石家庄市大气颗粒物元素组分特征分析

为研究石家庄市大气颗粒物的污染特征及其来源,于2013年4—5月在主城6区分别采集TSP、PM10和PM2.5颗粒物样品,利用ICP-MS分析其中的22种元素浓度。结果表明,石家庄市城区Ca、Fe元素在各粒径颗粒物中含量都较高,PM2.5中的S、K含量较高,PM10和TSP中Mg、Al的浓度相对较高。颗粒物的主要来源为燃煤尘、道路尘和建筑尘,TSP、PM10和PM2.5具有较好的统计相关性和同源性。     

Characterisation of Particulate Matter Sampled during a Study of Children's Personal Exposure to Airborne Particulate Matter in a UK Urban Environment

The personal exposure of children aged 9 – 11 years to particulate matter (PM₁₀ and PM_2.5) was carried out between January and September 1997 in the London Borough of Barnet. Personal sampling along with home, garden and classroom microenvironmental monitoring was completed for all ten children. Each child was monitored for five days during winter, spring and summer. All children completed daily time activity diaries to provide information on any potential activities that could influence their exposure to particulate matter. Each evening a household activity questionnaire was also completed by the parents. Personal Environmental Monitors were used to sample personal exposure to PM₁₀ and PM_2.5. Harvard Impactors were used for the microenvironmental sampling of both size fractions. The children's mean personal exposure concentrations for PM₁₀ during winter, spring and summer were 72, 54 and 35 µg/m³ respectively and for PM_2.5 22, 17 and 18 µg/m³ respectively. In order to determine the potential sources of particulate matter, analysis of the Teflon filters has been undertaken. The physical characteristics of the particles have been identified using Scanning Electron Microscopy. The relationships between personal exposure concentrations and the different microenvironments will be discussed.     

Influence of Meteorological Parameters on Particulates and Atmospheric Pollutants at Taichung Harbor Sampling Site

Atmospheric aerosol particles and metallic concentrations, ionic species were monitored at the Experimental harbor of Taichung sampling site in this study. This work attempted to characterize metallic elements and ionic species associated with meteorological conditions variation on atmospheric particulate matter in TSP, PM_2.5, PM_2.5–10. The concentration distribution trend between TSP, PM_2.5, PM_2.5–10 particle concentration at the TH (Taichung harbor) sampling site were also displayed in this study. Besides, the meteorological conditions variation of metallic elements (Fe, Mg, Cr, Cu, Zn, Mn and Pb) and ions species (Cl⁻, NO₃ ⁻, SO₄ ²⁻, NH₄ ⁺, Mg²⁺, Ca²⁺ and Na⁺) concentrations attached with those particulate were also analyzed in this study. On non-parametric (Spearman) correlation analysis, the results indicated that the meteorological conditions have high correlation at largest particulate concentrations for TSP at TH sampling site in this study. In addition, the temperature and relative humidity of meteorological conditions that played a key role to affect particulate matter (PM) and have higher correlations then other meteorological conditions such as wind speed and atmospheric pressure. The parameter temperature and relative humidity also have high correlations with atmospheric pollutants compared with those of the other meteorological variables (wind speed, atmospheric pressure and prevalent wind direction). In addition, relative statistical equations between pollutants and meteorological variables were also characterized in this study.     

波长色散-X射线荧光光谱法测定PM2.5中23种元素

研究以单元素标准膜为基础，结合NIST SRM 2783颗粒物滤膜标准样品，建立了波长色散-X射线荧光光谱法测定PM_2.5中23种无机元素的测定方法，优化了测试条件，测量一个样品耗时约15 min，计算了各元素的方法检出限。对NIST SRM 2783滤膜标准品在一周内重复测定10次来计算方法的准确度与精密度，测定结果显示大多数元素的测量值在给出的参考值范围内，且测量标准偏差一般在10%以内。对比了石英与聚四氟乙烯材质（Teflon）滤膜的空白值，石英滤膜中Si、Fe、Na、Mg、Al、K、Ca等元素的背景值较高，Teflon滤膜的背景值较低，推荐选用Teflon滤膜作为PM_2.5组分分析采样滤膜。分别用波长色散-X射线荧光光谱法及酸消解-ICP-MS法测定了样品膜中的元素组分，得到的测定结果基本一致。     

