Hygroscopic properties of sodium and potassium salts as related to saline mineral dusts and sea salt aerosols

Mineral dust, soil, and sea salt aerosols are among the most abundant primary inorganic aerosols in the atmosphere, and their hygroscopicity affects the hydrological cycle and global climate. We investigated the hygroscopic behaviors of six Na- and K-containing salts commonly found in those primary organic aerosols. Their hygroscopic growths as a function of relative humidity (RH) agree well with thermodynamic model prediction. Temperature dependence of deliquescence RH (DRH) values for five of those salts was also investigated, which are comparable to those in literature within 1%–2% RH, most showing negative dependence on temperature. Hygroscopic growth curves of real-world soil and sea salt samples were also measured. The hygroscopic growths of two more-hydroscopic saline soil samples and of sea salt can be predicted by the thermodynamic model based on the measured water-soluble ionic composition. The substantial amounts of water-soluble ions, including Na⁺ and K⁺, in saline soil samples imply that even nascent saline soil samples are quite hygroscopic at high-RH (>80%) conditions. For three less-hygroscopic dust samples, however, measurements showed higher water uptake ability than that predicted by the thermodynamic model. The small amount of water taken up by less-hygroscopic dust samples suggests that dust particles might contain thin layers of water even to very low RH. The results of this study provide a comprehensive characterization of the hygroscopicity of Na- and K-containing salts as related to their roles in the hygroscopic behaviors of saline mineral dusts and sea salt aerosols.     

Atmospheric Particle Hygroscopicity and the Influence by Oxidation State of Organic Aerosols in Urban Beijing

A hygroscopic tandem differential mobility analyser (H-TDMA) was used to observe the size-resolved hygroscopic characteristics of submicron particles in January and April 2018 in urban Beijing. The probability distribution of the hygroscopic growth factor (HGF-PDF) in winter and spring usually showed a bimodal pattern, with more hygroscopic mode (MH) being more dominant. The seasonal variation in particle hygroscopicity was related to the origin of air mass, which received polluted southerly air masses in spring and clean northwesterly air masses in winter. Particles showed stronger hygroscopic behaviour during heavy pollution episodes (HPEs) with elevated concentrations of secondary aerosols, especially higher mass fraction of nitrate, which were indicated using the PM_2.5 (particulate matter with diameter below 2.5 µm) mass concentration normalised by CO mass concentration. The hygroscopic parameter (κ) values were calculated using H-TDMA (κ_htdma) and chemical composition (κ_chem). The closure study showed that κ_chem was overestimated in winter afternoon when compared with κ_htdma, because the organic particle hygroscopic parameter (κ_org) was overestimated in the calculations. It was influenced by the presence of a high concentration of hydrocarbon-like organic aerosol (HOA) with a weak water uptake ability. A positive relationship was observed between κ_org and the ratio of oxygenated organic aerosol (OOA) and HOA, thereby indicating that the strong oxidation state enhanced the hygroscopicity of the particles. This study revealed the effect of local emission sources and secondary aerosol formation processes on particle hygroscopicity, which is of great significance for understanding the pollution formation mechanism in the North China Plain.     

Evolution in physiochemical and cloud condensation nuclei activation properties of crop residue burning particles during photochemical aging

As a main form of biomass burning in agricultural countries, crop residue burning is a significant source of atmospheric fine particles. In this study, the aging of particles emitted from the burning of four major crop residues in China was investigated in a smog chamber.The particle size distribution, chemical composition and cloud condensation nuclei(CCN)activity were simultaneously measured. The properties of crop residue burning particles varied substantially among different fuel types. During aging, the particle size and mass concentration increased substantially, suggesting condensational growth by formation of secondary aerosols. The particle composition was dominated by organics. Aging resulted in considerable enhancement of organics and inorganics, with enhancement ratios of 1.24–1.44 and 1.33–1.76 respectively, as well as a continuous increase in the oxidation level of organics. Elevated CCN activity was observed during aging, with the hygroscopicity parameter κ varying from 0.16 to 0.34 for fresh particles and 0.19 to 0.40 for aged particles.Based on the volume mixing rule, the hygroscopicity parameter of organic components(κorg) was derived. κorgexhibited an increasing tendency with aging, which was generally consistent with the tendency of the O:C ratio, indicating that the oxidation level was related to the hygroscopicity and CCN activity of organic aerosols from crop residue burning. Our results indicated that photochemical aging could significantly impact the CCN activation of crop burning aerosols, not only by the production of secondary aerosols, but also by enhancing the hygroscopicity of organic components, thereby contributing to the aerosol indirect climate forcing.     

