Investigation on condensable particulate matter emission characteristics in wet ammonia-based desulfurization system

Particulate matter emissions from ammonia-based wet flue gas desulfurization (Ammonia-WFGD) systems are composed of a filterable particulate matter and a condensable particulate matter (CPM) portion. However, the CPM part has been ignored for a long time, which results in an underestimation of the aerosol problems caused by Ammonia-WFGD systems. In our research, the characteristics of the CPM that emits from an Ammonia-WFGD system are investigated experimentally for the first time, with the US Environmental Protection Agency Method 202 employed as the primary measurement. The influences of some essential desulfurizing parameters are evaluated based on the experimental data. The results show that CPM contributes about 68.8% to the total particulate matter emission. CPM consists mainly of ammonium sulfates/sulfites, with the organic part accounting for less than 4%. CPM is mostly in the submicron fraction, about 71.1% of which originates from the NH₃–H₂O–SO₂ reactions. The appropriate adjustments for the parameters of the flue gas and the desulfurizing solution can inhibit CPM formation to different extents. This indicates that the parameter optimizations are promising in solving CPM emission problems in Ammonia-WFGD systems, in which the pH adjustment alone can abate CPM emission by around 49%. The opposite variations of the parameters need attention because they can cause tremendous CPM emission increase.     

Physicochemical and toxicological characteristics of nanoparticles in aerosols in southern Thailand during recent haze episodes in lower southeast Asia

Transboundary haze from biomass burning is one of the most important air pollutions in Southeast Asia. The most recent serious haze episode occurred in 2015. Southern Thailand was affected by the haze during September to October when the particulate matter concentration hit a record high. We investigated physical and chemical characteristics of aerosols, including concentration and aerosol size distribution down to sub-micron sizes during haze episodes in 2013 and 2015 and, for reference, an insignificant haze period in 2017. The highest total suspended particulates and PM₁₀ levels in Hat Yai city were 340.1 and 322.5 µg/m³. The mass fractions were nanoparticles (< 100 nm) 3.1%-14.8% and fine particles (< 1 µm) 54.6%-59.1%. Polycyclic aromatic hydrocarbon size distributions in haze periods peaked at 0.75 µm and the concentrations are 2-30 times higher than the normal period. High molecular weight (4-6 ring) PAHs during the haze episode contribute to about 56.7%-88.0% for nanoparticles. The average values of benzo(a)pyrene toxic equivalency quotient were 3.34±2.54ng/m³ in the 2015 haze period but only 0.89±0.17 ng/m³ in 2017. It is clear that particles smaller than 1 µm, were highly toxic. Nanoparticles contributed 19.4%-26.0% of total BaP-TEQ, whereas the mass fraction is 13.1%-14.8%. Thus the nanoparticles were more carcinogenic and can cause greater health effect than larger particles. The fraction of BaP-TEQ for nanoparticles during 2017 non-haze period was nearly the same, while the mass fraction was lower. This indicates that nanoparticles are the significant source of carcinogenic aerosols both during haze and non-haze periods.     

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer(AMS) and Single Particle Aerosol Mass Spectrometer(SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2–1.0 μm, accounting for over 97% of the total particles measured by both instruments.Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH4+was obtained by AMS, while extremely low value of NH4+was detected by SPAMS. Contrarily, high particle number counts of NO3-and Clwere given by SPAMS while low concentrations of NO3-and Cl-were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments.     

测定气溶胶灭火剂产物PH值的新方法

气溶胶灭火剂是高效灭火剂，气溶胶灭火剂产物PH值测量对新型气溶胶灭火剂的开发有指导作用。与传统方法不同，本方法测量出的PH值具有唯一性，即每种气溶胶灭火剂产物的PH测定值与气溶胶灭火剂产物的组成有关而与吸收水量、吸收时间、气溶胶的留空时间无关。该方法能更好的比较不同气溶胶灭火剂产物间的酸碱度。     

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.     

