影响北仑区域能见度的因素研究

利用对北仑区域内的气溶胶散射系数、气溶胶浓度、黑炭浓度以及NO2浓度的监测和分析,对区域影响能见度的的因素进行了研究,研究结果表明,影响能见度的消光系数主要由气溶胶的散射、气溶胶的吸收,干洁大气的散射和气态污染物的吸收四项组成,且组成比例总体稳定,但是,不同空气质量级别和灰霾天与非灰霾天之间的消光系数值及组成差异较大;通过对气溶胶与光散射系数的拟合得到,两者存在较好的正相关性。     

Evaluation of the influence of El Niño–Southern Oscillation on air quality in southern China from long-term historical observations

•Strong ENSO influence on AOD is found in southern China region. •Low AOD occurs in El Niño but high AOD occurs in La Niña events in southern China. •Angstrom exponent anomalies reveals the circulation pattern during each ENSO phase. •ENSO exerts large influence (70.5%) on annual variations of AOD during 2002–2020. •Change of anthropogenic emissions is the dominant driver for AOD trend (2002–2020). Previous studies demonstrated that the El Niño–Southern Oscillation (ENSO) could modulate regional climate thus influencing air quality in the low-middle latitude regions like southern China. However, such influence has not been well evaluated at a long-term historical scale. To filling the gap, this study investigated two-decade (2002 to 2020) aerosol concentration and particle size in southern China during the whole dynamic development of ENSO phases. Results suggest strong positive correlations between aerosol optical depth (AOD) and ENSO phases, as low AOD occurred during El Niño while high AOD occurred during La Niña event. Such correlations are mainly attributed to the variation of atmospheric circulation and precipitation during corresponding ENSO phase. Analysis of the angstrom exponent (AE) anomalies further confirmed the circulation pattern, as negative AE anomalies is pronounced in El Niño indicating the enhanced transport of sea salt aerosols from the South China Sea, while the La Niña event exhibits positive AE anomalies which can be attributed to the enhanced import of northern fine anthropogenic aerosols. This study further quantified the AOD variation attributed to changes in ENSO phases and anthropogenic emissions. Results suggest that the long-term AOD variation from 2002 to 2020 in southern China is mostly driven (by 64.2%) by the change of anthropogenic emissions from 2002 to 2020. However, the ENSO presents dominant influence (70.5%) on year-to-year variations of AOD during 2002–2020, implying the importance of ENSO on varying aerosol concentration in a short-term period.     

MAX-DOAS observation in the midlatitude marine boundary layer: Influences of typhoon forced air mass

As a passive remote sensing technique, MAX-DOAS method was widely used to investigate the vertical profiles of aerosol and trace gases in the lower troposphere. However, the measurements for midlatitude marine boundary layer are rarely reported, especially during the storm weather system. In this study, the MAX-DOAS was used to retrieve the aerosol, HCHO and NO₂ vertical distribution at Huaniao Island of East China Sea in summer 2018, during which a strong tropical cyclone developed and passed through the measurement site. The observed aerosol optical depth (AOD), HCHO- and NO_2-VCDs (Vertical Column Density) were in the range of 0.19-0.97, (2.57-12.27) × 10¹⁵ molec/cm², (1.24-4.71) × 10¹⁵ molec/cm², which is much higher than remote ocean area due to the short distance to continent. The vertically resolved aerosol extinction coefficient (AEC), HCHO and NO₂ presented the decline trend with the increase of height. After the typhoon passing through, the distribution of high levels of aerosol and HCHO stretched to about 1 km and the abundances of the bottom layer were found as double higher than before, reaching 0.51 km⁻¹ and 2.44 ppbv, while NO₂ was still constrained within about 300 m with 2.59 ppbv in the bottom layer. The impacts of typhoon process forced air mass were also observed at the suburban site in Shanghai in view of both the aerosol extinction and chemical components. The different changes on air quality associated with typhoon and its mechanism in two different environments: coastal island and coastal city are worthy of further investigation as it frequent occurred in East Asia during summer and fall.     

