Characterization of airborne trace metal and trace organic species from coal gasification

Fugitive emissions from a slagging fixed-bed coal-gasification pilot plant were analyzed by flameless atomic absorption spectrophotometry, gas chromatography, and mass spectrometry for trace metal and trace organic species. Analysis of the size distributions of airborne particulate matter inside the plant showed an abundance of large metal-containing particles; outdoor distributions in the vicinity of the plant resembled the indoor distributions, suggesting the importance of the gasifier in influencing ambient air quality. This conclusion was further supported by identification of similar organic compounds inside and outside the plant. Trace element enrichment factors based on the earth's crustal composition were greater than those based on the composition of the lignite used in the gasifier, showing the importance of characterizing the proper source material when inverstigating chemical fraction during aerosol formation. Enrichments in the present study were much greater than those found in previous sampling during aborted start-up and cleaning procedures, where normal operating temperatures had not yet been reached. Both studies showed evidence of enrichment factors which decreased with increasing particle size. Although much of the airborne mass was associated with large particles having low respirability, the high concentrations of some metals indoors suggests that further assessment of potential occupational exposures is warranted.     

西安城北地区秋季PM_(2.5)中的矿尘颗粒污染特征

采用单颗粒气溶胶飞行时间质谱仪(Single Particle Aerosol Mass Spectrometer,SPAMS)对西安市大气矿尘颗粒物进行连续12 d在线分析,共采集到107 425个同时含有正负质谱信息的矿尘颗粒,矿尘颗粒物占PM_(2.5)样本数的8.44%。结果表明,矿尘颗粒物的正离子碎片成分以Na~+、K~+、Al~+、Ca~+、CaO~+、Fe~+为主,同时还含有Pb~+等,负离子碎片成分以NO~-_2和NO~-_3为主,另外还含有HSO~-_4、SiO~-_3、HSiO~-_3、H(NO_3)~-_2等。在西安市大气细颗粒物中,矿尘颗粒物中贡献较大的几类(如含钙、含铁、铁氧颗粒物等)大多是老化的成分。将观测阶段采集到的矿尘颗粒纳入本地污染源谱进行来源分析,其主要来源为扬尘源、工业源、燃煤源和汽车尾气源等。     

利用大气超级站对乌鲁木齐市一次沙尘天气过程及组份的分析

本研究利用大气超级站对乌鲁木齐市4月9日至10日沙尘天气过程,粒径谱、离子和重金属组成及变化进行分析。研究结果表明激光雷达观测结果与环境空气质量监测基本一致;小粒径颗粒在沙尘和非沙尘时段含量最多,但在沙尘时段大粒径颗粒的增长幅度远大于小粒径;沙尘过程中的离子主要来源于土壤一次源;沙尘过程中地壳元素浓度及占比均显著升高,会稀释环境空气中人为污染元素。     

Statistical methods to apportion the sources of particles in the industrial region of Estarreja—Portugal

Factor analysis models are very attractive for source apportionment and have been widely applied. They do not require a priori knowledge of the number and composition of the sources, and they can actually uncover previously unsuspected sources and estimate the composition of the sources using only ambient monitoring data.Aerosol particles were collected from an industrial atmosphere and analyses for water soluble and carbon components. Principal components analysis permitted the evaluation of the contribution due to industries, soil fraction, secondary pollutants and sea spray particles of the total suspended aerosol mass.It can be concluded that the atmospheric aerosol in the Industrial Area of Estarreja (Portugal) contains a relative important fraction that is water soluble. Ammonium sulphates and nitrates are the main components of this fraction. Carbon compounds constitute about 30% of the total aerosol mass. These compounds are mainly formed by organic matter emitted by the industries. Due to the mutagenic and carcinogenic characteristics of some organic compounds processed in the Industrial Area (vinyl chloride, benzene, aniline, etc.), the concern exists of negative human health effects as a result of prolonged inhalation. Soil compounds is another important fraction of the aerosol mass, mainly in summer with dry, sunny and windy weather conditions.A more conclusive idea of the sources and effects of aerosol matter can only be obtained with the specific analysis of organic compounds and the determination of trace elements, characteristic of each particular source.     