Hygroscopicity of particles generated from photooxidation of α-pinene under different oxidation conditions in the presence of sulfate seed aerosols

Smog chamber experiments were conducted to investigate the hygroscopicity of particles generated from photooxidation of α-pinene/NOx with different sulfate seed aerosols or oxidation conditions. Hygroscopicity of particles was measured by a tandem differential mobility analyzer （TDMA） in terms of hygroscopic growth factor （Gf）, with a relative humidity of 85%. With sulfate seed aerosols present, Gf of the aerosols decreased very fast before notable secondary organic aerosols （SOA） formation was observed, indicating a heterogeneous process between inorganic seeds and organic products might take place as soon as oxidation begins, rather than only happening after gas-aerosol partition of organic products starts. The final SOA-coated sulfate particles had similar or lower Gf than seed-free SOA. The hygroscopicity of the final particles was not dependent on the thickness but on the hygroscopicity properties of the SOA, which were influenced by the initial sulfate seed particles. In the two designed aging processes, Gf of the particles increased more significantly with introduction of OH radical than with ozone. However, the hygroscopicity of SOA was very low even after a long time of aging, implying that either SOA aging in the chamber was very slow or the Gf of SOA did not change significantly in aging. Using an aerosol composition speciation monitor （ACSM） and matrix factorization （PMF） method, two factors for the components of SOA were identified, but the correlation between SOA hygroscopicity and the proportion of the more highly oxidized factor could be either positive or negative depending on the speciation of seed aerosols present.     

Hygroscopicity of particles generated from photooxidation of α-pinene under diferent oxidation conditions in the presence of sulfate seed aerosols

Smog chamber experiments were conducted to investigate the hygroscopicity of particles generated from photooxidation of α-pinene/NOx with diferent sulfate seed aerosols or oxidation conditions. Hygroscopicity of particles was measured by a tandem diferential mobility analyzer(TDMA) in terms of hygroscopic growth factor(Gf), with a relative humidity of 85%. With sulfate seed aerosols present, Gf of the aerosols decreased very fast before notable secondary organic aerosols(SOA) formation was observed, indicating a heterogeneous process between inorganic seeds and organic products might take place as soon as oxidation begins, rather than only happening after gas-aerosol partition of organic products starts. The final SOA-coated sulfate particles had similar or lower Gf than seed-free SOA. The hygroscopicity of the final particles was not dependent on the thickness but on the hygroscopicity properties of the SOA, which were influenced by the initial sulfate seed particles. In the two designed aging processes, Gf of the particles increased more significantly with introduction of OH radical than with ozone. However, the hygroscopicity of SOA was very low even after a long time of aging, implying that either SOA aging in the chamber was very slow or the Gf of SOA did not change significantly in aging. Using an aerosol composition speciation monitor(ACSM) and matrix factorization(PMF) method, two factors for the components of SOA were identified, but the correlation between SOA hygroscopicity and the proportion of the more highly oxidized factor could be either positive or negative depending on the speciation of seed aerosols present.     

Hygroscopicity and optical properties of alkylaminium sulfates

The hygroscopicity and optical properties of alkylaminium sulfates （AASs） were investigated using a hygroscopicity tandem differential mobility analyzer coupled to a cavity ring-down spectrometer and a nephelometer. AAS particles do not exhibit a deliquescence phenomenon and show a monotonic increase in diameter as the relative humidity （RH） ascends. Hygroscopic growth factors （GFs） for 40, 100 and 150 nm alkylaminium sulfate particles do not show an apparent Kelvin effect when RH is less than 45%, whereas GFs of the salt aerosols increase with initial particle size when RH is higher than 45%. Calculation using the Zdanovskii-Stokes-Robinson mixing rule suggests that hygroscopic growth of triethylaminium sulfate-ammonium sulfate mixtures is non-deliquescent, occurring at very low RH, implying that the displacement of ammonia by amine will significantly enhance the hygroscopicity of （NH4）2SO4 aerosols. In addition, light extinction of AAS particles is a combined effect of both scattering and absorption under dry conditions, but is dominated by scattering under wet conditions.     

