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- ItemRespiratory tract deposition of inhaled roadside ultrafine refractory particles in a polluted megacity of South-East Asia(Amsterdam [u.a.] : Elsevier Science, 2019) Kecorius, Simonas; Madueño, Leizel; Löndahl, Jakob; Vallar, Edgar; Galvez, Maria Cecilia; Idolor, Luisito F.; Gonzaga-Cayetano, Mylene; Müller, Thomas; Birmili, Wolfram; Wiedensohler, AlfredRecent studies demonstrate that Black Carbon (BC) pollution in economically developing megacities remain higher than the values, which the World Health Organization considers to be safe. Despite the scientific evidence of the degrees of BC exposure, there is still a lack of understanding on how the severe levels of BC pollution affect human health in these regions. We consider information on the respiratory tract deposition dose (DD) of BC to be essential in understanding the link between personal exposure to air pollutants and corresponding health effects. In this work, we combine data on fine and ultrafine refractory particle number concentrations (BC proxy), and activity patterns to derive the respiratory tract deposited amounts of BC particles for the population of the highly polluted metropolitan area of Manila, Philippines. We calculated the total DD of refractory particles based on three metrics: refractory particle number, surface area, and mass concentrations. The calculated DD of total refractory particle number in Metro Manila was found to be 1.6 to 17 times higher than average values reported from Europe and the U.S. In the case of Manila, ultrafine particles smaller than 100 nm accounted for more than 90% of the total deposited refractory particle dose in terms of particle number. This work is a first attempt to quantitatively evaluate the DD of refractory particles and raise awareness in assessing pollution-related health effects in developing megacities. We demonstrate that the majority of the population may be highly affected by BC pollution, which is known to have negative health outcomes if no actions are taken to mitigate its emission. For the governments of such metropolitan areas, we suggest to revise currently existing environmental legislation, raise public awareness, and to establish supplementary monitoring of black carbon in parallel to already existing PM 10 and PM 2.5 measures. © 2019
- ItemA new method to measure real-world respiratory tract deposition of inhaled ambient black carbon(Amsterdam [u.a.] : Elsevier Science, 2019) Madueño, Leizel; Kecorius, Simonas; Löndahl, Jakob; Müller, Thomas; Pfeifer, Sascha; Haudek, Andrea; Mardoñez, Valeria; Wiedensohler, AlfredIn this study, we present the development of a mobile system to measure real-world total respiratory tract deposition of inhaled ambient black carbon (BC). Such information can be used to supplement the existing knowledge on air pollution-related health effects, especially in the regions where the use of standard methods and intricate instrumentation is limited. The study is divided in two parts. Firstly, we present the design of portable system and methodology to evaluate the exhaled air BC content. We demonstrate that under real-world conditions, the proposed system exhibit negligible particle losses, and can additionally be used to determine the minute ventilation. Secondly, exemplary experimental data from the system is presented. A feasibility study was conducted in the city of La Paz, Bolivia. In a pilot experiment, we found that the cumulative total respiratory tract deposition dose over 1-h commuting trip would result in approximately 2.6 μg of BC. This is up to 5 times lower than the values obtained from conjectural approach (e.g. using physical parameters from previously reported worksheets). Measured total respiratory tract deposited BC fraction varied from 39% to 48% during walking and commuting inside a micro-bus, respectively. To the best of our knowledge, no studies focusing on experimental determination of real-world deposition dose of BC have been performed in developing regions. This can be especially important because the BC mass concentration is significant and determines a large fraction of particle mass concentration. In this work, we propose a potential method, recommendations, as well as the limitations in establishing an easy and relatively cheap way to estimate the respiratory tract deposition of BC. In this study we present a novel method to measure real-world respiratory tract deposition dose of Black Carbon. Results from a pilot study in La Paz, Bolivia, are presented. © 2019 The Authors