Submicron particle characteristics of atmospheres in a long highway tunnel

This study used a scanning mobility particle sizer (SMPS) to measure and categorize submicron atmospheric particles in the 14–737-nm size range for ambient and urban roadside air and for air in the Hsuehshan Tunnel (12.9 km), Taiwan. Principal component analysis, traffic flow, and particle size distributions were used to identify the emission characteristics of light-duty vehicles (LDV) with the SMPS data. In the Hsuehshan Tunnel, the particle size from the majority of emissions discharged by LDV is approximately 20–60 nm, and the maximum particle number can reach up to 2.5?×?10⁵. In contrast, submicron particle size distribution for urban roadsides is mostly 14–200 nm, and the maximum particle number is approximately 4?×?10⁴ with the particle number for most particle sizes being below 1,200. The submicron particle size distribution at the ambient air station was unimodal with a mode sizes at 30–50 nm with the maximum particle number of 3,000.     

Characterization of mineral particles in winter fog of Beijing analyzed by TEM and SEM

Aerosol samples were collected during winter fog and nonfog episodes in Beijing. Transmission electron microscopy (TEM) and scanning electron microscopy (SEM) were applied to study morphologies, sizes, and compositions of aerosol particles. TEM observation indicates that most mineral particles collected in fog episode are scavenged in fog droplets. Number–size distributions of mineral particles collected in fog and nonfog episodes show two main peaks at the ranges of 0.1–0.3 and 1–2.5 μm, respectively. Based on their major compositions, mineral particles mainly include Si-rich, Ca-rich, and S-rich. Average S/Ca ratio of mineral particles collected in fog episode is 6.11, being eight times higher than that in nonfog episodes. Development mechanism of individual mineral particles in fog droplets is proposed. It is suggested that mineral particles with abundant alkaline components (e.g., “Ca-rich” particles) occurred in air should alleviate acidic degree of fog and contribute to complexity of fog droplets in Beijing.     

Elemental and individual particle analysis of atmospheric aerosols from high Himalayas

Atmospheric aerosols were collected during the scientific expedition to Mt. Qomolangma (Everest) in May–June, 2005. The elemental concentrations of the aerosols were determined by inductively coupled plasma mass spectrometry. This yielded data for the concentration of 14 elements: Na, Mg, Al, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, and Pb. The mean elemental concentrations were generally comparable with those from central Asia and the Arctic, while much higher than those from Antarctic. Size, morphology, and chemical composition of 900 individual aerosol particles were determined by scanning electron microscopy and energy-dispersive X-ray microanalysis. Based on morphology and elemental composition, the particles were clustered into eight groups: soot (8%), tar ball (3%), alumosilicates/silica (55%), calcium sulfate (16%), Ca/Mg carbonate (2%), Fe/Ti-rich particles (3%), Pb-rich particles (1%), and biological particles (12%). The sampling site, located at 6,520 m in the Himalayas, is particularly remote and located at high altitude. Nonetheless, high aerosol enrichment factors for copper, chromium, lead, nickel, vanadium, and zinc all suggest the influence of long-range transported pollution, while enrichment in calcium and the presence of alumino-silicates in individual particle analyses indicates a distinct mineral dust influence. The backward air mass trajectories showed that the northwestern part of India may contribute to the atmospheric aerosol in the central high Himalayas.     

Study on Size Distribution of Total Aerosol and Water-Soluble Ions During an Asian Dust Storm Event at Jeju Island, Korea

