scholarly journals Urban increments of gaseous and aerosol pollutants and their sources using mobile aerosol mass spectrometry measurements

2016 ◽  
Vol 16 (11) ◽  
pp. 7117-7134 ◽  
Author(s):  
Miriam Elser ◽  
Carlo Bozzetti ◽  
Imad El-Haddad ◽  
Marek Maasikmets ◽  
Erik Teinemaa ◽  
...  

Abstract. Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially resolved detailed characterization of PM2.5 (particulate matter with aerodynamic equivalent diameter daero  ≤  2.5 µm) in two major Estonian cities, Tallinn and Tartu. The measurements were performed in March 2014 using a mobile platform. In both cities, the non-refractory (NR)-PM2.5 was characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC) and several trace gases including carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were also measured. The chemical composition of PM2.5 was found to be very similar in the two cities. Organic aerosol (OA) constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF): hydrocarbon-like OA (HOA, from traffic emissions), biomass burning OA (BBOA, from biomass combustion), residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning), and oxygenated OA (OOA, related to secondary aerosol formation). OOA was the major OA source during nighttime, explaining on average half of the OA mass, while during daytime mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from northern Germany, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and the assessment of the extent to which pollutants concentrations exceeded regional background levels (urban increments). HOA, eBC, CO2, and CO showed stronger enhancements on busy roads during the morning and evening traffic rush hours; BBOA had its maximum enhancement in the residential areas during the evening hours and RIOA was enhanced in both the city center (emissions from restaurants) and in the residential areas (emissions from residential cooking). In contrast, secondary components (OOA, sulfate (SO4), nitrate (NO3), ammonium (NH4), and chloride (Cl)) had very homogeneous distributions in time and space. We were able to determine a total PM2.5 urban increment in Tartu of 6.0 µg m−3 over a regional background concentration of 4.0 µg m−3 (i.e., a factor of 2.5 increase). Traffic exhaust emissions were identified as the most important source of this increase, with eBC and HOA explaining on average 53.3 and 20.5 % of the total increment, respectively.

2016 ◽  
Author(s):  
M. Elser ◽  
C. Bozzetti ◽  
I. El-Haddad ◽  
M. Maasikmets ◽  
E. Teinemaa ◽  
...  

Abstract. Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially-resolved detailed characterization of the PM2.5 in two major Estonian cities (Tallinn and Tartu), using mobile measurements. In both cities, the non-refractory (NR)-PM2.5 was characterized by a highresolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC) and several trace gases including carbon monoxide (CO), carbon dioxide (CO2) and methane (CH4) were also measured. The chemical composition of the PM2.5 was found to be very similar in the two cities. Organic aerosol (OA) constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF): hydrocarbon-like OA (HOA, from traffic emissions), biomass burning OA (BBOA, from biomass combustion), residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning) and oxygenated OA (OOA, related to secondary aerosol formation). OOA was the major OA source during night-time, explaining on average half of the OA mass, while during day-time mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from polluted continental areas, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and an accurate calculation of the urban increments. HOA, eBC, CO2 and CO showed stronger enhancements on busy roads during the morning and evening traffic rush hours; BBOA had its maximum enhancement in the residential areas during the evening hours and RIOA was enhanced in both the city center (emissions from restaurants) and in the residential areas (emissions from residential cooking). In contrast, secondary components (OOA, SO4, NO3, NH4, and Cl) had very homogeneous distributions in time and space. We were able to determine a total PM2.5 urban increment in Tartu of 6.0 μg m−3 over a regional background concentration of 4.0 μg m−3 (i.e., a factor of 2.5 increase). Traffic exhaust emissions were identified as the most important source of this increase, with eBC and HOA explaining on average 53.3 and 20.5 % of the total increment, respectively.


2021 ◽  
Author(s):  
Sanna Saarikoski ◽  
Jarkko V. Niemi ◽  
Minna Aurela ◽  
Liisa Pirjola ◽  
Anu Kousa ◽  
...  

