Analysis of carbon isotopes in airborne carbonate and implications for aeolian sources

Methods were developed to determine the mass ratios of carbon isotopes in trace amounts of aerosol carbonate. A Finnigan MAT 252 mass spectrometer fitted with an on-line Kiel device was to determine the ^13C/^12C ratio in CO2 produced from the carbonate. A study using these methods was conducted to characterize the carbonate carbon isotopes in aerosol samples collected in Xi‘an on dusty and normal days during March and April 2002. Results of the study demonstrate that insights into the origin of the dust can be deduced from its isotopic composition. That is, the δ^13C ofcarbonate for dust storm samples ranged from -1.4‰ to -4.2‰, and this is consistent with sandy materials in dust source regions upwind. In contrast, for non-dusty days δ^13C ranged from -7.5% to -9.3‰, which is more similar to fine particles emitted from local surface soils. Comparisons of dust storm aerosols with surface soils from source regions and with aerosol samples collected downwind indicate that the δ^13C values did not change appreciably during longrange transport. Therefore, carbon isotopes have the potential for distinguishing among source materials, and this approach provides a powerful new tool for identifying dust provenance.     

The compositions, sources, and size distribution of the dust storm from China in spring of 2000 and its impact on the global environment

The average mass concentration of the aerosols in Beijing during the dust storm in the spring of 2000 was ~6000 mg·m^-3, ~30 times as high as that in the non-dust storm days. The enrichment factors of the pollution elements As, Sb and Se were higher than those in the non-dust storm days. This indicated that As, Sb and Se resulted from the pollution sources of those areas, through which the dust storm passed during their long-range transport, in addition to the local pollution sources in Beijing. The enrichment factors of the Pb, Zn, Cd and Cu were much less than those in the non-dust storm days, suggesting that the local pollution sources in Beijing area contributed to them mostly. The enrichment factors of elements Al, Fe, Sc, Mn, Na, Ni, Cr, V and Co were close to 1, showing that these elements originated from crust. The concentration of S in the dust storm was ~10 mg·m^-3, 4 times as high as that in non-dust storm. S in the aerosols resulted from the adsorption of gaseous SO₂ and the consequent transformation on it. The aerosols of the dust storm contained 16.1% and 76.9% of fine particles with the sizes less than 2.1 and 9.0 mm, respectively, while it had a large number of coarse particles. It was noted that a considerable portion of Fe(Ⅱ) was detected from the dust storm. Fe(Ⅱ) could easily dissolve in seawater to be nutrient for phytoplankton and would lead to the increase of the emission of dimethylsulfide (DMS) from the ocean. The feedbacks of Fe coupled with S in atmosphere might be the important mechanism that would affect the primary productivity in Pacific and/or the global climate change.     

Coupling and feedback between iron and sulphur in air-sea exchange

Iron in surface seawater has been demonstrated to be the limiting nutrient factor for primary productivity in certain oceanic regions where other major nutrients are abundant[1—5]. The available Fe to the phytoplankton in seawater is related to the uptake of carbon dioxide through the ocean and, in turn, to the global greenhouse effect[6—11]. Recent reports showed that the available Fe in the seawater is closely correlative to nitrogen fixation in the ocean[12—17]. Understanding which Fe s…     

Comparison of Aerosol Optical Properties over the Semi-arid Region of Loess Plateau between Dusty and Non-dusty Periods in Winter and Spring

Some field experiments of aerosols had been carried out over the arid and semi-arid regions in China over the past 30 years,but there were little learning of the semi- arid region of Loess Plateau. Using Version 2.0 Level 2.0 dataset from the AERONET (Aerosol Robotic Network) Lanzhon_city site,the aerosol optical properties during dusty and non-dusty periods in winter and sprig when air pollrtion frequently occured most frequently were demonstrated. A comparison of the same parameters between Lanzhou and Beijing for spring was also analyzed. Some new information was gained concerning aerosol optical properties over the semi-arid region of Loess Plateau. The results show that the aerosol properties measured during dusty and non-dusty periods are significantly different at Lanzhon,particularly in spring,and also different from those at Beijing.     

