matter (PM), element carbon (EC), organic carbon (OC), SO_2, NO_x, CO, CO_2, and ten ions (Na~ , NH_4~ , K~ , Mg~(2 ), Ca~(2 ), F~-, Cl~-, NO_2~-, NO_3~-, SO_4~(2-)) were estimated from the domestic burning of four types of commonly produced crop residues in rural China: rice straw, wheat straw, corn stover, and cotton stalk, which were collected from the representative regions across China. A combustion tower was designed to simulate the cooking conditions under which the peasants burned their crop residues in rural China, to measure the emission factors. Results showed that wheat straw had the highest emission factor for the total PM (8.75 g/kg) among the four crop residues, whereas, corn stover and wheat straw have the highest emission factor for EC (0.95 g/kg) and OC (3.46 g/kg), respectively. Corn stover also presents as having the highest emission factors of NO, NO_x, and CO_2, whereas, wheat straw, rice straw, and cotton stalk had the highest emission factors of NO_2, SO_2, and CO, respectively. The water-soluble ions, K~ and Cl~-, had the highest emission factors from all the crops. Wheat straw had a relatively higher emission factor of cation species and F~-, Cl~-, NO_2~- than other residues.     

Spatial and temporal variation of particulate matter and gaseous pollutants in 26 cities in China

O3and PM2.5were introduced into the newly revised air quality standard system in February 2012, representing a milestone in the history of air pollution control, and China's urban air quality will be evaluated using six factors(SO2, NO2, O3, CO, PM2.5and PM10) from the beginning of 2013. To achieve the new air quality standard, it is extremely important to have a primary understanding of the current pollution status in various cities. The spatial and temporal variations of the air pollutants were investigated in 26 pilot cities in China from August 2011 to February 2012, just before the new standard was executed. Hourly averaged SO2, NO2and PM10were observed in 26 cities, and the pollutants O3, CO and PM2.5were measured in 15 of the 26 cities. The concentrations of SO2and CO were much higher in the cities in north China than those in the south. As for O3and NO2, however, there was no significant diference between northern and southern cities. Fine particles were found to account for a large proportion of airborne particles, with the ratio of PM2.5to PM10ranging from 55% to 77%. The concentrations of PM2.5(57.5 μg/m3) and PM10(91.2 μg/m3) were much higher than the values(PM2.5: 11.2 μg/m3; PM10 : 35.6 μg/m3) recommended by the World Health Organization. The attainment of the new urban air quality standard in the investigated cities is decreased by 20% in comparison with the older standard without considering O3, CO and PM2.5, suggesting a great challenge in urban air quality improvement, and more eforts will to be taken to control air pollution in China.     

Submicron particle-bound polycyclic aromatic hydrocarbons in the Polish teaching rooms: Concentrations, origin and health hazard

The goal of the work was to investigate the concentrations of the 16 US EPA priority polycyclic aromatic hydrocarbons(PAH) bound to submicrometer particles(particulate matter, PM_1) suspended in the air of university teaching rooms and in the atmospheric air outside. Two teaching rooms were selected in two Polish cities, Gliwice, southern Poland,and Warsaw, central Poland, differing with regard to the ambient concentrations and major sources of PM and PAH. The variabilities of indoor and outdoor 24-hr concentrations of PM_1-bound PAH, the ratio(I/O) of the indoor to outdoor 24-hr concentrations of PM_1-bound PAH, probable sources of PAH and the level of the hazard from the mixture of the 16 PAH(ΣPAH) to humans at both sites were analyzed. In both Warsaw and Gliwice, the mean concentrations of PM_1-bound ΣPAH were slightly higher in the atmospheric air than in the rooms. The indoor and outdoor concentrations of individual PAH in Gliwice were correlated,in Warsaw – they were not. Most probably, the lack of the correlations in Warsaw was due to the existence of an unidentified indoor source of gaseous PAH enriching PM_1 in phenanthrene, fluorene, and pyrene. Although the ambient concentrations of PM_1-bound PAH were low compared to the ones observed earlier at both sites, they were much higher than in other urbanized European areas. However, because of low mass share of heavy PAH in ΣPAH, the various indicators of the health hazard from the 16 PAH mixture were low compared to other regions.     