Soil dust particles transported from loess regions of the Asian continent, called Asian dust, highly influences the air quality of north-eastern Asia and the northern Pacific Ocean. In order to investigate the effects of these dust storms on the chemical composition of atmospheric aerosol particles with different size, measurements of size distributions of total aerosol and major ion species were carried out on Jeju Island, Korea during April 2001. Juju Island was chosen for the study because the levels of emissions of anthropogenic air pollutants are very low. A 5-stage cascade impactor was used to sample size-fractionated aerosol particles. Samples were analyzed for major water-soluble ions using Dionex DX-120 ion chromatograph. The average mass concentration of total aerosol was found to be 24.4 and 108.3 microg m(-3) for non-Asian dust and Asian dust periods, respectively. The total aerosol size distribution, measured during the non-Asian dust period, was bimodal, whereas the coarse particles dominated the size distribution of total aerosol during the Asian dust period. It was found that SO4(2-), NH4+ and K+ were mainly distributed in fine particles, while Cl-, NO3-, Na+, Mg2+ and Ca2+ were in coarse particles. Although SO4(2-) was mainly distributed in fine particles, during the Asian dust period, the concentrations in coarse particles were significantly increased. This indicates heterogeneous oxidation of SO2 on wet surfaces of basic soil dust particles. The NH4+ was found to exist as (NH4)2SO4 in fine particles, with a molar ratio of NH4+ to SO4(2-) of 2.37 and 1.52 for non-Asian dust and Asian dust periods, respectively. Taking into account the proximity of the sampling site to the sea, and the observed chloride depletion, coarse mode nitrate, during the non-Asian dust period, is assumed to originate from the reaction of nitric acid with sodium chloride on the surfaces of sea-salt particles although the chloride depletion was not shown to be large enough to prove this assumption. During the Asian dust period, however, chloride depletion was much smaller, indicating coarse nitrate particles were mainly produced by the reaction of nitric acid with surfaces of basic soil particles. Most chloride and sodium components were shown to originate from sea-salt particles. Asian dust aerosols, arriving at Jeju Island, contained considerable amounts of sea-salt particles as they passed over the Yellow Sea. Ca2+ was shown to be the most abundant species in Asian dust particles.     

渤海大气气溶胶元素组成及物源分析

利用电感耦合等离子体-光发射光谱法(ICP-OES)分析了2000年夏季渤海大气气溶胶样品,给出了渤海气溶胶污染物浓度分布特点,结合气象资料和富集因子进行了元素物源分析.分析结果表明,辽东湾的污染程度高于其他海区,气溶胶中含量最高的元素是Zn(1638ng/m3),含量最低的是V(2ng/m3).渤海气溶胶中Pb、Zn、Cu和Ni等具有较高的富集因子.辽东湾Pb的富集因子达4000以上,Zn的富集因子普遍大于其他海区.Pb、Mn、Cu、V等含量的相对大小与同期北京的分析结果一致.综合分析表明,渤海大气严重受到陆地人为排放污染物的影响.     

PM10 in the ambient air of Chandrapur coal mine and its comparison with other environments

This study compares the ambient air particulate matter (PM10) data of 15 different coal mine environments. For most of these mine environments, the monitoring was carried out by different researchers using respirable dust sampler (RDS) that separates PM10 by centrifugal inertial separation. At two sites — Padmapur and Ghugus (Chandrapur, Maharashtra, India) — mass inertial impaction-based sampler was used for PM10 monitoring. It is observed that the spatiotemporal average value of ambient air PM10 monitored using mass inertial impactor reports relatively higher values (240–372 μg/m³) compared to those monitored using RDS (<227 μg/m³). In order to realize the severity of mine area pollution, it is compared with PM10 values found in an urban area (Delhi, India). It is found that PM10 values in Delhi (using mass inertial impactor) are much higher (300–400 μg/m³) than those reported for the mine environment. The data seems to indicate that the mine environment is relatively cleaner than urban air and therefore raises doubt about the appropriateness of using either mass impactor or RDS for PM10 sampling.     

Monitoring of Particle Mass and Number in Urban Air

Measurements of aerosol particles in the air of an urban area in the UK have been made. Ambient air was sampled and the particulates measured after passing through a size selective PM₁₀ inlet. Particle mass was measured using a Tapered Element Oscillating Microbalance (TEOM). Particle number and size distributions were obtained using an Electrical Aerosol Analyser (EAA) and an Aerodynamic Particle Sizer (APS). Measurements were also made of local meteorological parameters. Fine particle number concentrations were found to show better temporal agreement, including diurnal variation, with particle mass concentrations than the coarser particle number concentrations.     