<Emphasis Type="Italic">In situ</Emphasis> measurement of PM<Subscript>1</Subscript> organic aerosol in Beijing winter using a high-resolution aerosol mass spectrometer

Organic aerosol (OA) is a crucial component of atmospheric fine particles. To achieve a better understanding of the chemical characteristics and sources of OA in Beijing, the size-resolved chemical composition of submicron aerosols were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer in the winter of 2010, with a high time resolution of 5 min. During this study, the mean OA mass concentration was 20.9±25.3 μg/m3, varying between 1.9 and 284.6 μg/m3. Elemental analysis showed that the average H/C, O/C and N/C (molar ratio) were 1.70, 0.17, and 0.005, respectively, corresponding to an OM/OC ratio (mass ratio of organic matter to organic carbon) of 1.37. The average mass-based size distributions of OA present a promi- nent accumulation mode peaking at approximately 450 nm. The prominent presence of ultrafine particles (Dva < 100 nm) was mainly from the fresh emissions of combustion sources. A Positive Matrix Factorisation (PMF) analysis of the organic mass spectral dataset differentiated the OA into three components, including hydrocarbon-like (HOA), cooking-related (COA), and oxygenated (OOA) organic aerosols, which, on average, accounted for 26.9%, 49.7% and 23.4%, respectively, of the total organic mass. The HOA and COA likely corresponded to primary organic aerosol (POA) associated with combustion-related and cooking emissions, respectively, and the OOA components corresponded to aged secondary organic aerosol (SOA).     

Inorganic chemical composition and source signature of PM2.5 in Beijing during ACE-Asia period

Aerosol samples for PM2.5 were collected in Beijing for 38 consecutive days from March to April 2001 using an IMPROVE Sampler. Concentrations of 20 elements in PM2.5 were determined using a PIXE method. Results show that the average mineral dust concentration of PM2.5 was 14.6 Ilg/m3 during the observation period. On the sand-dust event days of March 21 and April 10, dust PM2.5 mass concentrations were 62.4 and 54.1 μg/m^3, respectively.These demonstrate that fine particle pollution by dust event in Beijing was very severe. The enrichment factors of S and Cu reached minimums on the dusty days and were high on the non-dusty days. It is considered that enrichment factors of elements in PM2.5, which are associated with human activities, can probably provide an effective method to distinguish local sources from external sources of dust. Factor analysis on the chemical composition in PM2.5 shows that sources of crustal matters, anthropogenic emission, and oil combustion contributed to PM2.5 levels in air in the springtime of 2001 in Beijing.     

Speciation of the elements and compositions on the surfaces of dust storm particles： The evidence for the coupling of iron with sulfur in aerosol during the long-range transport

The speciation of the elements on the surface of the particles collected during dust storm and non-dust storm in Beijing and Inner Mongolia was studied by XPS. The major species of iron on the surface were oxides, sulfate, silicate,FeOOH and minor part sorbed on SiO2/Al2O3. Sulfate is the dominant species of sulfur on the surface. SiO2 and Al2O3 are the main components of Si and Al on the surface respectively.One of the most important findings was that the Fe(Ⅱ) (FeS and FeSO4) produced could account for up to 44.3% and 45.6% of the total Fe on the surface in the aerosol sample collected at that night and next day of the “peak” time of the dust storm occurring on March 20, 2002, while Fe2(SO4)3,one of the Fe(Ⅲ) species on the surface decreased from 67.1% to 49.5% and 48.0% respectively. Both S and Fe enriched on the surface of aerosol particles. Fe(Ⅱ) accounted for 1.3%-5.3% of total Fe in bulk aerosol samples during dust storm. These results provided strong evidence to support the hypothesis of the coupling between iron and sulfur in aerosols during the long-range transport, which would have important impact on the global biogeochemical cycle.     