- ItemSignificant increase of aerosol number concentrations in air masses crossing a densely trafficked sea area(Amsterdam : Elsevier, 2015) Kecorius, Simonas; Kivekäs, Niku; Kristensson, Adam; Tuch, Thomas; Covert, David S.; Birmili, Wolfram; Lihavainen, Heikki; Hyvärinen, Antti-Pekka; Martinsson, Johan; Sporre, Moa K.; Swietlicki, Erik; Wiedensohler, Alfred; Ulevicius, VidmantasIn this study, we evaluated 10 months data (September 2009 to June 2010) of atmospheric aerosol particle number size distribution at three atmospheric observation stations along the Baltic Sea coast: Vavihill (upwind, Sweden), Utö (upwind, Finland), and Preila (downwind, Lithuania). Differences in aerosol particle number size distributions between the upwind and downwind stations during situations of connected atmospheric flow, when the air passed each station, were used to assess the contribution of ship emissions to the aerosol number concentration (diameter interval 50–400 nm) in the Lithuanian background coastal environment. A clear increase in particle number concentration could be noticed, by a factor of 1.9 from Utö to Preila (the average total number concentration at Utö was 791 cm−3), and by a factor of 1.6 from Vavihill to Preila (the average total number concentration at Vavihill was 998 cm−3). The simultaneous measurements of absorption Ångström exponents close to unity at Preila supported our conclusion that ship emissions in the Baltic Sea contributed to the increase in particle number concentration at Preila.
- ItemTerrestrial or marine – indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7° N(Katlenburg-Lindau : European Geosciences Union, 2021) Hartmann, Markus; Gong, Xianda; Kecorius, Simonas; van Pinxteren, Manuela; Vogl, Teresa; Welti, André; Wex, Heike; Zeppenfeld, Sebastian; Herrmann, Hartmut; Wiedensohler, Alfred; Stratmann, FrankIce-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. -38gC and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above -10gC and below -32gC, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95gC for 1ĝ€¯h, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2ĝ€¯μm syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2ĝ€¯μm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with -3.47gC, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above -10gC. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source. © Author(s) 2021.
- ItemAerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment: Case study of Metro Manila, Philippines(Oxford [u.a.] : Elsevier, 2017) Kecorius, Simonas; Madueño, Leizel; Vallar, Edgar; Alas, Honey; Betito, Grace; Birmili, Wolfram; Cambaliza, Maria Obiminda; Catipay, Grethyl; Gonzaga-Cayetano, Mylene; Galvez, Maria Cecilia; Lorenzo, Genie; Müller, Thomas; Simpas, James B.; Tamayo, Everlyn Gayle; Wiedensohler, AlfredUltrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM10 and PM2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm3. That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM2.5. The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authors’ knowledge, no other studies reported such high number concentration of ultrafine refractory particles under ambient conditions. Inverse modeling of emission factors of refractory particle number size distributions revealed that diesel-fed public utility Jeepneys, commonly used for public transportation, are responsible for 94% of total roadside emitted refractory particle mass. The observed results showed that the majority of urban pollution in Metro Manila is dominated by carbonaceous aerosol. This suggests that PM10 or PM2.5 metrics do not fully describe possible health related effects in this kind of urban environments. Extremely high concentrations of ultrafine particles have been and will continue to induce adverse health related effects, because of their potential toxicity. We imply that in megacities, where the major fraction of particulates originates from the transport sector, PM10 or PM2.5 mass concentration should be complemented by legislative measurements of equivalent black carbon mass concentration.