Human health damage caused by particulate matter PM10 and ozone in urban environments: the case of Athens, Greece

Studies conducted over the past decades have provided substantial evidence that both the long- and the short-term exposures to ozone and particulate matter are responsible for mortality and cardiopulmonary morbidity. This paper examines the relationship between exposure to ambient concentrations of ozone (O₃) and particulate matter with aerodynamic diameter of less than 10 μm (PM₁₀) and public health and provides the quantification of the burden of disease from PM₁₀ and O₃-related mortality and morbidity through a Life Cycle Impact Assessment focused on the greater area of Athens, Greece. Thus, characterizations factors (CFs) for human health damage are calculated in 17 sites in Athens, in terms of the annual marginal change in the disability-adjusted life years (DALYs) due to a marginal increase in the ambient concentrations. It is found that the PM₁₀ intake factors range between 1.25?×?10^?6 and 2.78?×?10^?6, suggesting that 1.25–2.78 μg of PM₁₀ are inhaled by the Athenian population per kg of PM₁₀ in the urban atmosphere. Mortality due to chronic exposure to PM₁₀ has a dominant contribution to years of life lost with values ranging between 6.2?×?10^?5 and 1.1?×?10^?4. On the other hand, the mortality caused by short-term exposure to O₃ is weaker with the CFs ranging between 1.58?×?10^?7?years of life lost in the urban/traffic areas and 4.71?×?10^?7?years in the suburbs. Finally, it is found that 9,000 DALYs are lost on average in Athens, corresponding to 0.0018 DALYs per person. This is equal to 0.135 DALYs per person over a lifetime of approximately 75 years, assuming constant emission rates for the whole period.     

Indoor and outdoor PM mass and number concentrations at schools in the Athens area

Simultaneous indoor and outdoor PM₁₀ and PM_2.5 concentration measurements were conducted in seven primary schools in the Athens area. Both gravimetric samplers and continuous monitors were used. Filters were subsequently analyzed for anion species. Moreover ultrafine particles number concentration was monitored continuously indoors and outdoors. Mean 8-hr PM₁₀ concentration was measured equal to 229 ± 182 μg/m³ indoors and 166 ± 133 μg/m³ outdoors. The respective PM_2.5 concentrations were 82 ± 56 μg/m³ indoors and 56 ± 26 μg/m³ outdoors. Ultrafine particles 8-h mean number concentration was measured equal to 24,000 ± 17,900 particles/cm³ indoors and 32,000 ± 14,200 particles/cm³ outdoors. PM₁₀ outdoor concentrations exhibited a greater spatial variability than the corresponding PM_2.5 ones. I/O ratios were close or above 1.00 for PM₁₀ and PM_2.5 and smaller than 1.00 for ultrafine particles. Very high I/O ratios were observed when intense activities took place. The initial results of the chemical analysis showed that accounts for the 6.6 ± 3.5% of the PM₁₀ and for the 3.1 ± 1.4%.The corresponding results for PM_2.5 are 12.0 ± 7.7% for and 3.1 ± 1.9% for . PM_2.5 indoor concentrations were highly correlated with outdoor ones and the regression line had the largest slope and a very low intercept, indicative of no indoor sources of fine particulate . The results of the statistical analysis of indoor and outdoor concentration data support the use of as a proper surrogate for indoor PM of outdoor origin.     

Particulate matter levels in a South American megacity: the metropolitan area of Lima-Callao,Peru

The temporal and spatial trends in the variability of PM₁₀ and PM_2.5 from 2010 to 2015 in the metropolitan area of Lima-Callao, Peru, are studied and interpreted in this work. The mean annual concentrations of PM₁₀ and PM_2.5 have ranges (averages) of 133–45 μg m^?3 (84 μg m^?3) and 35–16 μg m^?3 (26 μg m^?3) for the monitoring sites under study. In general, the highest annual concentrations are observed in the eastern part of the city, which is a result of the pattern of persistent local winds entering from the coast in a south-southwest direction. Seasonal fluctuations in the particulate matter (PM) concentrations are observed; these can be explained by subsidence thermal inversion. There is also a daytime pattern that corresponds to the peak traffic of a total of 9 million trips a day. The PM_2.5 value is approximately 40% of the PM₁₀ value. This proportion can be explained by PM₁₀ re-suspension due to weather conditions. The long-term trends based on the Theil-Sen estimator reveal decreasing PM₁₀ concentrations on the order of ?4.3 and ?5.3% year^?1 at two stations. For the other stations, no significant trend is observed. The metropolitan area of Lima-Callao is ranked 12th and 16th in terms of PM₁₀ and PM_2.5, respectively, out of 39 megacities. The annual World Health Organization thresholds and national air quality standards are exceeded. A large fraction of the Lima population is exposed to PM concentrations that exceed protection thresholds. Hence, the development of pollution control and reduction measures is paramount.     