Persistence and growth of faecal culturable bacterial indicators in water column and sediments of Vidy Bay, Lake Geneva, Switzerland

The aims of this study was to investigate the persistence and the growth of culturable bacterial indicators (CBI) including total coliforms (TC) and faecal coliforms represented by Escherichia coli, enterococcus (ENT), and aerobic mesophilic bacteria (AMB) in the surface sediments and the water column of Vidy Bay (Lake Geneva, City of Lausanne, Switzerland). The study was carried out for 60 d using microcosms containing Sewage Treatment Plant (STP) e uent and nonsterile water without CBI, as well as contaminated and non-contaminated sediments. The e ects of water temperature and of organic matter associated with sediments on the survival of CBI in the sediments and the water column were observed. The number of CBI colonies in the contaminated sediments of Vidy Bay and in the STP e uent was almost identical in the order of 105–107, 104–106, 103–105, and 104–107 CFU/100 g sediment or /100 mL water for TC, E. coli, ENT, and AMB respectively. A degradation of CBI was observed in the sediments where organic mater content was low and in the water column at a temperature of 10°C after 5 d of experimentation. In addition, a growth of CBI was observed in the sediment which is rich in organic matter at 20°C. The results of this study indicate: (1) the higher concentrations of the CBI observed in di erent points in the water column of Vidy Bay may not be explained only by the recent contribution of the three potential sources of the Bay contamination including STP and the Chamberonne and Flon Rivers, but also by the persistence, removal from sediment and multiplication of CBI in the sediment and water column; (2) the sediment of Vidy Bay constitute a reservoir of CBI and can even support their growth; and (3) the CBI not only survive in sediments, but also can be remobilized and increased in the water column, therefore, it become a permanent microbiological pollution in Vidy Bay.     

An intensive study on aerosol optical properties and affecting factors in Nanjing, China

The optical properties of aerosol as well as their impacting factors were investigated at a suburb site in Nanjing during autumn from 14 to 28 November 2012. More severe pollution was found together with lower visibility. The average scattering and absorption coefficients(B sca and B abs) were 375.7 ± 209.5 and 41.6 ± 18.7 Mm~(-1), respectively. Higher ?ngstr?m absorption and scattering exponents were attributed to the presence of more aged aerosol with smaller particles. Relative humidity(RH) was a key factor affecting aerosol extinction. High RH resulted in the impairment of visibility, with hygroscopic growth being independent of the dry extinction coefficient. The hygroscopic growth factor was 1.8 ± 1.2 with RH from 19% to 85%.Light absorption was enhanced by organic carbon(OC), elemental carbon(EC) and EC coatings,with contributions of 26%, 44% and 75%(532 nm), respectively. The B sca and B abs increased with increasing N_(100)(number concentration of PM_(2.5)with diameter above 100 nm), PM_1 surface concentration and PM_(2.5)mass concentration with good correlation.     

Role of interaction between selenium and organic matters on causes of Kaschin-Beck disease

Influences of organic matters of soil and water on speciation and biological utilization of selenium are discussed. Humic acid is found to be the main pool of selenium in soil and affects the bio-availability of the element in soil-plant system. Fulvic acid from drinking water inhibits the absorption of selenium taken from diet. The relationship between high content of organic matters of water and selenium deficiency on the causes of KBD could be reflected in the limited synthesis of glutathione peroxidase, which is generally stimulated by fulvic acid from drinking water.     

Drinking water treatment using a submerged internal-circulation membrane coagulation reactor coupled with permanganate oxidation

A submerged internal circulating membrane coagulation reactor(MCR) was used to treat surface water to produce drinking water. Polyaluminum chloride(PACl) was used as coagulant,and a hydrophilic polyvinylidene fluoride(PVDF) submerged hollow fiber microfiltration membrane was employed. The influences of trans-membrane pressure(TMP), zeta potential(ZP) of the suspended particles in raw water, and KMnO_4 dosing on water flux and the removal of turbidity and organic matter were systematically investigated. Continuous bench-scale experiments showed that the permeate quality of the MCR satisfied the requirement for a centralized water supply, according to the Standards for Drinking Water Quality of China(GB 5749-2006), as evaluated by turbidity(1 NTU) and total organic carbon(TOC)(5 mg/L)measurements. Besides water flux, the removal of turbidity, TOC and dissolved organic carbon(DOC) in the raw water also increased with increasing TMP in the range of 0.01–0.05 MPa. High ZP induced by PACl, such as 5–9 mV, led to an increase in the number of fine and total particles in the MCR, and consequently caused serious membrane fouling and high permeate turbidity.However, the removal of TOC and DOC increased with increasing ZP. A slightly positive ZP, such as 1–2 mV, corresponding to charge neutralization coagulation, was favorable for membrane fouling control. Moreover, dosing with KMnO_4 could further improve the removal of turbidity and DOC, thereby mitigating membrane fouling. The results are helpful for the application of the MCR in producing drinking water and also beneficial to the research and application of other coagulation and membrane separation hybrid processes.     