- ItemFrom Transfer to Knowledge Co-Production: A Transdisciplinary Research Approach to Reduce Black Carbon Emissions in Metro Manila, Philippines(Basel : MDPI, 2020) Tõnisson, Liina; Kunz, Yvonne; Kecorius, Simonas; Madueño, Leizel; Tamayo, Everlyn Gayle; Casanova, Dang Marviluz; Zhao, Qi; Schikowski, Tamara; Hornidge, Anna-Katharina; Wiedensohler, Alfred; Macke, AndreasAir pollution, which kills an estimated 7 million people every year, is one of the greatest environmental health risks of our times. Finding solutions to this threat poses challenges to practitioners and policymakers alike. Increasing awareness on the benefits of transdisciplinary research in solution-oriented sustainable development projects has led to the establishment of the research project “A Transdisciplinary Approach to Mitigate Emissions of Black Carbon” (TAME-BC). This paper introduces the TAME-BC research setup that took place with Metro Manila, Philippines, case study. The approach integrates BC measurements with technological, socio-political, and health aspects to improve the scientific state of the art, policymaking, transport sector planning, and clinical studies related to air pollution health effects. The first pillar in the setup presents an (1) air quality assessment through aerosol measurements and instrumentation, complemented by a (2) description and assessment of the current policies, technologies, and practices of the transport sector that is responsible for pollution levels in the Philippines, as well as a (3) BC exposure and associated health impacts assessment. The fourth pillar is intercrossing, fostering (4) knowledge co-creation through stakeholder involvement across scales. We argue that this transdisciplinary approach is useful for research endeavors aiming for emission mitigation in rapidly urbanizing regions beyond Metro Manila.
- ItemVariation of CCN activity during new particle formation events in the North China Plain(München : European Geopyhsical Union, 2016) Ma, Nan; Zhao, Chunsheng; Tao, Jiangchuan; Wu, Zhijun; Kecorius, Simonas; Wang, Zhibin; Größ, Johannes; Liu, Hongjian; Bian, Yuxuan; Kuang, Ye; Teich, Monique; Spindler, Gerald; Müller, Konrad; van Pinxteren, Dominik; Herrmann, Hartmut; Hu, Min; Wiedensohler, AlfredThe aim of this investigation was to obtain a better understanding of the variability of the cloud condensation nuclei (CCN) activity during new particle formation (NPF) events in an anthropogenically polluted atmosphere of the North China Plain (NCP). We investigated the size-resolved activation ratio as well as particle number size distribution, hygroscopicity, and volatility during a 4-week intensive field experiment in summertime at a regional atmospheric observatory in Xianghe. Interestingly, based on a case study, two types of NPF events were found, in which the newly formed particles exhibited either a higher or a lower hygroscopicity. Therefore, the CCN activity of newly formed particles in different NPF events was largely different, indicating that a simple parameterization of particle CCN activity during NPF events over the NCP might lead to poor estimates of CCN number concentration (NCCN). For a more accurate estimation of the potential NCCN during NPF events, the variation of CCN activity has to be taken into account. Considering that a fixed activation ratio curve or critical diameter are usually used to calculate NCCN, the influence of the variation of particle CCN activity on the calculation of NCCN during NPF events was evaluated based on the two parameterizations. It was found that NCCN might be underestimated by up to 30 % if a single activation ratio curve (representative of the region and season) were to be used in the calculation; and might be underestimated by up to 50 % if a fixed critical diameter (representative of the region and season) were used. Therefore, we suggest not using a fixed critical diameter in the prediction of NCCN in NPF. If real-time CCN activity data are not available, using a proper fixed activation ratio curve can be an alternative but compromised choice.
- ItemInfluence of biomass burning on mixing state of sub-micron aerosol particles in the North China Plain(Oxford [u.a.] : Elsevier, 2017) Kecorius, Simonas; Ma, Nan; Teich, Monique; van Pinxteren, Dominik; Zhang, Shenglan; Gröβ, Johannes; Spindler, Gerald; Müller, Konrad; Iinuma, Yoshiteru; Hu, Min; Herrmann, Hartmut; Wiedensohler, AlfredParticulate emissions from crop residue burning decrease the air quality as well as influence aerosol radiative properties on a regional scale. The North China Plain (NCP) is known for the large scale biomass burning (BB) of field residues, which often results in heavy haze pollution episodes across the region. We have been able to capture a unique BB episode during the international CAREBeijing-NCP intensive field campaign in Wangdu in the NCP (38.6°N, 115.2°E) from June to July 2014. It was found that aerosol particles originating from this BB event showed a significantly different mixing state compared with clean and non-BB pollution episodes. BB originated particles showed a narrower probability density function (PDF) of shrink factor (SF). And the maximum was found at shrink factor of 0.6, which is higher than in other episodes. The non-volatile particle number fraction during the BB episode decreased to 3% and was the lowest measured value compared to all other predefined episodes. To evaluate the influence of particle mixing state on aerosol single scattering albedo (SSA), SSA at different RHs was simulated using the measured aerosol physical-chemical properties. The differences between the calculated SSA for biomass burning, clean and pollution episodes are significant, meaning that the variation of SSA in different pollution conditions needs to be considered in the evaluation of aerosol direct radiative effects in the NCP. And the calculated SSA was found to be quite sensitive on the mixing state of BC, especially at low-RH condition. The simulated SSA was also compared with the measured values. For all the three predefined episodes, the measured SSA are very close to the calculated ones with assumed mixing states of homogeneously internal and core-shell internal mixing, indicating that both of the conception models are appropriate for the calculation of ambient SSA in the NCP.
- ItemHeterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: Roles of aerosol water content and chemical composition(Katlenburg-Lindau : EGU, 2018) Tham, Yee Jun; Wang, Zhe; Li, Qinyi; Wang, Weihao; Wang, Xinfeng; Lu, Keding; Ma, Nan; Yan, Chao; Kecorius, Simonas; Wiedensohler, Alfred; Zhang, Yuanhang; Wang, TaoHeterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (γ(N2O5)) and ClNO2 production yield (ϕ) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined γ(N2O5) and ϕ values varied greatly, with an average of 0.022 for γ(N2O5) (±0.012, standard deviation) and 0.34 for ϕ (±0.28, standard deviation). The variations in γ(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived ϕ showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for γ(N2O5) and ϕ to accurately assess photochemical and haze pollution.
- ItemSignificant concentrations of nitryl chloride sustained in the morning: Investigations of the causes and impacts on ozone production in a polluted region of northern China(München : European Geopyhsical Union, 2016) Tham, Yee Jun; Wang, Zhe; Li, Qinyi; Yun, Hui; Wang, Weihao; Wang, Xinfeng; Xue, Likun; Lu, Keding; Ma, Nan; Bohn, Birger; Li, Xin; Kecorius, Simonas; Größ, Johannes; Shao, Min; Wiedensohler, Alfred; Zhang, Yuanhang; Wang, TaoNitryl chloride (ClNO2) is a dominant source of chlorine radical in polluted environment, and can significantly affect the atmospheric oxidative chemistry. However, the abundance of ClNO2 and its exact role are not fully understood under different environmental conditions. During the summer of 2014, we deployed a chemical ionization mass spectrometer to measure ClNO2 and dinitrogen pentoxide (N2O5) at a rural site in the polluted North China Plain. Elevated mixing ratios of ClNO2 (> 350 pptv) were observed at most of the nights with low levels of N2O5 (< 200 pptv). The highest ClNO2 mixing ratio of 2070 pptv (1 min average) was observed in a plume from a megacity (Tianjin), and was characterized with a faster N2O5 heterogeneous loss rate and ClNO2 production rate compared to average conditions. The abundant ClNO2 concentration kept increasing even after sunrise, and reached a peak 4 h later. Such highly sustained ClNO2 peaks after sunrise are discrepant from the previously observed typical diurnal pattern. Meteorological and chemical analysis shows that the sustained ClNO2 morning peaks are caused by significant ClNO2 production in the residual layer at night followed by downward mixing after breakup of the nocturnal inversion layer in the morning. We estimated that ∼ 1.7–4.0 ppbv of ClNO2 would exist in the residual layer in order to maintain the observed morning ClNO2 peaks at the surface site. Observation-based box model analysis show that photolysis of ClNO2 produced chlorine radical with a rate up to 1.12 ppbv h−1, accounting for 10–30 % of primary ROx production in the morning hours. The perturbation in total radical production leads to an increase of integrated daytime net ozone production by 3 % (4.3 ppbv) on average, and with a larger increase of 13 % (11 ppbv) in megacity outflow that was characterized with higher ClNO2 and a relatively lower oxygenated hydrocarbon (OVOC) to non-methane hydrocarbon (NMHC) ratio.