Analysis of PCDD/Fs and dioxin-like PCBs in atmospheric deposition samples from the Flemish measurement network: correlation between the CALUX bioassay and GC-HRMS

Since the CALUX (Chemically Activated LUciferase gene eXpression) bioassay is a fast, sensitive and inexpensive tool for the analysis of a high number of samples, the use of this technique in routine analysis of atmospheric deposition samples may be a valuable alternative for GC-HRMS. In this study, a validated CALUX method was used for the analysis of PCDD/Fs and dioxin-like PCBs in more than 90 atmospheric deposition samples for different locations in Flanders. The samples were taken in residential and agricultural areas, where a threshold limit of 21 pg WHO-TEQ m⁻² d⁻¹ for the sum of PCDD/Fs and dioxin-like PCBs was set, and in industrial zones and natural reserves, where no official threshold limit is available. The results from the Flemish measurement program showed correlation between CALUX and GC-HRMS for all the samples, originating from the different areas (R² of 0.81, 0.53 and 0.64 for dl-PCBs, PCDD/Fs and sum of both fractions, respectively). Median CALUX/GC-HRMS ratios of 2.0, 0.9 and 1.3 were reported for the PCDD/Fs, dioxin-like PCBs and the sum of both fractions, respectively. The results show that the CALUX bioassay is a valuable alternative tool for the classic GC-HRMS analysis of atmospheric deposition samples in the Flemish measurement network.     

Explosive properties of selected aerosols determined in a spherical 5-L test chamber

Combustible liquids in the form of aerosols are important for many industrial processes. Therefore the problem of explosion hazards posed by the aerosols becomes increasingly more prominent. To correctly assess the explosion risk and fulfil the requirements of the ATEX directive, it is necessary to obtain information regarding the flammable and explosive properties of the aerosols. Unlike in the case of gases and dusts, no standard procedures aimed at obtaining quantitative information of this type exist. Factors that influence the explosion dynamics of aerosols include: concentration, droplet size, temperature etc. Some of these factors are strongly dependent on the aerosol generation methods. A prototype apparatus was designed and constructed to address that dependence. The apparatus was used in an attempt to determine the basic explosion parameters of liquid flammable aerosols. The device consisted of a 5-L spherical vessel equipped with a pump-injection system that generated aerosols as well as a spark ignition source. A wide variety of injection settings were tested to select the most suitable conditions over a broad range of concentrations and fluid properties. A measurement procedure was developed for operating the device. Prototype tests were carried out with fluids commonly used in industry: isopropanol and kerosene. The tests demonstrated the significant influence of the vessel wall temperature on the result accuracy. Correct temperature control made it possible to obtain relationships between the aerosol concentration and the following explosion parameters: maximum explosion pressure and maximum rate of pressure rise.     

Chemistry and aerosols in the marine boundary layer: 1-D modelling of the three ACE-2 Lagrangian experiments

Three Lagrangian experiments were conducted during IGAC's second aerosol characterization experiment (ACE-2) in the area between Portugal, Tenerife and Madeira in June/July 1997. During each Lagrangian experiment, a boundary layer air mass was followed for about 30 h, and the temporal evolution of its chemical and aerosol composition was documented by a series of vertical profiles and horizontal box pattern flown by the Meteorological Research Flight research aircraft Hercules C130. The wealth of observational data that has been collected during these three Lagrangian experiments is the basis for the development and testing of a one-dimensional Lagrangian boundary layer model with coupled gas, aqueous, and aerosol phase chemistry. The focus of this paper is on current model limitations and strengths. We show that the model is able to represent the dynamical and chemical evolution of the marine boundary layer, in some cases requiring adjustments of the subsidence velocity and of the surface heat fluxes. Entrainment of a layer rich in ozone and carbon monoxide from a residual continental boundary layer into the marine boundary layer as well as in-cloud oxidation of sulphur dioxide by hydrogen peroxide are simulated, and coherent results are obtained, concerning the evolution of the small, presumably sulphate–ammonia aerosol mode.     

Using the optical properties of aerosols from the AERONET database to calculate surface solar UV-B irradiance in Córdoba, Argentina: Comparison with measurements

The main purpose of this study was to perform an evaluation of the particles’ optical parameters’ influence on surface solar UV-B (280–315 nm) irradiance in Córdoba, Argentina. To achieve this objective UV-B irradiance dataset, AERONET (AErosol RObotic NETwork) database, and TUV (Tropospheric Ultraviolet and Visible) model were used to analyze the effects of aerosols on surface irradiance on cloudless days during specific days of winter and spring of the period 1999–2006. Together with a direct observer, total irradiance (300–3000 nm) measurements were used as an ancillary tool to verify the cloudless condition. Every year, during this period, important reductions in surface irradiance are observed due to the aerosol load. Aerosols were incorporated in the model through the aerosol optical depth at 340 nm, the asymmetry parameter at 440 nm, and the single scattering albedo at 440 nm, all of them provided by AERONET Córdoba-CETT site. These factors vary from near to zero up to 1.4, from 0.56 up to 0.83 and from 0.43 up to 0.99, respectively. The behaviors of these factors along the year are analyzed considering the meteorology of Córdoba. When AERONET data are included in the TUV model they allow an accurate simulation of the UV-B irradiance, making the agreement with the experimental measurements substantially better. Only a small differences (±2%) remains, which can be attributed to diverse factors. As the AERONET site is 20 km away from the irradiance measurement site, these results show the regional character of the aerosols in Córdoba, although small contributions of urban aerosols are not discarded. An episode of high aerosol and pollutants laden due to fires in the surrounding hills is briefly analyzed. A set of additional studies are needed to describe comprehensively the characteristics and behavior of the Córdoba aerosols. Some of them are being already carried out.     