Abstract. This study investigated the sources of black carbon (BC) at two contrasting urban environments in Helsinki, Finland; residential area and street canyon. The sources of BC were explored by using positive matrix factorization (PMF) for the organic and refractory black carbon (rBC) mass spectra collected with a soot particle aerosol mass spectrometer (SP-AMS). Two sites had different local BC sources; the largest fraction of BC originated from biomass burning at the residential site (38 %) and from the vehicular emissions at the street canyon (57 %). Also, the mass size distribution of BC diverged at the sites as BC from traffic was found at the particle size of ~100–150 nm whereas BC from biomass combustion was detected at ~300 nm. At both sites, a large fraction of BC was associated with urban background or long-range transported BC indicated by the high oxidation state of organics related to those PMF factors. The results from the PMF analysis were compared with the source apportionment from the aethalometer model calculated with two pair of absorption Ångström values. It was found that several PMF factors can be attributed to wood combustion and fossil fuel fraction of BC provided by the aethalometer model. In general, the aethalometer model showed less variation between the sources within a day than PMF being less responsive to the fast changes in the BC sources at the site. The results of this study increase understanding of the limitations and validity of the BC source apportionment methods in different environments. Moreover, this study advances the current knowledge of BC sources and especially the contribution of residential combustion in urban areas.


2011 ◽  
Vol 11 (14) ◽  
pp. 6911-6929 ◽  
Author(s):  
R. Xiao ◽  
N. Takegawa ◽  
M. Zheng ◽  
Y. Kondo ◽  
Y. Miyazaki ◽  
...  

Abstract. Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8 ± 8.4 μg m−3 and 13.5 ± 8.7 μg m−3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva) ∼200 nm and the second mode occurred at Dva from 300–700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and oxygenated aerosol. The origin of HOA and OOA (the sum of LV-OOA and SV-OOA) has been further confirmed by the statistics that primary organic carbon (POC) and secondary organic carbon (SOC), estimated by the EC tracer method, were closely correlated with HOA and OOA, respectively. The results of the EC tracer method and of the PMF model revealed that primary organic aerosol (POA) constituted ~34–47 % of OA mass and secondary organic aerosol (SOA) constituted ~53–66 % of regional organic aerosol in PRD during summer season. The presence of abundant SOA was consistent with water soluble organic carbon (WSOC) results (accounting for ~60 % of OC on average) by Miyazaki et al. (2009) for the same campaign. OOA correlated well with WSOC at the BG site, indicating that most OOA were water soluble. More specifically, approximately 86 % of LV-OOA and 61 % of SV-OOA were estimated as water soluble species on the basis of carbon content comparison.


2013 ◽  
Vol 13 (12) ◽  
pp. 6101-6116 ◽  
Author(s):  
E. Z. Nordin ◽  
A. C. Eriksson ◽  
P. Roldin ◽  
P. T. Nilsson ◽  
J. E. Carlsson ◽  
...  

Abstract. Gasoline vehicles have recently been pointed out as potentially the main source of anthropogenic secondary organic aerosol (SOA) in megacities. However, there is a lack of laboratory studies to systematically investigate SOA formation in real-world exhaust. In this study, SOA formation from pure aromatic precursors, idling and cold start gasoline exhaust from three passenger vehicles (EURO2–EURO4) were investigated with photo-oxidation experiments in a 6 m3 smog chamber. The experiments were carried out down to atmospherically relevant organic aerosol mass concentrations. The characterization instruments included a high-resolution aerosol mass spectrometer and a proton transfer mass spectrometer. It was found that gasoline exhaust readily forms SOA with a signature aerosol mass spectrum similar to the oxidized organic aerosol that commonly dominates the organic aerosol mass spectra downwind of urban areas. After a cumulative OH exposure of ~5 × 106 cm−3 h, the formed SOA was 1–2 orders of magnitude higher than the primary OA emissions. The SOA mass spectrum from a relevant mixture of traditional light aromatic precursors gave f43 (mass fraction at m/z = 43), approximately two times higher than to the gasoline SOA. However O : C and H : C ratios were similar for the two cases. Classical C6–C9 light aromatic precursors were responsible for up to 60% of the formed SOA, which is significantly higher than for diesel exhaust. Important candidates for additional precursors are higher-order aromatic compounds such as C10 and C11 light aromatics, naphthalene and methyl-naphthalenes. We conclude that approaches using only light aromatic precursors give an incomplete picture of the magnitude of SOA formation and the SOA composition from gasoline exhaust.