Characterisation of particulate matter on the receptor level in a city environment

Airborne particulate matter (PM) has become one of the dominant pollutants with the increasing material and energy demand due to global economic growth. The main objective of this research is to provide a comprehensive receptor level characterisation of the particulate matter collected in a city environment. Particulate matter samples were collected on Tapered Element Oscillating Microbalance (TEOM) filters from five monitoring sites over a period of 1 year. An Andersen eight-stage cascade impactor was also used to collect airborne PM samples from three other locations to compare with the samples collected by TEOM. All the samples were then subjected to individual particle morphology and chemical composition analysis by SEM/EDS. Bulk chemical composition of the samples were also analysed through ICP–OES. Based on these analyses, possible sources of the PM samples were identified. The results showed that the monitoring sites in residential environments were dominated by transportation-derived particles and other migratory particulates. Monitoring sites near the city centre were dominant by particles from transportation, with biological particles abundant for the site closer to a river. The monitoring station located close to the industrial area, despite only 200 m away from a motorway, has low contribution of non-exhaust particulates from vehicles. Instead, the particulates collected from this site were dominated by industrial sources. An air dispersion modelling package was also used to model the particulate matter dispersion in the city area for the period of sampling. The results from the model showed that the points of high emissions were around industrial areas.     

Correlations in the chemical composition of rural background atmospheric aerosol in the UK determined in real time using time-of-flight mass spectrometry

An aerosol time-of-flight mass spectrometer (ATOFMS) was used to determine, in real time, the size and chemical composition of individual particles in the atmosphere at the remote inland site of Eskdalemuir, Scotland. A total of 51,980 particles, in the size range 0.3-7.4 microm, were detected between the 25th and 30th June 2001. Rapid changes in the number density, size and chemical composition of the atmospheric aerosol were observed. These changes are attributed to two distinct types of air mass; a polluted air mass that had passed over the British mainland before reaching Eskdalemuir, interposed between two cleaner air masses that had arrived directly from the sea. Such changes in the background aerosol could clearly be very important to studies of urban aerosols and attempts at source apportionment. The results of an objective method of data analysis are presented. Correlations were sought between the occurrence of: lithium, potassium, rubidium, caesium, beryllium, strontium, barium, ammonium, amines, nitrate, nitrite, boron, mercury, sulfate, phosphate, fluorine, chlorine, bromine, iodine and carbon (both elemental and organic hydrocarbon) in both fine (d < 2.5 microm) and coarse (d > 2.5 microm) particle fractions. Several previously unreported correlations were observed, for instance between the elements lithium, beryllium and boron. The results suggest that about 2 in 3 of all fine particles (by number rather than by mass), and 1 in 2 of all coarse particles containing carbon, consisted of elemental carbon rather than organic hydrocarbon (although a bias in the sensitivity of the ATOFMS could have affected these numbers). The ratio of the number of coarse particles containing nitrate anions to the number of particles containing chloride anions exceeded unity when the air mass had travelled over the British mainland. The analysis also illustrates that an air mass of marine origin that had travelled slowly over agricultural land can accumulate amines and ammonium.     

Characterization of physicochemical properties of beryllium aerosols associated with prevalence of chronic beryllium disease

Little is known about the physicochemical properties of beryllium aerosols associated with increased risk of beryllium sensitization and chronic beryllium disease (CBD). Such information is needed to evaluate whether airborne mass of beryllium is the appropriate metric of exposure or alternatively to provide a scientific basis for using information on particle size, surface area, and chemistry to support an improved exposure limit based on bioavailability through the inhalation and dermal routes of exposure. Thus, we used a suite of analytical techniques to characterize aerodynamically size-fractionated beryllium particles and powders that have been associated in epidemiological studies with higher prevalence of CBD. Aerosol particles were sampled from the ventilation systems of production lines for powders of beryllium metal and beryllium oxide and for ingots of copper-beryllium alloy. End product powders from the metal and oxide production lines were also collected.Particles released during production of beryllium metal were found to be complex, having heterogeneous composition, including reactive species such as fluorine. Powders from beryllium metal production were of high purity with only a minor component of beryllium oxide. Both particles and powders from oxide production were high-purity oxide. Particles released during production of copper-beryllium alloy were heterogeneous, being predominantly copper oxides. Thus, all particles and powders contain at least some beryllium in the form of beryllium oxide.These data justify efforts to thoroughly characterize beryllium aerosol properties when performing exposure assessments. The data also suggest that differences in particle chemical composition, size, number, and surface area may influence bioavailability of beryllium and contribute to risk of CBD. However, a scientific basis does not yet exist to replace mass as the current metric of exposure.     