基于化学组分参数化的大气气溶胶吸湿性特征

为了探讨大气气溶胶的吸湿性特征,基于观测气溶胶化学组分,计算了吸湿性参数κ.首先,通过PCA分析法,得到了对吸湿性参数κ贡献率较大的化学因子;其次,基于K?hler公式与ZSR混合理论,对各化学组分加权得到各时刻对应的吸湿性参数κchemical;最后,基于κ-K?hler理论,讨论κchemical与其相关性,并通过...     

Hygroscopicity of ambient submicron particles in urban Hangzhou, China

In this study, hygroscopicity of size-segregated ambient submicron particles in urban Hangzhou was studied from 28th December 2009 to 18th January 2010, using a hygroscopicity-tandem differential mobility analyzer (H-TDMA). The submicron particles in Hangzhou showed a minor hygroscopic growth at 73% relative humidity (RH), and then grew significantly between 77% and 82% RH. Monomodal distribution accounted for 90% for 30 nm particles, 17% for 50 nm particles, and less than 7% for particles larger than 50 nm at 82% RH. Deconvolution of the bimodal distribution indicated a less hygroscopic group and a more hygroscopic group, with the fraction of the more hygroscopic group increasing with the initial dry particle size and then remaining almost constant for accumulation mode particles. Our results imply that submicron particles in urban Hangzhou were almost entirely externally mixed, and the hygroscopic properties of ambient particles in urban Hangzhou were mainly a function of their size and chemical composition.     

实验室发生纳米气溶胶吸湿性表征

气溶胶吸湿特性对于灰霾的形成、气溶胶对气候变化的影响及人体健康效应具有重要意义. 采用加湿迁移差分分析(HTDMA)法,对实验室发生的8种纳米级无机和有机气溶胶进行吸湿特性定量表征,从而判定影响气溶胶吸湿特性的主要因素. 结果表明,NaCl和(NH₄)₂SO₄气溶胶的潮解点为相对湿度(RH)75%±2%,与理论计算结果相接近,说明测试系统具有一定的可靠性. 对以往研究较少的NaNO₃,CaCl₂,CaSO₄,合成海盐,乙二酸和己二酸气溶胶的测试表明,NaNO₃,CaCl₂以及合成海盐气溶胶随RH的升高粒径逐渐增大;合成海盐气溶胶在RH为86%时吸湿性生长因子(Gf)达到1.80;CaSO₄,乙二酸和己二酸气溶胶随着RH增大未见明显吸湿增长. 通过扫描电镜分析了8种化合物气溶液在不同RH下的形态特征,为掌握各种化学组分对气溶胶吸湿特性的影响提供了微观形态分析的依据.      

大气颗粒物吸湿性研究

大气颗粒物吸湿性是反映颗粒物理化性质的重要指标,吸湿性研究对深入了解颗粒物的环境和健康效应具有重要意义. 总结了国外近年来大气颗粒物吸湿性研究进展:①典型的大气颗粒物吸湿性分析方法为H-TDMA(吸湿性串联差分电迁移率粒径分析仪)系统及其优化方法. ②大气颗粒物吸湿性呈单峰、双峰甚至多峰分布;根据G_f(吸湿性生长因子)随粒径变化的模式,可将大气颗粒物分为强吸湿性和弱吸湿性2类,也可分为纯不溶性、混合不溶性、混合可溶性和纯可溶性4类. ③城市背景点颗粒物的G_f比城市观测点高;城市观测点的颗粒物G_f分布呈夏季高、冬季低,白天高、晚上低的特征. ④颗粒物吸湿性与其化学组成和形态密切相关,纯可溶性盐颗粒物的G_f通常较高. ⑤柴油燃烧源新排放的颗粒物属于弱吸湿性颗粒物,G_f非常小,但在其表面老化后或随燃料中硫含量的增加G_f会明显变大. ⑥生物质燃烧排放颗粒物的G_f相对较高,但存在区域差异性. 针对国内大气颗粒物吸湿性研究现状,提出了未来重点研究方向.      