Source profiles of particulate organic matters emitted from cereal straw burnings

Cereal straw is one of the most abundant biomass burned in China but its contribution to fine particulates is not adequately understood. In this study, three main kinds of cereal straws were collected from five grain producing areas in China. Fine particulate matters （PMzs） from the cereal straws subjected to control burnings, both under smoldering and flaming status, were sampled by using a custom made dilution chamber and sampling system in the laboratory. Element carbon （EC） and organic carbon （OC） was analyzed. 141 compounds of organic matters were measured by gas chromatography-mass spectrum （GC-MS）. Source profiles of particulate organic matters emitted from cereal straw burnings were obtained. The results indicated that organic matters contribute a large fraction in fine particulate matters. Levoglucosan had the highest contributions with averagely 4.5% in mass of fine particulates and can be considered as the tracer of biomass burnings. Methyloxylated phenols from lignin degradation also had high concentrations in PM2.5, and contained approximately equal amounts of guaiacyl and syringyl compounds. 13-Sitostrol also made up relatively a large fraction of PMz5 compared with the other sterols （0.18%-0.63% of the total fine particle mass）. Normal alkanes, PAHs, fatty acids, as well as normal alkanols had relatively lower concentrations compared with the compounds mentioned above. Carbon preference index （CPI） of normal alkanes and alkanoic acids showed characteristics of biogenic fuel burnings. Burning status significantly influenced the formations of EC and PAHs. The differences between the emission profiles of straw and wood combustions were displayed by the fingerprint compounds, which may be used to identify the contributions between wood and straw burnings in source apportionment researches.     

福建省4种主要乔木枝叶燃烧含碳物质排放特性分析

森林可燃物燃烧释放的大量含碳物质对大气环境和生态系统碳平衡具有重要影响,揭示森林可燃物燃烧的含碳物质排放特性具有重要的科学意义.运用自主设计的生物质燃烧系统,模拟福建省4种主要乔木树种——马尾松、杉木、樟树、桉树的枝、叶燃烧,分析其在不同燃烧状态（阴燃、明燃）下含碳气体（CO、CO₂、C_xH_y）和PM_2.5的排放因子（分别以EF_CO2、EF_CO、EF_CxHy、EF_PM2.5表示）及PM_2.5中的碳质组分之间的差异性.结果表明,马尾松、杉木、樟树、桉树燃烧排放的含碳气体、PM_2.5的排放因子及PM_2.5的碳质组分在不同燃烧状态下差异较大,阴燃时EF_CO2、EF_CO、EF_CxHy、EF_PM2.5平均值在分别为（1 400.7±76.5）（297.6±16.2）（25.2±3.9）（23.9±4.3）g/kg,明燃时分别为（1 582.8±73.2）（253.6±16.1）（17.2±3.7）（8.4±2.8）g/kg,除CO₂外其他多为阴燃显著高于明燃.针叶树种（杉木、马尾松）枝、叶在阴燃时EF_PM2.5高于阔叶树种（樟树、桉树）,而明燃时差异相对较小.PM_2.5中OC（有机碳）、EC（元素碳）、TC（OC+EC）的质量分数阴燃时分别为45.6%、12.0%、57.6%,明燃时分别为42.9%、17.6%、60.5%.EF_OC/EF_PM2.5、EF_EC/EF_PM2.5、EF_OC/EF_EC在两种燃烧状态下具有不同的特征,其特征值可作为区分不同燃烧源或不同燃烧状态的指标;EF_OC/EF_PM2.5在明燃和阴燃时差异不大,平均值分别为0.49、0.46;EF_EC/EF_PM2.5明燃显著高于阴燃,平均值分别为0.18、0.12;4种乔木的枝、叶燃烧的EF_OC/EF_EC明燃低于阴燃,平均值分别为2.59和4.01.在两种燃烧状态下OC与PM_2.5的排放因子均呈显著相关.研究显示,不同燃烧条件以及不同燃料燃烧对排放含碳物质具有显著影响.      

森林生物质燃烧烟尘中的有机碳和元素碳

选取10种乔木制备风干树枝、新鲜树枝两种类型的样品,通过自制的生物质燃烧装置模拟阴、明燃两种燃烧方式燃烧制备的树枝样品,采集排放的烟尘,并使用DRI2001A热/光分析仪测定样品中的有机碳(OC)、元素碳(EC).结果表明,风干树枝明燃排放烟尘中OC的排放因子(EFOC)、EC的排放因子(EFEC)、PM的排放因子(EFPM)均值分别为6.8、2.1、16.5g·kg-1,阴燃排放烟尘中均值分别为57.5、11.1、130.9 g·kg-1;新鲜树枝明燃排放烟尘中EFOC、EFEC、EFPM均值分别为13.6、3.3、30.5 g·kg-1,阴燃排放烟尘中均值分别为57.6、9.6、125.6 g·kg-1.树枝(风干树枝、新鲜树枝)阴燃时EFOC、EFEC、EFPM均高于明燃时,在明燃(高温度)条件下含水率与树枝燃烧时EFOC、EFEC、EFPM是呈正相关关系.树枝燃烧烟尘中OC、EC、TC(TC=OC+EC)占PM的百分比约为45%、10%、55%,乔木树枝阴燃排放烟尘中OC的质量分数高于明燃,EC的质量分数低于明燃.新鲜树枝排放烟尘中OC的质量分数高于风干树枝,EC的质量分数低于风干树枝.风干树枝明燃条件下OC/EC的均值为3.3(2.5~5.2),阴燃条件下均值为5.2(4.3~6.3);新鲜树枝明燃条件下OC/EC的均值为4.1(3.1~5.3),阴燃条件下均值为6.2(4.2~8.4),乔木树枝阴燃时OC/EC的值高于明燃,含水率高的乔木树枝(新鲜树枝)燃烧排放烟尘中OC/EC的值高于含水率低的树枝(风干树枝).风干树枝燃烧烟尘中OC、EC的相关系数为0.985,新鲜树枝燃烧烟尘中OC、EC的相关系数为0.915,含水率不同的乔木树枝(风干树枝、新鲜树枝)在不同燃烧条件下(明燃、阴燃)排放烟尘中OC与EC都具有良好的相关性.     