Characterization of particulate matter and its related metal toxicity in an urban location in South West India

This study reports the quantification of the toxicity of particulate matter (PM)-bound metals and their possible associated risks to human health. For assessment of PM, 24-h samples of PM₁₀ and PM_2.5 were collected by Mini Vol-TAS sampler at an urban site of Pune. Samples were sequentially extracted with ultrapure water and concentrated HNO₃ and analyzed for “soluble” and “total” metals. Factor analysis identified the resuspension of road dust due to traffic, biomass burning, construction activities, and wind-blown dust as possible sources that played an important role for overall pollution throughout the year. Water-soluble proportion was found to be ≤20 % for Cr, Co, Fe, and Al; ≥50 % for Sr, Cd, Ca, and Zn; and a substantial proportion (～25–45 %) for Mn, Ba, K, Na, Ni, Mg, Cu, and Pb metals in PM₁₀. For PM_2.5, the water-soluble proportion was ≤20 % for Fe, Co, Ni, Cr, and Al, while Sr, K, and Cd were mostly soluble (>50 %) and Cu, Ba, Mn, Ca, Zn, Pb, Na, and Mg were substantially soluble (～25–45 %). In the present study, among the toxic metals, Cd and Pb show higher concentration in the soluble fraction and thus represent the higher bioavailability index and especially are harmful to the environment and exposed person. Risk calculations with a simple exposure assessment method showed that the cancer risks of the bioavailable fractions of Cr, Cd and Ni were greater than the standard goal.     

Differences in the Spatial Distribution and Chemical Composition of PM10 Between the UK and Poland

The Fine Resolution Atmospheric Multi-pollutant Exchange Model was used to calculate the spatial distribution and chemical composition of PM₁₀ concentrations for two geographically remote countries in Europe—the UK and Poland—for the year 2007. These countries are diverse in terms of pollutant emissions as well as climate conditions. Information on the contribution of natural and anthropogenic as well as national and imported particles in total PM₁₀ concentrations in both countries is presented. The paper shows that the modelled national annual average PM₁₀ concentrations, calculated for the entire country area, are similar for the UK and Poland and close to 12 μg m^?3. Secondary inorganic aerosols dominate the total PM₁₀ concentrations in Poland. Primary particulate matter has the greatest contribution to total PM₁₀ in the UK, with large contribution of base cations. Anthropogenic sources predominate (81 %) in total PM₁₀ concentrations in Poland, whereas natural prevail in the UK—hence, the future reduction of PM₁₀ air concentrations by emissions reduction could be more difficult in the UK than in Poland.     

Size-segregated trace elements in continental suburban aerosols: seasonal variation and estimation of local,regional, and remote emission sources

We have measured trace element contents in suburban aerosols from six size fractions in the range of PM_0.27–16 from a background station in Belgrade (Serbia). The distribution and concentration of elements were determined within each of the investigated Dp fractions with emphasis on the fine and coarse modes. Fine/coarse mode ratios of element can provide information regarding their anthropogenic or natural origin. Analysis of seasonal variations of element contents in fine and coarse mode show that Cd, Co, K, and V have higher concentrations in the fine mode during heating season, while Fe contents are lower. In the coarse mode, Cu and V have higher concentrations during the heating season, while Al, Fe, Mg, Mn, and Sb contents are lower. We also apply a distribution probability model (normal, log-normal, and three-parameter Weibull) as new approach to estimate the distances of emission sources that can contribute to pollutant contents in particulate matter of the investigated location.     

