Spatial and Temporal Variability of PM_(2.5) Concentration in China

PM_(2.5) has become an increasing public concern recently because of its visibility reduction and severe health risks. For the whole year of 2013, hourly PM_(2.5) data of 496 monitoring sites scattered in 74 cities of China are collected to analyze temporal and spatial variability of PM_(2.5) concentration. Different temporal scales(seasonal variation, monthly variation and daily variation) and spatial scales(urban versus rural, typical areas and national scale) are discussed. Results show that PM_(2.5) concentration changes significantly in both long-term and short-term scales. An apparent bimodal pattern exists in daily variation of PM_(2.5) concentration and the daytime peak appears around 10:00 am while the lowest concentration appears around 16:00 pm. Spatial autocorrelation analysis and Ordinary Kriging are used to characterize spatial variability. Moran's I of PM_(2.5) concentration in three typical regions, the Beijing-Tianjin-Hebei region, the Yangtze River Delta region and the Pearl River Delta region, is 0.906, 0.693, 0.746, respectively, which indicates that PM_(2.5) is strong spatial correlated. Spatial distribution of annual PM_(2.5) concentration simulated by Ordinary Kriging shows that 7.94 million km2(83%) areas fail in meeting the requirement of China's National Ambient Air Quality Standards Level-2(35 mg/m3) and there are at least three concentrated highly polluted areas across the country.     

Source apportionment for urban PM10 and PM2.5 in the Beijing area

Airborne particulate matter (PM2.5 and PM10) samples were collected at the Beijing Normal University sampling site in the urban area of Beijing, China in dry and wet seasons during 2001―2004. Concen-trations of 23 elements and 14 ions in particulate samples were determined by ICP-AES and IC, re-spectively. Source apportionment results derived from both Positive Matrix Factorization (PMF) and Chemical Mass Balance (CMB) models indicate that the major contributors of PM2.5 and PM10 in Beijing are: soil dust, fossil fuel combustion, vehicle exhausts, secondary particulate, biomass burning and some industrial sources. We have identified both regional common sources, such as vehicular emis-sions, particulate of secondary origin and biomass burning, as well as country-specific problems, such as sand storms and soil dust that should be addressed for effective air quality control.     

燃煤电厂锅炉PM2.5现场实测与排放特征研究

采用自设固定源PM_2.5稀释采集系统对陕西省关中地区多个燃煤电厂烟气中的颗粒物开展了现场实测与样品化学源组分分析。结果表明：4个燃煤电厂PM_2.5、PM₁₀占颗粒物比重差异较大（PM_2.5占比范围为6.92%~54.34%,PM₁₀占比范围为36.36%~73.02%）;4个燃煤电厂数浓度水平最高值（2.0×10⁴~4.0×10⁵个/cm³）差异较大,相差约1个数量级;燃煤电厂PM_2.5小粒径段颗粒物质量浓度占比大多较低,但其对PM_2.5数浓度贡献却很大（最小值>95%）,大粒径段颗粒物则相反;煤粉炉PM₁/PM_2.5较大,占比范围为35.29%~51.35%,循环流化床锅炉PM₁/PM_2.5较小,占比范围为16.62%~21.47%;SO₄^2-是燃煤电厂PM_2.5中最丰富的离子成分,各电厂SO₄^2-占总离子浓度比重范围为50.02~65.52%,Na⁺和Ca²⁺位于第2或第3位;各燃煤电厂主要检出无机元素是Si、Al、Ca、Na、Fe、Na等地壳元素;燃煤电厂PM_2.5、PM₁₀和颗粒物的排放因子范围分别为0.001~0.028 kg/t、0.002~0.086 kg/t、0.003~0.236 kg/t;除尘设施组合越复杂先进,排放因子就可能越小。     

Formation and causes of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> pollution on the east side of the Taihang Mountains in China

Tropospheric column amounts of NO 2 from OMI/Aura products were applied to investigate the seasonal variation of NO x on the east side of the Taihang Mountains (ESTM) in China. The NO 2 concentration varied seasonally, with winter maxima and summer minima. To explore the causes of the heavy NO 2 pollution in this region, wind field simulations were conducted by using the Fifth-Generation NCAR/Penn State Mesoscale Model (MM5). MM5 simulations showed that wind directions in the ESTM region were dominated by northeasterly and northwesterly winds throughout the year and to a lesser degree by southwesterlies. Elevated NO 2 concentrations (higher than 50×10 15 molec/cm 2 ) occurred in three meteorological situations: convergent wind fields (5 days), northeasterly winds (2 days), and calm days (1 day) in January. Although the local anthropogenic NO x emission strength was not so high as that in other developed areas, the calms and frequent occurrence of convergent wind fields, as well as unfavorable terrains for diffusion, resulted in the accumulation of atmospheric pollutants and hence heavy NO x pollution. Furthermore, long-distance NO x transportation from the Beijing-Tianjin-Tangshan region to the ESTM area could be seen when the wind was from a northeasterly direction, especially under high wind speeds.     