长三角地区秸秆燃烧排放因子与颗粒物成分谱研究

为获取长三角地区秸秆燃烧污染物排放因子及其颗粒物成分谱,利用自行设计开发的开放式燃烧源排放测试系统,选取小麦、水稻、油菜、豆秸和薪柴等5类典型作物秸秆,分别采用露天焚烧和炉灶燃烧2种燃烧方式,实测其气态污染物和颗粒物排放特征.结果表明,露天燃烧各类秸秆的CO、NOx和PM2.5平均排放因子约为28.7、1.2和2.65 g·kg-1,由于炉灶氧含量相对较低,燃烧不充分,其污染物排放因子总体高于露天燃烧,分别为81.9、2.1和8.5 g·kg-1.各类秸秆中,油菜的排放水平相对较高.含碳组分(OC和EC)是生物质秸秆燃烧产生PM2.5的主要组成,在露天燃烧中OC和EC的质量分数分别占(38.92±13.93)%和(5.66±1.54)%;炉灶燃烧中OC和EC分别为(26.37±10.14)%和(18.97±10.76)%.Cl-、K+等水溶性离子也有较大贡献,在露天燃烧中分别为(13.27±6.82)%和(12.41±3.02)%;在炉灶燃烧中分别为(16.25±9.34)%和(13.62±7.91)%.小麦、水稻、油菜和豆秸等作物秸秆露天燃烧排放颗粒物的K+/OC值分别为0.30、0.52、0.49和0.15,这些特征值可用于判断长三角区域空气质量受秸秆燃烧排放影响的程度,为大气污染来源解析提供直接的判断依据.     

生物质燃烧排放PM2.5中无机离子及有机组分的分布特征

为探讨生物质在明火和阴燃两种不同条件下PM_(2.5)及主要成分的排放差异,选取了7种具有代表性的生物质样品(小麦、水稻、马尾松叶、马尾松枝、杂草、玉米、棉花)进行了燃烧实验,并对PM_(2.5)样品中的7种主要水溶性离子(Na~+、NH_4~+、K~+、Ca~(2+)、Cl~-、NO_3~-、SO_4~(2-))及有机碳(OC)、元素碳(EC)、水溶性有机碳(WSOC)、有机酸和左旋葡聚糖(LG)等有机成分进行了分析.结果表明,明火和阴燃条件下PM_(2.5)的排放因子分别为2.82~7.74 mg·g~(-1)和3.24~22.56 mg·g~(-1),阴燃时的排放因子偏高,不同燃料类型也存在一定差异.燃烧排放PM_(2.5)中水溶性离子以Cl~-为最高,占总离子的比例为72%~94%,且与NH_4~+存在显著正相关关系,水溶性离子整体表现为明火条件下的浓度显著高于阴燃条件下的浓度.受阴燃条件下氧气不足的影响,PM_(2.5)中有机组分的浓度表现为阴燃高于明火,进而导致阴燃时PM_(2.5)的排放因子增加.水稻秸秆燃烧烟尘中3种来源特征比值(LG/PM_(2.5)、LG/OC和LG/WSOC)仅为小麦和玉米秸秆燃烧排放相应比值均值的0.34、0.24和0.27倍,表明在不同农作物的收获季节采用上述特征比值进行生物质燃烧来源估算时,应区别对待.     