2011 ◽  
Vol 11 (4) ◽  
pp. 12323-12365 ◽  
Author(s):  
C. Mohr ◽  
R. Richter ◽  
P. F. DeCarlo ◽  
A. S. H. Prévôt ◽  
U. Baltensperger

Abstract. Mobile measurements of PM1 (PM with an aerodynamic diameter D<1 μm) chemical composition using a quadrupole aerosol mass spectrometer and a multi-angle absorption photometer were performed using the PSI mobile laboratory during winter 2007/2008 and December 2008 in the metropolitan area of Zurich, Switzerland. Positive matrix factorization (PMF) applied to the organic fraction of PM1 yielded 3 factors: Hydrocarbon-like organic aerosol (HOA) related to traffic emissions; organic aerosol from wood burning for domestic heating purposes (WBOA); and oxygenated organic aerosol (OOA), assigned to secondary organic aerosol formed by oxidation of volatile precursors. The spatial variation of the chemical composition of PM1 shows a uniform distribution throughout the city: for primary emissions, road traffic is important along major roads (varying between 7 and 14% of PM1 for different sites within the city), but overall, domestic wood burning is more important for the organic aerosol concentrations in Zurich during winter time (varying between 8–15% of PM1 for different sites within the city). OOA makes up the largest fraction of organic aerosol (44% on average). A new method, based on simultaneous on-road mobile and stationary background measurements and using the ratio of on-road sulfate to stationary sulfate to correct for small-scale dynamic effects, allows for the separation of PM1 emitted or produced locally and the PM1 from the regional background. It could be shown that especially during thermal inversions over the Swiss plateau, regional background concentrations contribute substantially to particulate number concentrations (60% on average) as well as to the concentrations of PM1 components (on average 60% for black carbon and HOA, over 97% for WBOA and OOA, and more than 94% for the measured inorganic components) in downtown Zurich. The results emphasize, on a scientific level, the advantage of mobile measurements for distinguishing local from regional air pollution, and on a political level, the importance of regional collaboration for mitigating air pollution issues.


2020 ◽  
Author(s):  
Sophia M. Charan ◽  
Reina S. Buenconsejo ◽  
John H. Seinfeld

Abstract. Recent inventory-based analysis suggests that emissions of volatile chemical products in urban areas are now competitive with those from the transportation sector. Understanding the potential for secondary organic aerosol formation from these volatile chemical products is, therefore, critical to predicting levels of aerosol and for formulating policy to reduce aerosol exposure. It is clear that a plethora of oxygenated compounds are either emitted directly into the atmosphere or emitted indoors and later escape into the outdoors. Experimental and computationally simulated environmental chamber data provide an understanding of aerosol yield and chemistry under relevant urban conditions (5–200 ppb NO and 291–312 K) and give insight into the effect of volatile chemical products on the production of secondary organic aerosol. Benzyl alcohol, one of these volatile chemical products, is found to have a large secondary organic aerosol formation potential. At NO concentrations of ~ 80 ppb and 291 K, secondary organic aerosol mass yields for benzyl alcohol can reach 1.


2012 ◽  
Vol 12 (12) ◽  
pp. 31725-31765 ◽  
Author(s):  
E. Z. Nordin ◽  
A. C. Eriksson ◽  
P. Roldin ◽  
P. T. Nilsson ◽  
J. E. Carlsson ◽  
...  