Characteristics and sources of 2002 super dust storm in Beijing

~~Characteristics and sources of 2002 super dust storm in Beijing~~     

Radiative forcing due to dust aerosol over east Asia-north Pacific region during spring, 2001

Atmosphericaerosolsinfluencetheradiationbudgetoftheatmosphere-terrestrialsystem,andthereforeinflu-encetheclimate.Dustaerosolisconsideredtobeacriticalfactortoclimateforcingamongotherkindsofaerosols,whichaccountsfor30percentofaerosolloadingandop-ticaldepth[1].Therearelargeuncertaintiesinthequantita-tiveassessmentsoftheradiativeeffectofdustatthepre-sentday,involvingvariousfactors:refractiveindices,par-ticlesizedistribution,atmosphericaerosolloading,parti-cleshape,etc.[2].Dustaerosolgenerallyorigi…     

Measurement of aerosol optical extinction using diode laser cavity ringdown spectroscopy

Accurate measurement of optical extinction of atmospheric aerosols is important for quantifying the direct climate effects of aerosols. A portable cavity ringdown spectrometer utilizing a modulated multimode blue diode laser (linewidth ～0.2 nm) is developed to measure the aerosol optical extinction. Laboratory generated ammonia sulfate particles (<1 μm in diameter) are characterized, with good agreements between the experimental measurements and Mie theory calculations. An optical extinction detection sensitivity of 0.24 Mm-1 (1σ) is achieved. Measurements of ambient aerosols are also carried out. This study demonstrates the feasibility of a compact, multimode diode laser cavity ringdown spectrometer for sensitive measurements of the optical extinction of atmospheric aerosols.     

FTIR-ATR chamber for observation of efflorescence and deliquescence processes of NaClO4 aerosol particles on ZnSe substrate

NaClO4 aerosol particles with diameter of 5-20 microns are deposited on the ZnSe substrate. An FTIR-ATR chamber on the ZnSe substrate is set up to observe the structural changes of NaClO4 aerosol particles at crystallization relative humidity （CRH） and deliquescence relative humidity （DRH）. With the decrease of RH （relative humidity） from 96% to 24% in the efflorescence process, the absorbance of O-H stretching band of the aerosol solutions continuously decreases. A sudden decrease of the water peak is observed at RH20%, where solid particles form. Very small amount of residual interfacial water, with two weak peaks at 3602 and 3533 cm^-1, can still be resolved in the FTIR-ATR spectra of the solid particles. In the deliquescence process of the same sample, little spectral changes are observed when the value of RH varies from 5% to 29%. Before the abrupt increase of the O-H stretching band at the DRH of about RH46%, a pre-deliquescence process is observed, i.e. in the RH range between 33% and 46%, there is really a slow absorbance increase for the peak area of O-H stretching band. The O-H stretching band shows an arciform O-H en- velope, totally different from not only the FTIR-ATR spectra of ClO4^- solutions either under supersaturated state or in diluted state, but also the characteristic of the residually interfacial water discussed in the efflorescence process. Such kind of water is considered as pure water, indicating that small amount of water aggregates in the microspaces of solid aerosol particles due to the capillary cohesion effect. When the RH arrives at RH44%, two weak shoulders at 3384 and 3260 cm^-1 can be resolved, and the solid NaClO4 particles begin to be dissolved by increasing capillary cohesion water. The spectral characteristic of the v3-ClO4^- band also shows the transition from solid particles to mainly solvated ClO4^- ions.     