长三角典型城市PM2.5浓度变化特征及与气象要素的关系

利用长三角地区4个典型城市南京、上海、杭州、合肥2014年4月1日~2015年3月31日的PM2.5监测数据,以及同期MICAPS地面气象要素的观测资料,对该地区PM2.5浓度的变化规律及其与气象要素的关系进行了分析和讨论。结果表明:长三角地区PM2.5浓度总达标率总体表现为夏季最高,冬季最低的态势。4个城市中,上海全年总达标率最高,杭州其次,合肥最低。上海和杭州达标率月变化特征相近,南京和合肥相近;PM2.5逐小时浓度日变化曲线呈现两峰一谷型分布,最大值均出现在早晨,最小值均出现在下午16~17时之间;月平均浓度具有明显的季节变化特征,冬季最高,夏季最低;PM2.5浓度与风速呈现显著现负相关关系,受地面风向影响明显,污染物在主导风的作用下从上游污染源扩散至下风区域;与气温呈现负相关关系;从全年来看,PM2.5浓度与相对湿度呈现负相关关系,高湿度状态更有利于降水从而增加PM2.5湿清除;各个城市PM2.5浓度与气压相关性很弱,并且未通过显著性检验,可见气压是影响PM2.5浓度变化的次要因素;降水对PM2.5清除作用明显。不同城市PM2.5的变化特征及其受气象要素的影响存在差异,主要是由不同城市的地理环境、产业布局以及污染源等因素造成的。     

Temporal and spatial distribution of tropospheric CO<Subscript>2</Subscript> over China based on satellite observations

Mid-troposphere CO₂ data retrieved by the AIRS (atmospheric infrared sounder) were validated with five ground-based stations and aircraft measurements in the Northern Hemisphere. AIRS CO₂ products show good agreement with ground and aircraft observations. The data had a monthly average accuracy better than 3 ppmv. In this study, the spatial and temporal distribution of mid-troposphere CO₂ from January 2003 to December 2008 was analyzed based on this satellite product. The average concentration of atmospheric CO₂ was higher in the Northern Hemisphere than in the Southern Hemisphere. The yearly average results show a gradual increase from 2003 to 2008. In China, the annual growth rate was about 2 ppmv/a, similar to the United States, Europe, Australia and India, but was slightly lower than Canada and Russia. Mid-troposphere CO₂ concentrations were higher over northern China than over southern areas, due to differences in natural conditions and industrial layout. There were four centers of high CO₂ concentration between 35° and 45°N over China, with low concentrations over Yunnan Province. There was a significant seasonal CO₂ variation with peak concentration in spring and the lowest concentration in autumn.     

南宁市灰霾天气与空气污染物关系分析

根据2010年6月1日至2011年5月31日南宁市的环境监测数据和气象数据,分析南宁市灰霾天气特征,然后通过SPSS软件分析灰霾天气与能见度、颗粒物(PM2.5、PM10)浓度、气态污染物浓度和空气污染指数的关系,探讨南宁市灰霾天气与空气污染物的关系。结果发现,南宁市灰霾天气主要分布在秋、冬两季,PM2.5是直接造成南宁市灰霾天气的主要因子,PM10、SO2、NO2、CO和O3对灰霾天气的发生也有一定影响。PM2.5与PM10相关性最显著,与SO2、NO2相关性较显著,与CO相关性显著,与O3相关性不显著。     

Doping effect on thermoelectric properties of nonstoichiometric AgSbTe<Subscript>2</Subscript> compounds

Nonstoichiometric ternary thermoelectric materials Ag_0.84Sb_1.15M_0.01Te_2.16 (M=Ce, Yb, Cu) were prepared by a direct melt-quench and hot press process. The carrier concentration of all the samples increased after doping. Thermoelectric properties, namely electrical conductivity, Seebeck coefficient, and thermal conductivity, were measured from 300 to 673 K. The phase transition occurring at about 418 K representing the phase transition from β-Ag₂Te to α-Ag₂Te influenced the electrical transport properties. The electrical conductivities of Ce and Yb doped samples increased after doping from 1.9×10⁴ to 2.5×10⁴ and 2.3×10⁴ S·m⁻¹, respectively, at 673 K. Also, at room temperature, the Seebeck coefficient of the Ce doped sample relatively increased corresponding to the high carrier concentration due to the changes in the band structure. However, all the thermal conductivities increased after doping at low temperature. Because of the higher thermal conductivity, the dimensionless figure of merit ZT of these doped samples has not been improved.     