Volcanic sulphate and arctic dust plumes over the North Atlantic Ocean

High time resolution aerosol mass spectrometry measurements were conducted during a field campaign at Mace Head Research Station, Ireland, in June 2007. Observations on one particular day of the campaign clearly indicated advection of aerosol from volcanoes and desert plains in Iceland which could be traced with NOAA Hysplit air mass back trajectories and satellite images. In conjunction with this event, elevated levels of sulphate and light absorbing particles were encountered at Mace Head. While sulphate concentration was continuously increasing, nitrate levels remained low indicating no significant contribution from anthropogenic pollutants. Sulphate concentration increased about 3.8 μg m⁻³ in comparison with the background conditions. Corresponding sulphur flux from volcanic emissions was estimated to about 0.3 TgS yr⁻¹, suggesting that a large amount of sulphur released from Icelandic volcanoes may be distributed over distances larger than 1000 km. Overall, our results corroborate that transport of volcanogenic sulphate and dust particles can significantly change the chemical composition, size distribution, and optical properties of aerosol over the North Atlantic Ocean and should be considered accordingly by regional climate models.     

Analysis of the origin of peak aerosol optical depth in springtime over the Gulf of Tonkin

By aggregating MODIS(moderate-resolution imaging spectroradiometer) AOD(aerosol optical depth) and OMI(ozone monitoring instrument) UVAI(ultra violet aerosol index)datasets over 2010–2014, it was found that peak aerosol loading in seasonal variation occurred annually in spring over the Gulf of Tonkin(17–23°N, 105–110°E). The vertical structure of the aerosol extinction coefficient retrieved from the spaceborne lidar CALIOP(cloud-aerosol lidar with orthogonal polarization) showed that the springtime peak AOD could be attributed to an abrupt increase in aerosol loading between altitudes of 2 and 5 km.In contrast, aerosol loading in the low atmosphere(below 1 km) was only half of that in winter. Wind fields in the low and high atmosphere exhibited opposite transportation patterns in spring over the Gulf of Tonkin, implying different sources for each level. By comparing the emission inventory of anthropogenic sources with biomass burning, and analyzing the seasonal variation of the vertical structure of aerosols over the Northern Indo-China Peninsula(NIC), it was concluded that biomass burning emissions contributed to high aerosol loading in spring. The relatively high topography and the high surface temperature in spring made planetary boundary layer height greater than 3 km over NIC. In addition, small-scale cumulus convection frequently occurred, facilitating pollutant rising to over 3 km, which was a height favoring long-range transport. Thus, pollutants emitted from biomass burning over NIC in spring were raised to the high atmosphere, then experienced long-range transport, leading to the increase in aerosol loading at high altitudes over the Gulf of Tonkin during spring.     

Infrared spectroscopic probing of dimethylamine clusters in an Ar matrix

Amines have many atmospheric sources and their clusters play an important role in aerosol nucleation processes. Clusters of a typical amine, dimethylamine (DMA), of different sizes were measured with matrix isolation IR (infrared) and NIR (near infrared) spectroscopy. The NIR vibrations are more separated and therefore it is easier to distinguish different sizes of clusters in this region. The DMA clusters, up to DMA tetramer, have been optimized using density functional methods, and the geometries, binding energies and thermodynamic properties of DMA clusters were obtained. The computed frequencies and intensities of NH-stretching vibrations in the DMA clusters were used to interpret the experimental spectra. We have identified the fundamental transitions of the bonded NH-stretching vibration and the first overtone transitions of the bonded and free NH-stretching vibration in the DMA clusters. Based on the changes in vibrational intensities during the annealing processes, the growth of clusters was clearly observed. The results of annealing processes indicate that DMA molecules tend to form larger clusters with lower energies under matrix temperatures, which is also supported by the calculated reaction energies of cluster formation.