甘肃半干旱区城乡气溶胶光学特性的观测与分析

利用CE318型太阳光度计(532nm波段)在2004年5月-2007年5月的城乡观测资料,反演分析了半干旱地区城乡气溶胶的光学特征.得到了气溶胶光学厚度(AOD)的年季变化,并对不同季节气溶胶的光学厚度以及波长指数的变化规律进行了讨论.结合兰州市郊区资料,对城郊大气气溶胶光学特征进行了对比及原因分析.认为较城市而言,半干旱区乡村大气总体上较城市更为洁净.城市气溶胶受到冬季采暖期等人为因素的影响,出现了AOD冬季大、夏季小的特点.气溶胶主要以工业粉尘和沙尘气溶胶为主,夜间逆温层对AOD的日变化影响较大.乡村春季沙尘天气较多,气溶胶浓度变化受季节的影响,春季AOD最大.气溶胶主控粒子多为沙尘粒子.     

Validating a dust production model by field experiment in Mu Us Desert, China

It is essential for validation and improvement of a dust production model to perform field observations on dust emissions. The dust production model (DPM model) consists of two physically explicit sub-models, namely saltation model [1, 2] (eq. (1)) and sandblasting model [3] (eqs. (2) and (3)). Fh is saltation flux, E is fraction of erodible surface, C is a dimensional constant, ρa is air density, g is gravitational acceleration, U* is the wind friction velocity, Ut*(Dp) is threshold frict…     

大气复合污染新型观测技术研究进展

 大气中的污染物种类繁多,来源和演化过程复杂,而且污染物之间在一定的条件下发生相互作用,形成一种彼此耦合的复杂污染体系,被称为复合污染。为了研究大气复合污染的形成原因及其控制手段,必然要求对各种大气污染的主要物种浓度进行测量,特别是超细粒子、有机气溶胶和挥发性有机物组分复杂,对检测技术要求较高。介绍了针对大气复合污染的新型观测技术,综述了以下3项技术的发展：超细气溶胶颗粒物观测新技术、气溶胶有机物组分分析新技术和挥发性有机物分析新技术,同时综述了大气复合污染的其他监测手段。     

Crystallization kinetics of sea-salt aerosols studied by high-speed photography

Morphological changes with decreasing relative humidity(RH) of supersaturated sea-salt aerosol droplets on a quartz substrate were observed using a high-speed video-camera.Stable gypsum(CaSO4·2H2O) or the metastable hemihydrate(CaSO4·0.5H2O) were precipitated as the RH decreased.The dynamic process of crystal growth under steady-state humidity was studied by controlling the RH;the metastable hemihydrate was precipitated at 70.5%-77.1% RH,and the apparent crystal growth rate was between 1.42 and 2.33 μm3/s.Stable gypsum was formed at 80.7%-82.2% RH,and the apparent crystal growth rate was between 0.70 and 0.81 μm3/s.     

兰州远郊区春季碳气溶胶的质量浓度特征

 为探讨春季沙尘(暴)期间兰州大学半干旱气候与环境观测站(SACOL)碳气溶胶的变化特征, 2012 年5 月17-26 日于SACOL 站采用石英膜收集PM₁₀样品, 利用DRI-2001A 热/光碳分析仪测量元素碳(EC)和有机碳(OC)的质量浓度。结果显示, 沙尘(暴)是导致OC、EC 质量浓度增大的主要因素。采样期间EC、OC 和总碳(TC)的平均质量浓度分别为2.71、11.26 和13.97 μg/m³。进一步分析显示, 沙尘(暴)期间兰州城区碳气溶胶污染逐渐加重主要受本地源的影响。PM₁₀中OC 和EC 的相关系数达到0.94, 揭示SACOL 站OC、EC 的来源相对一致。OC/EC 的均值为5.05, 表明春季SACOL 站PM₁₀中碳气溶胶存在二次污染。二次有机碳(SOC)的质量浓度为3.37 μg/m³, 为OC 的29.9%。结合考察周边环境, 分析表明SACOL 站春季碳气溶胶的主要来源是直接污染源, 来自周边环境中的燃煤以及机动车尾气排放。对碳气溶胶8 种组分的因子分析结果也表明, 周边环境的燃煤和机动车尾气排放是春季SACOL 站碳气溶胶的主要贡献源。     