Variability and reduction of atmospheric pollutants in Beijing and its surrounding area during the Beijing 2008 Olympic Games

The Beijing-Tianjin-Hebei Atmospheric Environment Monitoring Network was established by the Institute of Atmospheric Physics, Chinese Academy of Sciences. The goals of the network were to monitor and provide warnings of the atmospheric quality in Beijing and its surrounding area during the Beijing 2008 Olympic Games. The results showed that the atmospheric complex pollution exhibited high concentrations of ozone and fine particles and oxidation in summer, with a ubiquitous regional source. The regional mean concentrations of SO₂, PM_2.5, NO₂, and O_{3_8h max} (the maximum daily 8 h mean) and O_x were 22±11, 90±40, 25±5, 136±35 and 112±21 μg/m³ in summer, respectively. During the Olympic Games, the mean concentration of SO₂, PM_2.5, NO_{2, O3_8h} max, and O_x were 12.5±4, 56±28, 23±4, 114±29, 95±17 μg/m³ in the region, respectively, and fell by 51.0%, 43.7%, 13%, 20.2%, and 18.9%, respectively, compared to the prophase mean before the Olympic Games. The concentration of atmospheric pollutants declined significantly and achieved the “Green Olympics” control goal of air quality. After the Olympic Games, SO₂, PM_2.5 and NO_x increased significantly as the temporary atmospheric pollution control measures were terminated.     

Preparation and upconversion luminescence of YVO<Subscript>4</Subscript>:Er<Subscript>3+</Subscript>, Yb<Subscript>3+</Subscript>

YVO₄:Er³⁺, Yb³⁺ with varying Yb³⁺ concentrations were prepared by a precipitation method. The results of X-ray diffraction (XRD) show that all the samples have a tetragonal zircon structure; the calculated average crystallite sizes are in the range of 14–22 nm. The lattice constants and cell volume of the samples decrease slightly with the increase in Yb³⁺ concentration. The upconversion luminescence spectra of all the samples were studied under 980 nm laser excitation. The strong green emission is observed, which is attributed to the ²H_11/2 → ⁴I_15/2 and ⁴S_3/2→⁴I_15/2 transitions of Er³⁺, and the red emission peaks in 650–675 nm can be ignored. The emission intensity for the sample depends on the Yb³⁺ concentration. These results reveal that the upconversion processes of YVO₄:Er³⁺, Yb³⁺ are related to the structure and the doping Yb³⁺ concentration of the sample.     

Coral reef ecosystems in the South China Sea as a source of atmospheric CO<Subscript>2</Subscript> in summer

Field measurements of air-sea CO2 exchange in three coral reef areas of the South China Sea (i.e. the Yongshu Reef atoll of the Nansha Islands, southern South China Sea (SCS); Yongxing Island of Xisha Islands, north-central SCS; and Luhuitou Fringing Reef in Sanya of Hainan Island, northern SCS) during the summers of 2008 and 2009 revealed that both air and surface seawater partial pressures of CO2 (pCO2) showed regular diurnal cycles. Minimum values occurred in the evening and maximum values in the morning. Air pCO2 in each of the three study areas showed small diurnal variations, while large diurnal variations were ob-served in seawater pCO2. The diurnal variation amplitude of seawater pCO2 was ~70 μmol mol–1 at the Yongshu Reef lagoon, 420–619 μmol mol–1 on the Yongxing Island reef flat, and 264–579 μmol mol–1 on the reef flat of the Luhuitou Fringing Reef, and 324–492 μmol mol–1 in an adjacent area just outside of this fringing reef. With respect to spatial relations, there were large differences in air-sea CO2 flux across the South China Sea (e.g. ~0.4 mmol CO2 m–2 d–1 at Yongshu Reef, ~4.7 mmol CO2 m–2 d–1 at Yongxing Island, and ~9.8 mmol CO2 m–2 d–1 at Luhuitou Fringing Reef). However, these positive values suggest that coral reef ecosystems of the SCS may be a net source of CO2 to the atmosphere. Additional analyses indicated that diurnal variations of surface seawater pCO2 in the shallow water reef flat are controlled mainly by biological metabolic processes, while those of deeper water lagoons and outer reef areas are regulated by both biological metabolism and hydrodynamic factors. Unlike the open ocean, inorganic metabolism plays a significant role in influencing seawater pCO2 variations in coral reef ecosystems.     