云贵高原1961-2006年大气能见度和消光因素变化趋势及原因

根据云贵高原203个气象台站1961—2006年大气能见度、降水、相对湿度、风速和天气现象等观测资料,采用倾向率方法对能见度和大气消光系数的变化趋势进行了分析。还应用Mann-Kendall方法对19km能见度、霾日数和消光系数的多年变化进行了气候突变检验。结果表明,有84.2%台站出现了能见度减少趋势。减少最多为-11km·10a-1,最少为-1km·10a-1。减少的平均气候倾向率在1961—1979年为0.96km·10a-1,1980—2006年为1.6km·10a-1,高原平均能见度从60年代的约34km下降到目前的约27km。另一方面,有15.8%台站能见度有增加趋势,且多集中在人类活动较为稀少的高海拔山区。有71%的台站19km能见度频率出现减少的趋势,平均倾向率为-2%·10a-1,主要出现在高原东部和中部人口和工业稠密区。该地区同时也出现霾日增加的现象。Mann-Kendall检测结果表明,19km能见度频率减少和霾日数增加现象出现突变的时间相同。年平均消光系数发生突变的时间稍推后。认为能见度下降、消光因素增加的原因与人为排放污染物浓度增加有密切关系。     

δ15N-stable isotope analysis of NHx: An overview on analytical measurements,source sampling and its source apportionment

• Challenges in sampling of NH₃ sources for d¹⁵N analysis are highlighted. • Uncertainties in the isotope-based source apportionment of NH₃ and NH₄⁺ are outlined. • Characterizing dynamic isotopic fractionation may reduce uncertainties of NH_x science. Agricultural sources and non-agricultural emissions contribute to gaseous ammonia (NH₃) that plays a vital role in severe haze formation. Qualitative and quantitative contributions of these sources to ambient PM_2.5 (particulate matter with an aerodynamic equivalent diameter below 2.5 µm) concentrations remains uncertain. Stable nitrogen isotopic composition (δ¹⁵N) of NH₃ and NH₄⁺ (δ¹⁵N(NH₃) and δ¹⁵N(NH₄⁺), respectively) can yield valuable information about its sources and associated processes. This review provides an overview of the recent progress in analytical techniques for δ¹⁵N(NH₃) and δ¹⁵N(NH₄⁺) measurement, sampling of atmospheric NH₃ and NH₄⁺ in the ambient air and their sources signature (e.g., agricultural vs. fossil fuel), and isotope-based source apportionment of NH₃ in urban atmosphere. This study highlights that collecting sample that are fully representative of emission sources remains a challenge in fingerprinting δ¹⁵N(NH₃) values of NH₃ emission sources. Furthermore, isotopic fractionation during NH₃ gas-to-particle conversion under varying ambient field conditions (e.g., relative humidity, particle pH, temperature) remains unclear, which indicates more field and laboratory studies to validate theoretically predicted isotopic fractionation are required. Thus, this study concludes that lack of refined δ¹⁵N(NH₃) fingerprints and full understanding of isotopic fractionation during aerosol formation in a laboratory and field conditions is a limitation for isotope-based source apportionment of NH₃. More experimental work (in chamber studies) and theoretical estimations in combinations of field verification are necessary in characterizing isotopic fractionation under various environmental and atmospheric neutralization conditions, which would help to better interpret isotopic data and our understanding on NH_x (NH₃ + NH₄⁺) dynamics in the atmosphere.     

Electrostatic ignition of sensitive flammable mixtures: Is charge generation due to bubble bursting in aqueous solutions a credible hazard?

Experiments have been conducted to gain insight into the credibility of sparging aqueous solutions as an electrostatic ignition hazard for sensitive hydrogen/air or fuel/oxygen mixtures (Minimum Ignition Energies of ∼0.017 mJ and ∼0.002 mJ, respectively, compared to ∼0.25 mJ for hydrocarbon/air mixtures). Tests performed in a 0.5 m³ ullage produced electric field strengths between 125 and 560 V m⁻¹ for air flows of 5–60 l min⁻¹, respectively, comprised of 2–4 mm diameter bubbles. Field strength can be related to the space charge and fitting to an exponential accumulation curve enabled the charge generation rate from the air flows to be estimated. This was observed to be directly proportional to the air flow and its magnitude was consistent with literature data for bubble bursts. The charge accumulation observed at laboratory scale would not be a cause for concern. On the basis of a simple model, the charge accumulation in a 27 m³ ullage was predicted for a range of air flows. It is apparent from such calculations that ignition of hydrocarbon/air mixtures would not be expected. However, it would seem possible that field strengths might be sufficient to cause a risk of incendive spark or corona discharges in moderately sized vessels with sensitive flammable mixtures.     