南京北郊春季气溶胶吸湿性分析

大气气溶胶的吸湿性对气溶胶粒子的谱分布、云凝结核形成、气候强迫、人体健康等均有重要的影响.利用吸湿性串联差分迁移率分析仪(HTDMA)在2014年4月16日~5月21日对南京北郊的大气气溶胶吸湿特性进行观测.30~230 nm气溶胶粒子在90%相对湿度下的吸湿增长观测结果表明,气溶胶粒子的吸湿增长因子平均概率分布函数(GF-PDF)呈现明显的双峰分布,即一个占主导地位的强吸湿模态,和一个相对较小但仍很明显的弱吸湿模态.对吸湿性的日夜对比分析发现,整体上白天的气溶胶粒子吸湿性大于夜间气溶胶粒子,白天强吸湿模态的粒子数目比例高于夜间,夜间气溶胶粒子的外混合程度更高.利用HYSPLIT模式对气溶胶来源分析结果表明,观测期间南京北郊主要受到3类气团的影响.其中西北大陆气团背景下爱根核模态粒子在经过大陆的长距离输送过程后,老化程度较高,吸湿性也更强.而对于积聚模态粒子,则为来自东方气团的粒子吸湿性更强,强吸湿模态粒子数目比例也较高.局地气团背景下气溶胶粒子在各粒径段都具有较高的强吸湿比例.     

南京北郊大气气溶胶的吸湿性观测研究

大气气溶胶的吸湿性不仅影响气溶胶的光学特性进而影响大气能见度,并且影响气溶胶的直接和间接气候效应.本文利用加湿串联差分迁移分析仪H-TDMA,于2012年5~7月在南京地区,对40~200nm大气气溶胶粒子在不同相对湿度下的吸湿增长因子进行了观测研究.统计结果表明:在90%相对湿度下,颗粒物的吸湿增长因子GF多为双峰分布,分为GF1.15的强吸湿组分.弱吸湿组分的吸湿增长因子(GFLH)在1.10~1.14之间;对应的强吸湿组分增长因子(GFMH )范围在1.47~1.58之间变化.相同粒径下的离散程度(σ)强吸湿组大于弱吸湿组,说明强吸湿组的粒子化学成分更复杂,异质性更强.相对湿度的变化对粒子吸湿增长的影响与粒子大小及化学组分有关,爱根核模态和积聚模态粒子在相同的相对湿度下潮解点不同,硝酸铵和硫酸铵是颗粒物中的主要吸湿成分.对不同天气条件下的气溶胶吸湿性分析,发现污染期间的吸湿增长因子(GF)和强吸湿组的数目比例(NFMH)都高于清洁期间,这与当时的气象条件以及粒子的内外部混合状态相关.观测还发现气溶胶粒子的吸湿性有明显的日变化特征,白天光照所引发的光化学反应以及混合层演变而造成粒子的吸湿性较强.机动车尾气排放的黑碳等不吸湿或弱吸湿颗粒物也会因为影响颗粒物的化学成分并进而对气溶胶吸湿性产生影响.     

生物气溶胶的吸湿性

归纳了有关气溶胶吸湿性的测量方法以及过去近30a来文献中报道的生物气溶胶吸湿性的主要研究成果,总结了不同种类生物气溶胶之间吸湿性的差异.已有研究表明,绝大部分的生物气溶胶粒子都具有一定的吸湿性,当相对湿度为90%时,吸湿增长因子约为1.04（真菌孢子）~1.22（细菌）,花粉颗粒物吸湿后的质量与之前的比值为1.30~1.55.最后,提出了目前关于生物气溶胶吸湿性研究中尚未解决的科学问题及该领域的主要发展方向.     

生物气溶胶的吸湿性

归纳了有关气溶胶吸湿性的测量方法以及过去近30a来文献中报道的生物气溶胶吸湿性的主要研究成果,总结了不同种类生物气溶胶之间吸湿性的差异.已有研究表明,绝大部分的生物气溶胶粒子都具有一定的吸湿性,当相对湿度为90%时,吸湿增长因子约为1.04（真菌孢子）~1.22（细菌）,花粉颗粒物吸湿后的质量与之前的比值为1.30~1.55.最后,提出了目前关于生物气溶胶吸湿性研究中尚未解决的科学问题及该领域的主要发展方向.