南宁市一次严重空气污染期间颗粒污染物特征及气象条件分析

利用南宁市环境保护监测站2010年11月5日至12(污染个案期)在南宁市区振宁花园、市监测点、区农职院、大自然花园4个有代表性的国控环境空气监测点观测到的空气质量数据,分析颗粒污染物PM10和PM2.5的浓度变化及PM2.5的主要化学组分浓度,再利用广西气象服务中心观测的天气数据分析污染个案期的气象条件。结果表明:此次长时间空气污染重,南宁市大气中的颗粒物出现显著升高,颗粒物为此次诱发长时间空气污染物的首要污染因子,颗粒物中的组分以有机质OM和硫酸盐为主;观测时段内气象因素对空气污染存在重要影响,来自湖南方向的污染气团对南宁市的长时间轻微污染也存在一定影响。     

星地结合的细颗粒物超标防控区精确识别方法

为精确识别细颗粒物(PM_(2. 5))浓度超标的区域空间,依据卫星遥感与站点监测在PM_(2. 5)浓度观测方面的特点,建立遥感反演数据与站点监测数据间的临界映射分析法,综合卫星遥感覆盖面广和站点监测准确性高的技术优势。通过该方法研究珠三角区域2013年灰霾污染过程的PM_(2. 5)浓度超标区域,结果表明,利用星地结合的方法可以精确识别出PM_(2. 5)浓度超标的区域空间;广州市西部和南部、佛山市大部、肇庆市主城区及东南部、东莞市西部和北部、中山市北部和中部、江门市主城区及东部是珠三角PM_(2. 5)污染的高发地区,应作为防控重点。     

基于PCA-OS-ELM的大气PM2.5浓度预测

为了提高细颗粒物PM_2.5浓度预测精度,提出一种主元成分分析与在线序列极限学习机相结合（PCA-OS-ELM）的PM_2.5浓度预测方法. 首先,通过主成分分析方法（PCA）提取高维大气数据中影响空气质量的关键变量,并去除不必要的冗余变量;其次,利用提取的关键变量建立在线序列极限学习机（OS-ELM）网络预测模型,将批处理和逐次迭代相结合,不断更新训练数据和网络参数实现大气PM_2.5浓度快速预测.研究结果表明,PCA-OS-ELM预测方法采用不同批次训练数据更新模型的方式,能够快速实现大气PM_2.5浓度预测,证明了该方法的有效性.与其他方法相比,该方法预测误差小,预测精度高,具有更好的实用价值.      

石家庄市冬春季环境空气中挥发性有机物的污染特征

为了深入探究石家庄市冬春季环境空气中挥发性有机物的污染特征,采用EPA TO-15方法定性定量分析了石家庄市冬春季环境空气中62种挥发性有机物的污染特征,对比了环境空气中VOCs浓度的季度、月度变化情况,以及VOCs与PM2.5浓度之间的相关性,分析了环境空气中主要VOCs组分的来源。结果表明:在石家庄市冬春季环境空气中定量检测到其中的40种VOCs,主要有丙酮、苯、四氯化碳、二氯甲烷、甲苯、乙酸乙酯等;未定量的组分中,检测出了较高的乙酸丁酯、丁烷、乙醇等。在雾霾天气,PM2.5浓度和环境空气中VOCs浓度具有较好的正相关性。     

复杂山地环境下气候要素的空间插值方法比较研究

复杂山地环境下气候要素的空间插值长期以来是地理科学研究的一大热点和难点问题.该文以中国康滇区为研究区域,以康滇区基准气象站点的分布图和1 km精度的数字高程模型为实验数据,借助传统的普通克里格法和反距离加权法以及将海拔高程引为变量的薄板光顺样条插值方法,对多年月平均温度和降水量进行空间插值方法的比较研究.结果表明,康滇区温度的空间分布呈现出明显的地带差异,而降水量的空间分布没有明显的地带差异;均方根误差等统计指标评价薄板光顺样条插值方法的插值精度最高.与普通克里格法和反距离加权法相比,薄板光顺样条插值方法更适宜用于复杂山地环境下气候要素的空间插值.     