Ionic and heavy metal composition of respirable particulate in Madurai, India

Airborne particulate matter (PM₁₀) was collected for a period of 1 year at six locations in Madurai city, India. The chemical analyses on PM₁₀ samples were carried out for the estimation of heavy metals and ions using atomic absorption spectroscopy and ion chromatography respectively. The average PM₁₀ concentrations varied from 97.2 to 152.5 μg/m³, which were found to be below the Indian air quality standards. While industrial areas had the highest concentrations of heavy metals such as Fe, Zn and Cr and also the $\text{SO}_{4}^{2-}$ ions, traffic areas with relatively higher traffic densities in the city endured highest concentrations of Cd and the $\text{NO}_{3}^{-}$ ion. As gaseous pollutants serve as precursors of ionic particles in the atmospheric environment, gaseous pollution control is necessitated along with particulate with special reference to heavy metal and ion pollution abatement for the sustainable development of Madurai city.     

Seasonal Variations of PM10 and TSP in Residential and Industrial Sites in an Urban Area of Kolkata, India

The objective of the study is to investigate seasonal and spatial variations of PM₁₀ (particulate matter with aerodynamic diameter less than or equal to 10 μm) and TSP (total suspended particulate matter) of an Indian Metropolis with high pollution and population density from November 2003 to November 2004. Ambient concentration measurements of PM₁₀ and TSP were carried out at two monitoring sites of an urban region of Kolkata. Monitoring sites have been selected based on the dominant activities of the area. Meteorological parameters such as wind speed, wind direction, rainfall, temperature and relative humidity were also collected simultaneously during the sampling period from Indian Meteorological Department, Kolkata. The 24 h average concentrations of PM₁₀ and TSP were found in the range 68.2–280.6 μg/m³ and 139.3–580.3 μg/m³ for residential (Kasba) area, while 62.4–401.2 μg/m³ and 125.7–732.1 μg/m³ for industrial (Cossipore) area, respectively. Winter concentrations of particulate pollutants were higher than other seasons, irrespective of the monitoring sites. It indicates a longer residence time of particulates in the atmosphere during winter due to low winds and low mixing height. Spread of air pollution sources and non-uniform mixing conditions in an urban area often result in spatial variation of pollutant concentrations. The higher particulate pollution at industrial area may be attributed due to resuspension of road dust, soil dust, automobile traffic and nearby industrial emissions. Particle size analysis result shows that PM₁₀ is about 52% of TSP at residential area and 54% at industrial area.     

Seasonal air quality profile of inorganic ionic composition of PM10 near Taj Mahal in Agra, India

Atmospheric aerosols and their impacts on the environment particularly on human health is an issue of significant public and governmental concern. Though studies on air quality related to total suspended particulate matter have done by various authors in India, yet respirable suspended particulate matter (PM₁₀) is not characterized so far particularly in a historical and world heritage city like Agra. This study presents seasonal variation in mass levels of PM₁₀ and its ionic composition. PM₁₀ samples were collected in the proximity of Taj Mahal and subjected to chemical analysis using ion chromatography technique. The preliminary findings reveal that the 24-h average of PM₁₀ mass level varies from 115 to 233, 155 to 321, and 33 to 178 μg/m³, respectively, in summer, winter, and rainy seasons indicating critical pollution situation. These values are very much higher than the National Ambient Air Quality Standards of 75 μg/m³ (prescribed by Central Pollution Control Board, India) in both of summer and winter seasons whereas quite near the permissible limits in rainy season. The equivalent ratios of NH₄ ⁺ to nonsea salt SO₄ ^2? and NO₃ ^? and ∑Cations to ∑Anios were found to be greater than unity indicating high source strength of ammonia and alkaline nature of aerosols. The study suggests the need for continuous and long-term systematical sampling and detailed physiochemical analysis of PM₁₀ and also to know the characteristics of PM in background areas for better understanding of the emission sources.     

Atmospheric aerosols at a regional background Himalayan site—Mukteshwar, India

Continuous aerosol measurements were made at a regional background station (Mukteshwar) located in a rural Himalayan mountain terrain from December 2005 to December 2008 for a period of 3 years. The average concentrations of particulate matter less than or equal to 10 μm (PM₁₀), particulate matter less than or equal to 2.5 μm (PM_2.5) and black carbon (BC) are 46.0, 26.6 and 0.85 μg/m³ during the study period. Majority of the PM₁₀ values lie below 100 μg/m³ while majority of the PM_2.5 values lie below 30 μg/m³. It is further seen that during the monsoon months, especially July and August, the average values are comparatively low. It is also noted that the PM_2.5/PM₁₀ ratios between 0.50 and 0.75 have the maximum frequency distribution in the data set. Furthermore, the monthly mean ratio of BC to PM_2.5 mass lies between 3.0 and 7.5 % during the study period. Though the average PM₁₀ and PM_2.5 concentrations during the study period are less than the respective Indian ambient air quality standards, however, they are still above the WHO guidelines and would have adverse health impacts. This shows that even in rural/background regions that are far away from major pollution sources or urban areas, the aerosol concentrations are significant and require long-term monitoring, source quantification and aerosol model simulations.     

