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.     

GIS-based analysis of population exposure to PM2.5 air pollution—A case study of Beijing

PM_(2.5), formally defined as particulate matter with diameter less than 2.5 μm, is one of most harmful air pollutants threatening human health. Numerous epidemiological studies have shown that both short-term and long-term exposures to PM_(2.5) are strongly linked with respiratory diseases. In this study, various types of spatio-temporal data were collected and used to estimate the spatio-temporal variation of PM_(2.5) exposure in Beijing in 2014. The seasonal and daily variation of the population-weighted exposure level(PWEL) in 2014 was estimated and compared. The results show that the population exposure to ambient air pollution differs significantly in the four seasons, and the exposure levels in winter and spring are notably higher than the other seasons; the exposure level changes greatly from North to South, and each sub-district maintains similarity to neighboring sub-districts.     

Estimation of daily PM2.5 concentration and its relationship with meteorological conditions in Beijing

When investigating the impact of air pollution on health, particulate matter less than 2.5 μm in aerodynamic diameter(PM_(2.5)) is considered more harmful than particulates of other sizes. Therefore, studies of PM_(2.5) have attracted more attention. Beijing, the capital of China,is notorious for its serious air pollution problem, an issue which has been of great concern to the residents, government, and related institutes for decades. However, in China,significantly less time has been devoted to observing PM_(2.5) than for PM_(10). Especially before 2013, the density of the PM_(2.5) ground observation network was relatively low, and the distribution of observation stations was uneven. One solution is to estimate PM_(2.5) concentrations from the existing data on PM_(10). In the present study, by analyzing the relationship between the concentrations of PM_(2.5) and PM_(10), and the meteorological conditions for each season in Beijing from 2008 to 2014, a U-shaped relationship was found between the daily maximum wind speed and the daily PM concentration, including both PM_(2.5) and PM_(10). That is, the relationship between wind speed and PM concentration is not a simple positive or negative correlation in these wind directions; their relationship has a complex effect, with higher PM at low and high wind than for moderate winds.Additionally, in contrast to previous studies, we found that the PM_(2.5)/PM_(10) ratio is proportional to the mean relative humidity(MRH). According to this relationship, for each season we established a multiple nonlinear regression(MNLR) model to estimate the PM_(2.5) concentrations of the missing periods.     

Exposure to air pollutants in Vietnam: Assessing potential risk for tourists

Tourism can form an important component of a nation's GDP,and Vietnam is among the most visited countries in Southeast Asia.Most studies on personal exposure focus on the general population,or occupational cohorts with exposure to specific pollutants.However,short-term exposure to air pollutants while visiting regions with high levels of air pollution can lead to acute health effects.A personal exposure study was conducted across three cities in Vietnam to estimate exposure to particulate matter(PM_(2.5)) and black carbon for tourists.Measurements were conducted during the wet season in 2014 in Ho Chi Minh City,Da Lat and Nha Trang using portable instrumentation.Average 24-hr PM_(2.5) and BC exposures were estimated as 18.9 ± 9.24 and 3.41 ± 1.33 μg/m~3 and among the three cities,Ho Chi Minh was found to have the highest PM_(2.5) concentrations.Environmental tobacco smoke,commuting and street food stands were found to contribute to highest levels of exposure to PM_(2.5) and BC across all cities.     

Are current Chinese national ambient air quality standards on 24-hour averages for particulate matter sufficient to protect public health?

With rapid economic development and urbanization in recent decades, China has experienced the worsening of ambient air quality. For better air quality management to protect human health, Chinese government revised national ambient air quality standards(NAAQS) for particulate matter(PM) in 2012(GB3095-2012). To assess the effectiveness of current NAAQS for PM on public health in Chinese population, we conducted a metaanalysis on published studies examining the mortality risk of short-term exposure to PM with aerodynamic diameters less than 10 and 2.5 μm(PM_(10) and PM_(2.5)) in China. The reported24-hour concentrations of PM_(10) and PM_(2.5) in studies ranged from 43.5 to 150.1 μg/m~3 and 37.5 to 176.7 μg/m~3. In the pooled excess, mortality risk estimates of short-term exposure to PM.In specific, per 10 μg/m~3 increase in PM_(10), we observed increases of 0.40%(95%CI: 0.33%,0.47%), 0.57%(95%CI: 0.44%, 0.70%) and 0.49%(95%CI: 0.40%, 0.58%) in total, respiratory and cardiovascular mortality, per 10 μg/m~3 increase in PM_(2.5), we observed increases of 0.51%(95%CI: 0.38%, 0.63%), 0.62%(95%CI: 0.52%, 0.73%) and 0.75%(95%CI: 0.54%, 0.95%) in total,respiratory and cardiovascular mortality. Finally, we derived 125 μg/m~3 for PM_(10) and 62.5 μg/m~3 for PM_(2.5) as 24-hour recommendation values based on the pooled estimates. Our results indicated that current Chinese NAAQS for PM could be sufficient in mitigating the excess mortality risk from short-term exposure to ambient PM. However, future research on longterm exposure cohort studies in Chinese population is also essential in revising annual averages for PM in Chinese NAAQS.     