钢铁过程细微颗粒物凝并性能研究

为寻求一种收集钢铁冶炼过程中产生的气溶胶颗粒的方法,研究了EAF粉尘颗粒物的性质.采用Zn蒸汽氧化产生的ZnO模拟气溶胶颗粒进行凝并实验研究,另采用熏香烟雾在不同的搅拌速度下进行气溶胶凝并实验,并将实验结果与理论计算进行比较.同时,采用一种考虑颗粒间相互作用的气溶胶凝并模型估算反应范德华力作用的Hamaker常数.实验结果表明,在搅拌条件下,对于气溶胶的凝并应考虑微细颗粒间的相互作用.     

Properties of garnet-type Li6La3ZrTaO12 solid electrolyte films fabricated by aerosol deposition method

The garnet-type Li_6La_3ZrTaO_(12)(LLZT) solid electrolyte films were fabricated by aerosol deposition(AD)method.Ball-milled LLZT powder with a cubic garnet structure and a particle size of 1-2 urn was used as raw material and deposited directly on a SUS316L or a glass substrate via impact consolidation.As-deposited LLZT film has a cubic garnet structure but contains Li_2CO_3 and La_2Zr_2O_7 phases.SEM observation revealed that the film consists of LLZT particles fractured into submicron size.The impurity phase formation during AD process was caused by the local heating by the collision between LLZT particles and deposition surface and reaction with CO_2.The Li~+ ion conductivity of LLZT film was estimated to be 0.24 × 10~(-5)S cm~(-1) at room temperature.Electronic conductivity of LLZT film was confirmed to be around 10~(-12) S cm~(-1),indicating the dominant Li~+ ion conduction of LLZT film.     

Distribution and origin of aerosol and its transform relationship with CCN derived from the spring multi-aircraft measurements of Beijing Cloud Experiment (BCE)

The atmospheric aerosol distribution,source and relationship with cloud condensation nuclei(CCN) observed during the Beijing Cloud Experiment(BCE) are analyzed.The results show that the high number concentrations of aerosol mainly distributed below 4500 m,and the magnitude could reach to 103 cm 3.Above 4500 m,the aerosol number concentrations decreased to 101 cm 3 as the altitude increases,and the aerosol mean diameters were between 0.16 and 0.19 μm.Below 4500 m,the number size distributions of aerosol showed a bimodal(multimodal) mode,and an unimodal mode above it.Due to the different sources of aerosol,the conversion ratios of aerosol to CCN were less than 20% below 4500 m,and reached 50% above the level at 0.3% supersaturation.The back trajectories showed that aerosols at higher levels above 4500 m were strongly affected by large-size particles and those below 4500 m were strongly affected by local or regional pollution.Based on observations,a relationship between the CCN number concentration and aerosol number concentration is established.     

Characteristics of distribution and seasonal variation of aerosol optical depth in eastern China with MODIS products

The accuracy of MODIS aerosol products from the NASA Terra Satellite is validated in comparison with the results of sun-photometer observations in Beijing and Hong Kong. By analyzing the MODIS aerosol products within the period of August 2000 to April 2003, it is believed that human activities are the main source of aerosols in the eastern part of China. This is based on the facts that all areas with relatively high values are consistent with regions of dense population and fast economic development, such as the North China Plain, the Sichuan Basin and the Pearl River Delta. It is also supported by the distribution of 舗gstr鰉 exponents showing that most aerosols in the eastern part of China are closely related to human activities, excepting the strong sandstorm episodes occurring in spring, fall and winter. In contrast to developed countries, the 舗gstr鰉 exponent of urban area in China is lower than its surroundings, indicating that the contribution of local floating dust and soot attributed to human activities is significant. Results presented in this paper provide important data for further research on climatic change and environmental study.