华东地区2000-2014年间秸秆燃烧排放PM2.5时空动态变化

秸秆燃烧释放大量细小颗粒物（Fine Particulate Matter）,对大气环境、生态系统和人类健康有重要影响.该研究基于2000-2014年中国华东地区农作物产量统计数据,估算各区域秸秆产量及室内外农作物秸秆燃烧总量.并运用排放因子法,估算15年间华东地区农作物秸秆燃烧PM_2.5排放总量.研究结果表明,华东地区秸秆产量及燃烧总量分别为：2033.2 Mt和32678.59 Wt,PM_2.5的排放总量为851.95 Wt.此外,PM_2.5排放在时间和空间上不均衡.卫星火点监测数据显示,农田秸秆燃烧密集区域主要分布在山东南部、安徽北部、江苏和浙江东北部及上海市大部分地区;单位网格PM_2.5最大的排放量多集中在山东、安徽北部、江苏中部和北部、浙江东北部和上海区域.时间序列上,山东、江苏和安徽呈显著增长趋势,上海、福建和浙江呈显著降低趋势.稻谷、小麦、玉米、豆类和油菜秸秆燃烧对污染物PM_2.5的贡献率分别为32.45%、30.18%、18.95%、3.77%和14.65%.农作物秸秆燃烧释放PM_2.5与工业粉尘的排放比变化趋势表明山东、安徽和江苏总体呈上升趋势;上海、福建和浙江总体保持平稳趋势.通过对华东地区农作物秸秆燃烧释放PM_2.5的时空变化研究,为更好的揭示秸秆燃烧对区域环境的影响提供数据支持.     

稻草烟尘中有机碳/元素碳及水溶性离子的组成

选取我国6种稻草,通过自制的生物质焚烧装置模拟秸秆露天焚烧.采用Model 2001A热/光分析仪和ISC 2000/ISC3000离子色谱仪测定了阴燃、明燃烟尘中有机碳(OC)、元素碳(EC)与水溶性离子的含量.结果表明,明燃条件下稻草中OC排放因子(EFOC)均值为(6.37±1.86)g·kg-1,EC排放因子(EFEC)均值为(1.07±0.30)g·kg-1;阴燃条件下稻草中EFOC均值为(37.63±6.26)g·kg-1,EFEC均值为(4.98±1.42)g·kg-1.同一品种稻草燃烧排放出的PM、OC与EC变化趋势一致.明燃时稻草中的OC/EC均值为5.96,阴燃时比值均值为7.80,OC/PM几乎不受燃烧状态的影响,阴燃、明燃时EC/PM分别在0.06~0.08、0.08~0.11范围内,通过EC/PM比值可以初步判断燃烧状态的趋势,两种燃烧方式中排放的OC、EC相关性达到0.97,在0.01水平上相关性显著.阴离子中,Cl-含量最高,明燃时稻草中Cl-的排放因子均值为(0.246±0.150)g·kg-1,阴燃下为(0.301±0.274)g·kg-1,明燃时K+排放因子均值为(0.118±0.051)g·kg-1,阴燃时排放因子远低于明燃排放量,均值为(0.053±0.031)g·kg-1.水溶性Na+在阴燃条件下的排放因子均高于明燃状态下的排放.明燃条件下水溶性离子间的相关性比阴燃时显著.通过OC/EC比值可以将稻草与石化燃料及其他一些生物质燃烧区分开,而水溶性离子中的K+/Na+、Cl-/Na+比值也可以将稻草与一些树木类焚烧区别开来.     

Local PM10 and PM2.5 emission inventories from agricultural tillage and harvest in northeastern China

Mineral particles or particulate matters(PMs) emitted during agricultural activities are major recurring sources of atmospheric aerosol loading.However,precise PM inventory from agricultural tillage and harvest in agricultural regions is challenged by infrequent local emission factor(EF) measurements.To understand PM emissions from these practices in northeastern China,we measured EFs of PM_(10) and PM_(2.5) from three field operations(i.e.,tilling,planting and harvesting) in major crop production(i.e.,corn and soybean),using portable real-time PM analyzers and weather station data.County-level PM_(10) and PM_(2.5) emissions from agricultural tillage and harvest were estimated,based on local EFs,crop areas and crop calendars.The EFs averaged(107 ± 27),(17 ± 5) and 26 mg/m~2 for field tilling,planting and harvesting under relatively dry conditions(i.e.,soil moisture 15%),respectively.The EFs of PM from field tillage and planting operations were negatively affected by topsoil moisture.The magnitude of PM_(10) and PM_(2.5) emissions from these three activities were estimated to be 35.1 and 9.8 kilotons/yr in northeastern China,respectively,of which Heilongjiang Province accounted for approximately45%.Spatiotemporal distribution showed that most PM_(10) emission occurred in April,May and October and were concentrated in the central regions of the northeastern plain,which is dominated by dryland crops.Further work is needed to estimate the contribution of agricultural dust emissions to regional air quality in northeastern China.