Variation of airborne quartz in air of Beijing during the Asia-Pacific Economic Cooperation Economic Leaders'' Meeting

Quartz particles are a toxic component of airborne paniculate matter(PM).Quartz concentrations were analyzed by X-ray diffraction in eighty-seven airborne PM samples collected from three locations in Beijing before,during,and after the Asia-Pacific Economic Cooperation(APEC) Leaders' Meeting in 2014.The results showed that the mean concentrations of quartz in PM samples from the two urban sites were considerably higher than those from the rural site.The quartz concentrations in samples collected after the APEC meeting,when the pollution restriction lever was lifted,were higher than those in the samples collected before or during the APEC meeting.The quartz concentrations ranged from 0.97 to 13.2 μg/m~3,which were among the highest values amid those reported from other countries.The highest quartz concentration exceeded the Californian Office of Environmental Health Hazard Assessment reference exposure level and was close to the occupational threshold limit values for occupational settings.Moreover,a correlation analysis showed that quartz concentrations were positively correlated with concentrations of pollution parameters PM_(10),PM_(2.5),SO_2 and NO_x,but were negatively correlated with O_3 concentration.The results suggest that the airborne quartz particles may potentially pose health risks to the general population of Beijing.     

Chemical characteristics of size-resolved aerosols in winter in Beijing

Size-resolved aerosols were continuously collected by a Nano Sampler for 13 days at an urban site in Beijing during winter 2012 to measure the chemical composition of ambient aerosol particles. Data collected by the Nano Sampler and an ACSM(Aerodyne Aerosol Chemical Speciation Monitor) were compared. Between the data sets,similar trends and strong correlations were observed,demonstrating the validity of the Nano Sampler. PM10 and PM2.5concentrations during the measurement were 150.5 ± 96.0 μg/m3(mean ± standard variation)and 106.9 ± 71.6 μg/m3,respectively. The PM2.5/PM10 ratio was 0.70 ± 0.10,indicating that PM2.5dominated PM10. The aerosol size distributions showed that three size bins of 0.5–1,1–2.5 and 2.5–10 μm contributed 21.8%,23.3% and 26.0% to the total mass concentration(TMC),respectively. OM(organic matter) and SIA(secondary ionic aerosol,mainly SO42-,NO3-and NH4+) were major components of PM2.5. Secondary compounds(SIA and secondary organic carbon) accounted for half of TMC(about 49.8%) in PM2.5,and suggested that secondary aerosols significantly contributed to the serious particulate matter pollution observed in winter. Coal burning,biomass combustion,vehicle emissions and SIA were found to be the main sources of PM2.5. Mass concentrations of water-soluble ions and undetected materials,as well as their fractions in TMC,strikingly increased with deteriorating particle pollution conditions,while OM and EC(elemental carbon) exhibited different variations,with mass concentrations slightly increasing but fractions in TMC decreasing.     