杭州市大气PM2.5和PM10污染特征及来源解析

2006年在杭州市两个环境受体点位采集不同季节大气中PM_2.5和PM₁₀样品,同时采集了多种颗粒物源类样品,分析了其质量浓度和多种化学成分,包括21种无机元素、5种无机水溶性离子以及有机碳和元素碳等,并据此构建了杭州市PM_2.5和PM₁₀的源与受体化学成分谱;用化学质量平衡(CMB)受体模型解析其来源。结果表明,杭州市PM_2.5和PM₁₀污染较严重,其年均浓度分别为77.5μg/m³和111.0μg/m³;各主要源类对PM_2.5的贡献率依次为机动车尾气尘21.6%、硫酸盐18.8%、煤烟尘16.7%、燃油尘10.2%、硝酸盐9.9%、土壤尘8.2%、建筑水泥尘4.0%、海盐粒子1.5%。各主要源类对PM₁₀贡献率依次为土壤尘17.0%、机动车尾气尘16.9%、硫酸盐14.3%、煤烟尘13.9%、硝酸盐粒8.2%、建筑水泥尘8.0%、燃油尘5.5%、海盐粒子3.4%、冶金尘3.2%。     

Field measurement of lead in workplace air and paint chip samples by ultrasonic extraction and portable anodic stripping voltammetry

On-site measurement of lead in workplace air filter samples and paint chip samples by ultrasonic extraction and anodic stripping voltammetry (UE-ASV) was evaluated in the field during renovation and remodeling activities in residences having leaded paint. Aerosol and paint samples were collected using standard techniques, and the samples were analyzed on-site for lead content by portable UE-ASV. Lead in sample extracts was subsequently determined by atomic absorption (AA) spectrometry in a fixed-site laboratory. The remaining sample extracts plus undissolved material (air filters or paint particles) were then subjected to hot plate digestion in concentrated nitric acid-30% hydrogen peroxide prior to AA analysis for lead. Field UE-ASV lead data were thereby compared to UE-AA and hot plate digestion-AA results from fixed-site laboratory lead measurement. Determination of lead in air filter samples by UE-ASV (over the range of 5 microg to approximately 800 microg Pb per sample) was extremely well correlated with lead measurement by UE-AA and hot plate digestion-AA procedures. However, a significant negative bias associated with ASV measurement was observed, and this was attributed to a matrix effect. Lead measurement in paint chip samples by UE-ASV (over the range of approximately 10 to approximately 550 microg Pb g(-1)) was well correlated with lead measurement by UE-AA and hot plate digestion-AA procedures. However, correlation and precision were lower for lead measurement in paint samples as compared to aerosol samples, and a negative bias was also observed. Lead measurements by UE-AA were compared to lead determinations by hot plate digestion-AA; these data were highly correlated and demonstrated no significant bias. Thus it was concluded that the ultrasonic extraction procedure performed equivalently to hot plate digestion. It was reasoned that matrix effects due to the preparation and analysis of paint chip particles resulted in greater imprecision as well as negative bias by ASV measurement. Despite significant negative bias in this sample set, UE-ASV offers promise for on-site measurement of lead in samples of interest in occupational and environmental health.     

Characteristics of Hazardous Airborne Dust Around an Indian Surface Coal Mining Area

Surface coal mining creates more air pollution problems with respect to dust than underground mining . An investigation was conducted to evaluate the characteristics of the airborne dust created by surface coal mining in the Jharia Coalfield. Work zone air quality monitoring was conducted at six locations, and ambient air quality monitoring was conducted at five locations, for a period of 1 year. Total suspended particulate matter (TSP) concentration was found to be as high as 3,723 μg/m³, respirable particulate matter (PM10) 780 μg/m³, and benzene soluble matter was up to 32% in TSP in work zone air. In ambient air, the average maximum level of TSP was 837 μg/m³, PM10 170 μg/m³ and benzene soluble matter was up to 30%. Particle size analysis of TSP revealed that they were more respirable in nature and the median diameter was around 20 μm. Work zone air was found to have higher levels of TSP, PM10 and benzene soluble materials than ambient air. Variations in weight percentages for different size particles are discussed on the basis of mining activities. Anionic concentration in TSP was also determined. This paper concludes that more stringent air quality standards should be adopted for coal mining areas and due consideration should be given on particle size distribution of the air-borne dust while designing control equipment.     