Modeling radiative effects of haze on summer-time convective precipitation over North China: a case study

We modeled the impact of haze radiative effects on precipitation in North China. Shortwave heating induced by haze radiative effects would reduce heavy rainfalls. Convection was the key factor that whether precipitation was enhanced or suppressed. Precipitation was often suppressed where CAPE, RH and updraft velocities were high. The impact of haze radiative effect on summertime 24-h convective precipitation over North China was investigated using WRF model (version 3.3) through model sensitivity studies between scenarios with and without aerosol radiative effects. The haze radiative effect was represented by incorporating an idealized aerosol optical profile, with AOD values around 1, derived from the aircraft measurement into the WRF shortwave scheme. We found that the shortwave heating induced by aerosol radiative effects would significantly reduce heavy rainfalls, although its effect on the post-frontal localized thunderstorm precipitation was more diverse. To capture the key factors that determine whether precipitation is enhanced or suppressed, model grids with 24-h precipitation difference between the two scenarios exceeding certain threshold (>30 mm or<-30 mm) were separated into two sets. Analyses of key meteorological variables between the enhanced and suppressed regimes suggested that atmospheric convection was the most important factor that determined whether precipitation was enhanced or suppressed during summertime over North China. The convection was stronger over places with precipitation enhancement over 30 mm. Haze weakened the convection over places with precipitation suppression exceeding 30 mm and caused less water vapor to rise to a higher level and thus further suppressed precipitation. The suppression of precipitation was often accompanied with relatively high convective available potential energy (CAPE), relative humidity (RH) and updraft velocities.     

Water-soluble inorganic ions in airborne particulates from the nano to coarse mode: a case study of aerosol episodes in southern region of Taiwan

In 2004, airborne particulate matter (PM) was collected for several aerosol episodes occurring in the southern region of Taiwan. The particulate samples were taken using both a MOUDI (Micro-orifice Uniform Deposit Impactor) and a nano-MOUDI sampler. These particulate samples were analyzed for major water-soluble ionic species with an emphasis to characterize the mass concentrations and distributions of these ions in the ambient ultrafine (PM_0.1, diameter <0.1 μm) and nano mode (PM_nano, diameter <0.056 μm) particles. Particles collected at the sampling site (the Da-Liao station) on the whole exhibited a typical tri-modal size distribution on mass concentration. The mass concentration ratios of PM_nano/PM_2.5, PM_0.1/PM_2.5, and PM₁/PM_2.5 on average were 1.8, 2.9, and 71.0%, respectively. The peak mass concentration appeared in the submicron particle mode (0.1 μm < diameter <1.0 μm). Mass fractions (percentages) of the three major water-soluble ions (nitrate, sulfate, and ammonium) as a group in PM_nano, PM_0.1, PM₁, and PM_2.5 were 18.4, 21.7, 50.0, and 50.7%, respectively. Overall, results from this study supported the notion that secondary aerosols played a significant role in the formation of ambient submicron particulates (PM_0.1−1). Particles smaller than 0.1 μm were essentially basic, whereas those greater than 2.5 μm were neutral or slightly acidic. The neutralization ratio (NR) was close to unity for airborne particles with diameters ranging from 0.18 to 1 μm. The NRs of these airborne particles were found strongly correlated with their sizes, at least for samples taken during the aerosol episodes under study. Insofar as this study is exploratory in nature, as only a small number of particulate samples were used, there appears to be a need for further research into the chemical composition, source contribution, and formation of the nano and ultrafine mode airborne particulates.