Chemical characterisation of particulate matter in urban transport modes

Traffic is a main source of air pollutants in urban areas and consequently daily peak exposures tend to occur during commuting. Personal exposure to particulate matter (PM) was monitored while cycling and travelling by bus, car and metro along an assigned route in Lisbon (Portugal), focusing on PM2.5 and PM10 (PM with aerodynamic diameter <2.5 and 10 µm, respectively) mass concentrations and their chemical composition. In vehicles, the indoor-outdoor interplay was also evaluated. The PM2.5 mean concentrations were 28?±?5, 31?±?9, 34?±?9 and 38?±?21?µg/m³ for bus, bicycle, car and metro modes, respectively. Black carbon concentrations when travelling by car were 1.4 to 2.0 times higher than in the other transport modes due to the closer proximity to exhaust emissions. There are marked differences in PM chemical composition depending on transport mode. In particular, Fe was the most abundant component of metro PM, derived from abrasion of rail-wheel-brake interfaces. Enhanced concentrations of Zn and Cu in cars and buses were related with brake and tyre wear particles, which can penetrate into the vehicles. In the motorised transport modes, Fe, Zn, Cu, Ni and K were correlated, evidencing their common traffic-related source. On average, the highest inhaled dose of PM2.5 was observed while cycling (55 µg), and the lowest in car travels (17 µg). Cyclists inhaled higher doses of PM2.5 due to both higher inhalation rates and longer journey times, with a clear enrichment in mineral elements. The presented results evidence the importance of considering the transport mode in exposure assessment studies.     

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.     

Pollution levels and characteristics of phthalate esters in indoor air in hospitals

The concentrations of phthalate esters(PAEs) in Chinese hospitals were investigated by simultaneously determining concentrations of gas- and particle-phase PAEs. PAEs were detected in two third-class first-grade hospitals, two second-class first-grade hospitals, and a community health service center. Hospital drugstores had the highest concentration(24.19 μg/m3), which was 1.54 times that of newly decorated houses. The second highest concentration was found in the transfusion rooms, averaging 21.89 μg/m3; this was followed by the concentrations of PAEs in the nurse's workstations, the wards, and the doctor's offices, with mean concentrations of 20.66, 20.0, and 16.92 μg/m3, respectively. The lowest concentrations were found in the hallways(16.30 μg/m3). Of the six different kinds of PAEs found, major pollutants included diethyl phthalates, dibutyl phthalates, butylbenzyl phthalates and di(2-ethylhexyl) phthalates, comprising more than 80% of all PAEs present.Meanwhile, a comparison between different wards showed that PAE concentrations in the maternity wards were 1.63 times higher than in the main wards. Based on known health hazards, our results suggest that the PAEs seriously influence the health of the pregnant women and babies; therefore, it is of great importance to take the phthalate concentrations in hospitals into consideration. In addition, hospital indoor air was more seriously contaminated than the air of newly decorated houses.     

Quantifying hysteresis of atrazine desorption from a sandy loam soil

Batch experiments were carried out to investigate the effects of initial atrazine concentrations and consecutive desorption steps on the desorption characteristics of atrazine from a sandy loam soil.As initial atrazine concentration increased,the average percentage of atrazine desorption on the sandy loam soil ranged gradually from 23.1% to 38.5% after five consecutive desorption steps.The values of the Freundlich capacity parameter,kdes,derived from the initial concentration and time-dependent desorption isotherm were consistently higher than those associated with sorption.The opposite trend was observed only for the values of nonlinear parameter,ndes,from the initial concentration-dependent desorption isotherms.Atrazine hydrolysis to hydroxyatrazine and bound residue formation were mainly responsible for the observed hysteresis in its sorption and desorption isotherms.For the initial concentration-dependent desorption isotherms,as initial atrazine concentration increased,the values of hysteretic coefficients ω and λ decreased,and H values increased.However,the relationships between initial atrazine concentration and hysteretic coefficients were not pronounced for ω,H,or λ.For the time-dependent desorption isotherms,λ and H values increased as the atrazine desorption step proceeded.The correlation between hysteretic coefficient and desorption step was highly significant for λ (P 0.0001),but not for H.     

潮土中阿特拉津解吸滞后特征

采用批量动态实验方法,研究了阿特拉津初始浓度与解吸时间对潮土中阿特拉津解吸滞后特征的影响.结果表明:土壤溶液中阿特拉津的浓度随其解吸时间的增加而逐渐下降,二者间可用经验指数公式表达.阿特拉津连续解吸5d后,阿特拉津的初始浓度从50μg·L^-1增加到2 000μg·L^-1时,对应解吸率分别为23.1%、30.4%、33.0%、36.4%和38.5%.土壤吸附阿特拉津与对应土壤溶液中阿特拉津浓度关系可用传统和依时解吸等温线2种方式描述.无论传统还是依时解吸等温线都与吸附进行到168h的吸附等温线之间存在着解吸的滞后现象.传统和依时Freundlich解吸等温线参数能对吸附解吸等温线的滞后作用进行量化,滞后系数ω只适合传统解吸等温线的滞后量化,而滞后系数H和λ对2类解吸等温线都适用.     