Abstract. Gasoline vehicles have elevated emissions of volatile organic compounds during cold starts and idling and have recently been pointed out as potentially the main source of anthropogenic secondary organic aerosol (SOA) in megacities. However, there is a lack of laboratory studies to systematically investigate SOA formation in real-world exhaust. In this study, SOA formation from pure aromatic precursors, idling and cold start gasoline exhaust from one Euro II, one Euro III and one Euro IV passenger vehicles were investigated using photo-oxidation experiments in a 6 m3 smog chamber. The experiments were carried out at atmospherically relevant organic aerosol mass concentrations. The characterization methods included a high resolution aerosol mass spectrometer and a proton transfer mass spectrometer. It was found that gasoline exhaust readily forms SOA with a signature aerosol mass spectrum similar to the oxidized organic aerosol that commonly dominates the organic aerosol mass spectra downwind urban areas. After 4 h aging the formed SOA was 1–2 orders of magnitude higher than the Primary OA emissions. The SOA mass spectrum from a relevant mixture of traditional light aromatic precursors gave f43 (mass fraction at m/z = 4 3) approximately two times higher than to the gasoline SOA. However O : C and H : C ratios were similar for the two cases. Classical C6–C9 light aromatic precursors were responsible for up to 60% of the formed SOA, which is significantly higher than for diesel exhaust. Important candidates for additional precursors are higher order aromatic compounds such as C10, C11 light aromatics, naphthalene and methyl-naphthalenes.


2020 ◽  
Vol 20 (21) ◽  
pp. 13167-13190
Author(s):  
Sophia M. Charan ◽  
Reina S. Buenconsejo ◽  
John H. Seinfeld

Abstract. Recent inventory-based analysis suggests that emissions of volatile chemical products in urban areas are competitive with those from the transportation sector. Understanding the potential for secondary organic aerosol formation from these volatile chemical products is therefore critical to predicting levels of aerosol and for formulating policy to reduce aerosol exposure. Experimental and computationally simulated environmental chamber data provide an understanding of aerosol yield and chemistry under relevant urban conditions (5–200 ppb NO and 291–312 K) and give insight into the effect of volatile chemical products on the production of secondary organic aerosol. Benzyl alcohol, one of these volatile chemical products, is found to have a large secondary organic aerosol formation potential. At NO concentrations of ∼ 80 ppb and 291 K, secondary organic aerosol mass yields for benzyl alcohol can reach 1.


2011 ◽  
Vol 11 (1) ◽  
pp. 1891-1937
Author(s):  
R. Xiao ◽  
N. Takegawa ◽  
M. Zheng ◽  
Y. Kondo ◽  
Y. Miyazaki ◽  
...  

Abstract. Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the Southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8±8.4 μg m−3 and 13.5±8.7 μg m−3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva)~200 nm and the second mode occurred at Dva from 300–700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and oxygenated aerosol. The origin of HOA and OOA (the sum of LV-OOA and SV-OOA) has been further confirmed by the statistics that primary organic carbon (POC) and secondary organic carbon (SOC), estimated by the EC tracer method, were closely correlated with HOA and OOA, respectively. The results of the EC tracer method and of the PMF model revealed that primary organic aerosol (POA) constituted ~34–47% of OA mass and secondary organic aerosol (SOA) constituted ~53–66% of regional organic aerosol in PRD during summer reason. The presence of abundant SOA was consistent with water soluble organic carbon (WSOC) results (accounting for ~60% of OC on average) by Miyazaki et al. (2009) for the same campaign. OOA correlated well with WSOC at the BG site, indicating that most OOA were water soluble. More specifically, approximately 86% of LV-OOA and 61% of SV-OOA were estimated as water soluble species on the basis of carbon content comparison.