Workplace aerosol mass concentration measurement using optical particle counters

Direct-reading aerosol measurement usually uses the optical properties of airborne particles to detect and measure particle concentration. In the case of occupational hygiene, mass concentration measurement is often required. Two aerosol monitoring methods are based on the principle of light scattering: optical particle counting (OPC) and photometry. The former analyses the light scattered by a single particle, the latter by a cloud of particles. Both methods need calibration to transform the quantity of scattered light detected into particle concentration. Photometers are simpler to use and can be directly calibrated to measure mass concentration. However, their response varies not only with aerosol concentration but also with particle size distribution, which frequently contributes to biased measurement. Optical particle counters directly measure the particle number concentration and particle size that allows assessment of the particle mass provided the particles are spherical and of known density. An integrating algorithm is used to calculate the mass concentration of any conventional health-related aerosol fraction. The concentrations calculated thus have been compared with simultaneous measurements by conventional gravimetric sampling to check the possibility of field OPC calibration with real workplace aerosols with a view to further monitoring particle mass concentration. Aerosol concentrations were measured in the food industry using the OPC GRIMM? 1.108 and the CIP 10-Inhalable and CIP 10-Respirable (ARELCO?) aerosol samplers while meat sausages were being brushed and coated with calcium carbonate. Previously, the original OPC inlet had been adapted to sample inhalable aerosol. A mixed aerosol of calcium carbonate and fungi spores was present in the workplace. The OPC particle-size distribution and an estimated average particle density of both aerosol components were used to calculate the mass concentration. The inhalable and respirable aerosol fractions calculated from the OPC data are closely correlated with the results of the particle size-selective sampling using the CIP 10. Furthermore, the OPC data allow calculation of the thoracic fraction of workplace aerosol (not measured by sampling), which is interesting in the presence of allergenic particles like fungi spores. The results also show that the modified COP inlet adequately samples inhalable aerosol in the range of workplace particle-size distribution.     

Characterization of atmospheric aerosols in the city of S?o Paulo, Brazil: comparisons between polluted and unpolluted periods

The objective of this study was to determine the size and composition of atmospheric aerosols in the downtown area of the city of S?o Paulo, Brazil, for a polluted and an unpolluted period. Aerosols were sampled with a portable air sampler (PAS), Micro-Orifice Uniform Deposit Impactor (MOUDI), and Scanning Mobility Particle Sizer. At the study site, air quality is poor, especially during the winter, high concentrations of pollutants being emitted primarily by the light- and heavy-duty vehicle fleet. We analyzed mass, black carbon (BC), Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Rb, Sn, Zr, and Pb. During the polluted period, diurnal PM₁₀ was higher than nocturnal PM₁₀, whereas the inverse was true during the unpolluted period. The FPM was rich in BC, S, and Pb, whereas CPM was rich in Al, Si, Ca, Ti, and Fe. Mass balance was performed by category: ammonium sulfate, sodium chloride, crustal material, BC, and other. The PAS-determined FPM was mainly BC. The MOUDI-determined FPM crustal material explained more mass than did ammonium sulfate and BC during the polluted period, whereas ammonium sulfate had the largest mass during the unpolluted period. Crustal material was the major CPM component, followed by ammonium sulfate and BC. During the unpolluted period, FPM concentrations were lower, whereas those of ammonium sulfate were relatively higher, especially at night, and particle number was inversely proportional to particle size. Aerosol growth was more intense during the polluted period.     

区域大气细颗粒物化学组分及来源年变化趋势

利用单颗粒气溶胶质谱仪(SPAMS)于2018年1月1日—2019年12月31日对上海市浦东新区环境空气PM_2.5开展高时间分辨化学成分监测。结果表明，2019年监测点空气质量总体优于2018年，AQI达标率由74.8%升高至86.6%。通过对PM_2.5成分分类，最终确定了8类颗粒物，相较于2018年，2019年富钾颗粒物升幅较为明显，左旋葡聚糖、重金属和元素碳有小幅增加，其余各组分相对减少。对PM_2.5排放源分类分析显示，机动车尾气源占比>25%，其中2018年3月、2018年7月、2019年2和3月贡献超过40%；二次无机源和燃煤源呈现一定的季节变化特点，整体秋冬季高于春夏季，2019年燃煤源占比较2018年下降了41%；工业排放源2018年5和10月、2019年1和5月占比相对较高，其余各月份占比相对较为稳定。