天然土壤中菲的解吸行为特征研究

选取天然土壤样品,以菲作为代表性污染物,利用批量吸附-解吸实验考察不同初始浓度、不同吸附时间条件下菲解吸行为的滞后性特征.实验数据采用Freundlich方程式拟合,并由基于热力学的TII指数表征.结果表明,天然土壤吸持菲的比例随其初始浓度的增加而减少.在土壤多次解吸过程中,每次释放菲的比例随其初始浓度的升高而增加,随解吸次数的增加而减少.吸附过程的拟合指数n大于解吸过程的对应值,并随初始固相浓度的加大而增加.天然土壤吸附-解吸过程的滞后性特征表现为初始固相浓度越高,TII值越接近0,滞后性越弱;反之,则TII值越接近1,滞后性越强.另外,吸附平衡时间30 d对应的n值小于5 d的,而两者的TII值随初始浓度增高则呈现降低趋势.就同一浓度而言,吸附平衡30 d所对应的TII值高于5 d的.     

阿特拉津及其代谢物在砂质壤土中的吸附

采用批量平衡法研究了阿特拉津（AT）及其主要代谢物脱乙基阿特拉津（DEA）和脱异丙基阿特拉津（DIA）在砂质壤土中的吸附行为,讨论了离子强度和温度对吸附的影响.结果表明,3种化合物的吸附24h基本达到平衡,吸附量大小顺序为AT > DIA > DEA;二级动力学模型可以很好地预估平衡吸附容量和初始吸附速率常数,颗粒内扩散方程表明颗粒扩散不是唯一的控速手段,Elovich方程拟合所得AT、DEA和DIA的瞬时吸附占各自吸附总量的53%、85%和80%;Freundlich方程能很好地描述3种化合物在供试土壤中的吸附特性,吸附系数（K_f）范围为0.7992~1.3201mg^1-1/n·mL^1/n/kg,经验常数1/n范围为0.7440~0.7530.溶液的离子强度和温度影响土壤对化合物的吸附,温度升高,K_f值降低;CaCl₂从0~0.01mol/L,K_f值增大,再继续增加,吸附系数有降低的趋势.     

林丹的吸附解吸行为对其沉积物基准的影响

研究了林丹在3种沉积物上的吸附/解吸行为.结果表明,在3种沉积物上的吸附等温线都符合Freundlich模型,其吸附性能受有机碳含量和颗粒分布的影响.而解吸等温线明显地偏离吸附等温线,存在显著的解吸滞后现象,解吸用二元平衡解吸(DED)模型进行拟合,效果良好.解吸不可逆程度随着沉积物中林丹初始浓度增大而增大.由DED模型推算的沉积物基准值比用线性模型推算的基准值高46倍以上.     

熟污泥改性黄土对铜的吸附解吸特征

为探明熟污泥改性黄土对重金属的容纳能力,以熟污泥改性黄土为供试土样,采用序批实验法研究了供试土样对铜(Cu)的吸附解吸特征,并分析了供试土样对铜的固定能力及影响因素.供试土样对铜的吸附量在铜添加浓度小于100mg/L时急剧增加,在铜添加浓度大于100mg/L时增加缓慢,而解吸量的变化趋势则恰恰相反.Langmuir型吸附等温式是描述供试土样对铜的吸附过程的最佳模型,而吸附量与解吸量的关系可以很好的用指数函数来描述.供试土样对铜的固定吸附量随熟污泥含量的增加而增加,有机质含量是决定性因素.     