Diurnal concentrations variations,size distributions for ambient air particles and metallic pollutants (Cr,Mn, Ni,Cd, Pb) during summer season at a traffic area

This study characterized and discussed particulate ambient air particulate concentrations and seasonal variations for PM₁₈, PM₁₀, PM_2.5, and PM₁ during June 2013–July 2013 at this traffic sampling site. In addition, this study also characterized the ambient air particulates size distributions by using MOUDI-100S4 sampler to collect 1-day the ambient suspended particles (PM₁₈, PM₁₀, PM_2.5, and PM₁) at this sampling site. In addition, the study also showed that the main pollutants contributions were from traffic and residual areas. As for the pollutants seasonal concentrations variations, the results indicated that the average particle concentrations orders were all displayed as daytime?>?nighttime for PM₁₈, PM₁₀, PM_2.5 and PM₁ at this characteristic sampling site. The results further indicated that the mean highest of metal concentrations in this study indicated that the average metal concentration were all displayed as Mn?>?Cr?>?Ni?>?Pb?>?Cd for PM₁₈, PM₁₀, PM_2.5 and PM₁ on daytime and nighttime at this characteristic sampling site.     

Chemical composition of ambient particulate matter and redox activity

Exposure to ambient particulate matter (PM) has been associated with a number of adverse health effects. Increasing studies have suggested that such adverse health effects may derive from oxidative stress, initiated by the formation of reactive oxygen species (ROS) within affected cells. The study aimed to assess physical characteristics and chemical compositions of PM and to correlate the results to their redox activity. PM_2.5 (mass aerodynamic diameter ≤2.5 μm) and ultrafine particles (UFPs, mass media aerodynamic diameter <0.1 μm) were collected in an urban area, which had heavy traffic and represented ambient air pollution associated with vehicle exhaust. Background samples were collected in a rural area, with low traffic flow. Organic carbon (OC), elemental carbon (EC), polycyclic aromatic hydrocarbons (PAHs), and metals were analyzed. The dithiothreitol activity assay was used to measure the redox activity of PM. Results showed that UFPs have higher concentrations of OC, EC, and PAHs than those of PM_2.5. Several metals, including Fe, Cu, Zn, Ti, Pb, and Mn, were detected. Among them, Cu had the highest concentrations, followed by Fe and Zn. Organic carbon constituted 22.8% to 59.7% of the content on the surface of PM_2.5 and UFPs. Our results showed higher redox activity on a per PM mass basis for UFPs as compared to PM_2.5. Linear multivariable regression analyses showed that redox activity highly correlated with PAH concentrations and organic compounds, and insignificantly correlated with EC and metals, except soluble Fe, which increased redox activity in particle suspension due to the presence of ROS.     

抚顺市PM10中元素分布特征及来源分析

为了确定抚顺市PM10中元素的浓度特征及其来源,于2006—2007年的采暖季、风沙季和非采暖季在抚顺市的6个采样点采集PM10样品,并用等离子体原子发射光谱法(ICP-AES)测定样品中Ti、Al、Mn、Mg、Ca、Na、K、Cu、Zn、As、Pb、Cr、Ni、Co、Cd、Fe、V等17种元素的含量。结果表明,Al、Mg、Ca、Na、K、Mn、Fe等地壳元素在17种元素中占有较大比重,全年平均达到97.0%。富集因子分析结果表明,Cu、Zn、Pb、Cr、Co、Cd等元素在各季和各采样点明显受到人为活动影响,是典型的污染元素。主因子分析结果显示,土壤风沙尘、建筑尘、燃煤尘、道路扬尘、机动车尾气排放、金属冶炼、锰、铜、钛工业源是抚顺市PM10中元素的主要来源。     