Author(s):  
А.В. Терешкин ◽  
А.Л. Калмыкова ◽  
Т.А. Андрушко

Вертикальное озеленение с участием различных видов лиан в современных условиях имеет важное эстетическое и санитарно-гигиеническое значение. Особо актуально решение вопросов обогащения флоры городских территорий лианами в степных районах в связи с бедным видовым составом и резким ухудшением экологической ситуации. Объектами исследований являлись 7 видов лиан, различных жизненных форм (однолетние, многолетние), произрастающие в населенных пунктах Саратовской области (Аткарск, Саратов). Цель исследований – изучение эколого-биологических особенностей и мелиоративных свойств лиан и выявление перспектив их использования в вертикальном озеленении селитебных территорий Саратовской области. В ходе исследования видового состава, были выявлены наиболее популярные виды однолетних лиан: ипомея красно-голубая (Ipomea tricolor (L.) Roth) и ипомея пурпурная (Ipomea purpurea (L.) Roth), горошек душистый (Lathyrus edoratus L.), настурция (Tropacolum peregrinum L.) и фасоль огненно-красная (Phaseolus coccineus). Большинство (70%) из них произрастают в местах ограниченного пользования. Изученные виды лиан в исследуемых регионах достигают средних природных показателей (при наличии надлежащего ухода), обладают хорошими показателями жизненного состояния, обильно цветут и плодоносят. При воздействии токсикантами различной концентрации на листовые пластинки лиан установлено их степень устойчивости. Выявлено, что однолетние лианы лучше использовать в декоративных целях, а не в санитарно-гигиенических. Сравнительная оценка однолетних видов с многолетними лианами (девичий виноград пятилисточковый и клематис тангутский) показывает устойчивость многолетних видов (в среднем на 3 балла - 40%). Разработаны варианты декоративных композиций с участием травянистых лиан. По степени декоративности выделены однолетние лианы – Ipomea tricolor, I. purpurea (37 – 41 балл), средней степенью отличаются – Lathyrus edoratus (33 балла), Tropacolum peregrinum (30 баллов) и Phaseolus coccineus (20 – 27 баллов). Преимущество многолетних лиан заключается в их устойчивости к резким изменениям климатических условий (на 40 %) по сравнению с однолетними формами. Поэтому они более предпочтительны для озеленения городской среды. Для усиления декоративного эффекта в сезонном аспекте рекомендуются сочетать расширение видового и формового разнообразия растений (многолетние и однолетние лианы, древесно-кустарниковая, цветочная растительность). Установлено, что природно-климатические условия зоны степи и лесостепи в пределах Саратовской области являются достаточно благоприятными для нормального роста и развития древесно-кустарниковой растительности, в том числе травянистых лиан. Таким образом, обоснованное применение древесных лиан в комплексе с традиционными видами насаждений позволит создать комфортные условия проживания населения, регулировать оптимальный температурный баланс и создавать благоприятные микроклиматические условия. Vertical gardening with different types of vines in modern conditions is important aesthetic and sanitary-hygienic value. It is especially important to address the issues of enrichment of the flora of urban areas with vines in the steppe regions due to poor species composition and a sharp deterioration of the ecological situation. The objects of research were 7 species of lianas, various life forms (annual, perennial), growing in the settlements of the Saratov region (Atkarsk, Saratov). The aim of the research is to study the ecological and biological features and reclamation properties of vines and identify the prospects for their use in vertical gardening residential areas of the Saratov region. In the study, species composition was the most popular species of annual vines: morning glory red-blue (Ipomea tricolor (L.) Roth) and purple morning glory (Ipomea purpurea (L.) Roth), the fragrant pea (Lathyrus edoratus L.), nasturtium (Tropacolum peregrinum L.) and runner beans (Phaseolus coccineus). Most (70%) of them grow in restricted areas. Studied species of vines in the study regions reach average natural performance (with proper care), have good indicators of vital condition, bloom abundantly and bear fruit. When exposed to toxicants of different concentrations on the leaf blades of vines established their degree of stability. It was revealed that the annual vines are better used for decorative purposes, and not in the sanitary-hygienic. A comparative assessment of annual species with perennial vines (maiden grapes and clematis Tangut) shows the stability of perennial species (an average of 3 points-40%). The options and decorative compositions with the participation of herbaceous vines. According to the degree of decoration of the allocated annual vine – Ipomea tricolor, I. purpurea (37 – 41 points), the average degree of differ – Lathyrus edoratus (33 points), Tropacolum peregrinum (30 points) and Phaseolus coccineus (20 to 27 points). The advantage of perennial vines is their resistance to sudden changes in climatic conditions (40 %) compared to annual forms. Therefore, they are more preferable for greening the urban environment. To enhance the decorative effect in the seasonal aspect, it is recommended to combine the expansion of species and form diversity of plants (perennial and annual lianas, tree and shrub, floral vegetation). It is established that the climatic conditions of the steppe and forest-steppe zone within the Saratov region are quite favorable for the normal growth and development of tree and shrub vegetation, including herbaceous lianas. Thus, the reasonable use of wood vines in combination with traditional types of plantings will create comfortable living conditions for the population, regulate the optimal temperature balance and create favorable microclimatic conditions.


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