Adsorption–desorption behavior of atrazine on agricultural soils in China

Adsorptionanddesorptionareimportantprocessesthataffectatrazinetransport,transformation,andbioavailabilityinsoils.Inthisstudy,theadsorption–desorptioncharacteristicsofatrazinein three soils (laterite, paddy soil and alluvial soil) were evaluated using the batch equilibrium method. The results showed that the kinetics of atrazine in soils was completed in two steps: a “fast” adsorption and a “slow” adsorption and could be well described by pseudo-second-order model.In addition,the adsorption equilibrium isotherms were nonlinear and were well fitted by Freundlich and Langmuir models. It was found that the adsorption data on laterite, and paddy soil were better fitted by the Freundlich model;as for alluvial soil,the Langmuir model described it better. The maximum atrazine sorption capacities ranked as follows: paddy soil > alluvial soil > laterite. Results of thermodynamic calculations indicated that atrazine adsorption on three tested soils was spontaneous and endothermic. The desorption data showed that negative hysteresis occurred. Furthermore, lower solution pH value was conducive to the adsorptionofatrazineinsoils.Theatrazineadsorptioninthesethreetestedsoilswascontrolled by physical adsorption, including partition and surface adsorption. At lower equilibrium concentration, the atrazine adsorption process in soils was dominated by surface adsorption;while with the increase of equilibrium concentration, partition was predominant.     

Effect of biosurfactant[0] on the sorption of phenanthrene onto original and H2O2-treated soils

The objective of this study was to examine the effect of biosurfactant on sorption of phenanthrene (PHE) onto the original or H2O2-treated black loamy soil (typic isohumisols) and red sandy soil (typic ferralisols). The sorption isotherms were performed with the original and "soft" carbon-removed soils in the presence and absence of biosurfactant (200 mg/L). The sorption and degradation of biosurfactant were investigated. The result showed that organic matter played an important role in PHE sorption onto the black loamy and red sandy soils, and the PHE sorption isotherms on the "soft" carbon-removed soils exhibited more nonlinearity than those on the original soils. The values of partition coefficient (Kd) on the original black loamy soil with or without 200 mg/L biosurfactant were 181.6 and 494.5 mL/g, respectively. Correspondingly, in the red sandy soil, Kd was 246.4 and 212.8 mL/g in the presence or absence of biosurfactant, respectively. The changes of Kd suggested that biosurfactant inhibited PHE sorption onto the black loamy soil, but facilitated PHE sorption onto the red sandy soil. The nonlinearity of PHE sorption isotherm was decreased in the presence of biosurfactant. Site specific sorption might occur during PHE sorption onto both the original and the "soft" carbon-removed soils in the presence of biosurfactant. It was noted that biosurfactant could also be sorbed onto soils. The maximal sorption capacity of the red sandy soil for biosurfactant was (76.9 ± 0.007) μg/g, which was 1.31 times that of black loamy soil. Biosurfactant was degraded quickly in the two selected soils, and 92% of biosurfactant were mineralized throughout the incubation experiment for 7 d. It implied that biosurfactant should be added frequently when the remediation of polycyclic aromatic hydrocarbon (PAH)-contaminated soils was conducted through PAH desorption approach facilitated by biosurfactant.     

Impact of atrazine and nitrogen fertilizers on the sorption of chlorotoluron in soil and model sorbents

Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.     

表面活性剂对苯并[a]芘在黑炭表面吸附解吸的影响

通过静态吸附实验,研究了3种不同类型的表面活性剂(阳离子∶十六烷基三甲基溴化铵,CTAB;阴离子∶十二烷基苯磺酸钠,SDBS∶非离子,曲拉通100,TX100)对苯并[a]芘(BaP)在黑炭表面吸附解吸的影响.结果表明,3种表面活性剂的存在均会增加BaP在黑炭表面吸附的非线性程度.CTAB的存在可以促进BaP在黑炭表面的吸附同时抑制了BaP的解吸,然而SDBS的存在降低了BaP在黑炭表面的吸附并增加了吸附过程的可逆性.与CTAB和SDBS不同,TX100对BaP在黑炭表面吸附解吸的影响取决于其添加浓度.低浓度的TX100(50 mg.L-1)能够促进BaP在黑炭上的吸附并抑制BaP的解吸,吸附能力参数Kd值(在ce=50μg.L-1下)从188 062 mL.g-1增大到264 179 mL.g-1,解吸滞后指数HI从0.44降低到0.39.随着TX100浓度增加到150 mg.L-1和200 mg.L-1,TX100对BaP的吸附表现出抑制作用并能够促进BaP的解吸,Kd值(在ce=50μg.L-1下)从188 062 mL.g-1分别降低到182 751 mL.g-1和178 730 mL.g-1,解吸滞后指数从0.44分别升高到0.65和0.70.本研究为预测多环芳烃在表面活性剂污染的环境中的分布特征和最终归趋提供了理论依据.