Characterization of PM2.5/PM2.5-10 and source tracking in the juncture belt between urban and rural areas of Beijing

Coarse （PM2.5-10） and fine （PM2.5） atmospheric particulate samples were collected in summer and winter during 2005-2007 in the juncture belt between urban and rural areas of Beijing. Elements, ions, organic/elemental carbon （OC/EC） and polynuclear aromatic hydrocarbons （PAHs） were determined to obtain some latest information about the particulate pollution in the juncture belt of Beijing. Particulate matter levels at this site were high as compared with the levels at other sampling sites in Beijing. Pollution elements, secondary ions and PAHs were enriched in fine particles rather than in coarse particles. An obvious seasonal variation of the chemical composition of PM was observed. Source apportionment results showed that secondary components were the largest mass contributor of PM2.5, accounting for 28%; whereas soil-related sources were the largest contributor of PM2.5-10, explaining about 49% of the total mass. The abnormal levels of soil heavy metals at the electronic waste disassembly site in the upwind villages suggested the potential impact of such activities to the environment.     

黄河三角洲土壤表观电导率空间变异稳健性分析

针对目前黄河三角洲地区存在的土壤盐渍障碍问题,结合电磁感应仪EM38移动测定系统的田间测量,对表征该地区土壤盐分的土壤表观电导率进行了空间变异特征分析,研究了变异函数随样点数量变化的稳健性,并探讨了Kriging插值精度与样点数量之间的关系.结果表明,土壤表观电导率的变异函数表现出多层次叠加的尺度效应,其变异函数较好地符合球状套合模型,短程变异是构成空间异质性的最主要部分.变异函数对样点比例的减少总体不敏感,当样点比例低于lO%,变异函数开始发生形变.Kriging插值精度与空间相似性均随样点比例降低呈下降趋势,当样点比例在20%-80%时,Kriging插值精度对样点比例的降低不敏感;在保证得到稳健的变异函数图的前提下,样点比例降至30%,基本不会损失Kriging插值得到的空间分布信息.     

Comparative analysis of the dissolution kinetics of galena in binary solutions of HCl/FeCl<Subscript>3</Subscript> and HCl/H<Subscript>2</Subscript>O<Subscript>2</Subscript>

A comparative study of the dissolution kinetics of galena ore in binary solutions of FeCl₃/HCl and H₂O₂/HCl has been undertaken. The dissolution kinetics of the galena was found to depend on leachant concentration, reaction temperature, stirring speed, solid-to-liquid ratio, and particle diameter. The dissolution rate of galena ore increases with the increase of leachant concentration, reaction temperature, and stirring speed, while it decreases with the increase of solid-to-liquid ratio and particle diameter. The activation energy (E _a) of 26.5 kJ/mol was obtained for galena ore dissolution in 0.3 M FeCl₃/8.06 M HCl, and it suggests the surface diffusion model for the leaching reaction, while the E _a value of 40.6 kJ/mol was obtained for its dissolution in 8.06 M H₂O₂/8.06 M HCl, which suggests the surface chemical reaction model for the leaching reaction. Furthermore, the linear relationship between rate constants and the reciprocal of particle radius supports the fact that dissolution is controlled by the surface reaction in the two cases. Finally, the rate of reaction based on the reaction-controlled process has been described by a semiempirical mathematical model. The Arrhenius and reaction constants of 11.023 s⁻¹, 1.25×10⁴ and 3.65×10² s⁻¹, 8.02×10⁶ were calculated for the 0.3 M FeCl₃/8.06 M HCl and 8.06 M H₂O₂/8.06 M HCl binary solutions, respectively.     

Synthesis and characterization of wormhole-like mesoporous Ce0.6Zr0.35Y0.05O2 solid solutions

Nanoparticles of Ce0.6Zr0.35Y0.05O2 (CZY) solid solution have been prepared by the CTAB (hexadecyl-trimethyl ammonium bromide), CTAB-EG (ethylene glycol) templating, and CTAB-EG-NaCl (in which the pores of the precursor synthesized by the CTAB-EG method is filled by a certain amount of NaCl) method, respectively. The physical properties of these materials were characterized by means of tech-niques such as X-ray diffraction (XRD), high resolution scanning electron microscopy (HRSEM), transmission electron microscopy (TEM), selected area electron diffraction (SAED), and N2 adsorp-tion-desorption measurements. The CZY samples synthesized by the above three methods display wormhole-like mesoporous morphology and cubic crystal structures. The materials are narrow in pore size distribution (averaged pore diameter = 5.3―7.1 nm), high in surface areas (95―119 m2/g), and large in pore volumes (0.16―0.18 cm3/g). It has been demonstrated that the introduction of NaCl is capable of retaining the pore structures of solid nanomaterials at high-temperature calcination.