Particulate matter concentration in ambient air and its effects on lung functions among residents in the National Capital Region, India

The World Health Organization has estimated that air pollution is responsible for 1.4 % of all deaths and 0.8 % of disability-adjusted life years. NOIDA, located at the National Capital Region, India, was declared as one of the critically air-polluted areas by the Central Pollution Control Board of the Government of India. Studies on the relationship of reduction in lung functions of residents living in areas with higher concentrations of particulate matter (PM) in ambient air were inconclusive since the subjects of most of the studies are hospital admission cases. Very few studies, including one from India, have shown the relationship of PM concentration and its effects of lung functions in the same location. Hence, a cross-sectional study was undertaken to study the effect of particulate matter concentration in ambient air on the lung functions of residents living in a critically air-polluted area in India. PM concentrations in ambient air (PM_1, PM_2.5) were monitored at residential locations and identified locations with higher (NOIDA) and lower concentrations (Gurgaon). Lung function tests (FEV₁, PEFR) were conducted using a spirometer in 757 residents. Both air monitoring and lung function tests were conducted on the same day. Significant negative linear relationship exists between higher concentrations of PM₁ with reduced FEV₁ and increased concentrations of PM_2.5 with reduced PEFR and FEV₁. The study shows that reductions in lung functions (PEFR and FEV₁) can be attributed to higher particulate matter concentrations in ambient air. Decline in airflow obstruction in subjects exposed to high PM concentrations can be attributed to the fibrogenic response and associated airway wall remodeling. The study suggests the intervention of policy makers and stake holders to take necessary steps to reduce the emissions of PM concentrations, especially PM_1, PM_2.5, which can lead to serious respiratory health concerns in residents.     

北京城区降水对PM2.5和PM10清除作用分析

基于北京市PM_2.5和PM₁₀质量浓度、组分浓度以及降水数据,利用数理统计、相关性分析等方法分别从降水总量、降水时长和降水前颗粒物浓度3个角度研究降水对PM_2.5、PM₁₀的清除作用,同时以一次典型降水过程为例,具体分析降水对颗粒物的影响。结果表明：降水总量的增加有助于促进PM_2.5、PM₁₀的清除,随着降水总量增加,PM_2.5、PM₁₀的平均清除率提高,有效清除的比例增加;连续降水可增强对大气颗粒物的湿清除作用,连续降水达3d可有效降低PM_2.5、PM₁₀浓度;降水对PM_2.5、PM₁₀浓度的清除率和大气颗粒物前一日的平均浓度有较好的正相关性。降水对大气颗粒物的清除可分为清除、回升和平稳3个阶段,各个阶段大气颗粒物的变化趋势不同。降水对于大气气溶胶化学组分和酸碱性的改变具有明显作用,对于大气颗粒物各种组分的清除效果不完全相同。对于大气中OC、NO₃^-、SO₄^2-和NH₄⁺去除率较高,且这4种组分主要以颗粒态形式被冲刷进入降水中,加剧了北京市降水酸化程度。     

Estimation of air pollutant emission loads from construction and operational activities of a port and harbour in Mumbai, India

Port causes environmental and health concerns in coastal cities if its operation and development are not made environmentally compatible and sustainable. An emission inventory is necessary to assess the impact of port projects or growth in marine activity as well as to plan mitigation strategies. In this study, a detailed emission inventory of total suspended particulate (TSP) matter, respirable particulate matter (PM₁₀), sulphur dioxide (SO₂) and oxides of nitrogen (NO_x) for a port having operation and construction activities in parallel is compiled. The study has been done for 1 year. Results show that the maximum contribution of emission of air pollutants in the port area was from TSP (68.5%) and the minimum was from SO₂ (5.3%) to the total pollutants considered in this study. Total TSP emission from all activities of the port was 4,452 tyr^???1 and PM₁₀ emission was 903 tyr^???1 in the year 2006. Re-suspension of dust from paved roads was the major contributor of TSP and PM₁₀ in the road transport sector. Construction activities of the port had contributed 3.9% of TSP and 7.4% of PM₁₀ to total emission of particulate matter. Of the total particulate emissions from various port activities approximately 20% of TSP could be attributed to PM₁₀. The sectoral composition indicates that major contribution of SO₂ emission in the port was from maritime sector and major contribution of NO_x was from road transport sector.