scholarly journals Particulate matter (PM) episodes at a suburban site in Hong Kong: evolution of PM characteristics and role of photochemistry in secondary aerosol formation

2016 ◽  
Author(s):  
Yi Ming Qin ◽  
Yong Jie Li ◽  
Hao Wang ◽  
Berto Paul Yok Long Lee ◽  
Dan Dan Huang ◽  
...  

Abstract. Episodes with high concentrations of particulate matter (PM) across the seasons were investigated during four one-month campaigns at a suburban site in Hong Kong. High-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurements revealed that both regional transport and secondary formation contributed to high PM levels during the episodes at this site. Based on distinct meteorological conditions, episodes were categorized into three types: liquid water content (LWC), solar irradiance (IR), and long-range transport (LRT). Despite the difference in meteorological conditions, all episodes were characterized by a high fraction of sulfate (45 %–56 %) and organics (23 %–34 %). However, aerosols in LWC episodes were less aged, consisting of the lowest fraction of secondary organics aerosols (SOA) and the highest fraction of small particles. Large particles mixed internally while freshly formed small particles mixed externally in LWC episodes. Aerosols in LRT episodes, by contrast, were the most aged and consisted of the highest proportion of low-volatility oxygenated organic aerosols (LVOOA) and the lowest proportion of small particles. Both small and large particles mixed externally in LRT episodes. The highest proportion of semi-volatile oxygenated organic aerosols (SVOOA) and a medium proportion of small particles were observed in IR episodes. Both small and large particles were likely externally mixed during IR episodes. Unlike in the other two types of episodes, in IR episodes aerosols experienced the most dramatic size increase and diurnal variation, with a time lag between SVOOA and LVOOA and a gradual increase in carbon oxidation state (OSc ≈ 2 × O : C – H : C). Five out of ten episodes were of the IR type, further reflecting the importance of this type of episode. The evolution of aerosol components in one particular episode of the IR type, which exhibited a clear land-sea breeze pattern, was examined in detail. Sulfate and SOA due to photochemical aging were very efficiently produced during the course of six hours. The “fresh” SOA (SVOOA) was initially formed at a higher rate than the “aged” SOA (LVOOA). The SVOOA transformed to LVOOA at the later stage of photochemical aging. This tranformation was further supported by mass spectral analysis, which showed an increase in the most oxidized ion (CO2+) and decreases in moderately oxidized ones (C2H3O+, C3H3O+ and C3H5O+). By measuring the physical and chemical properties of PM in a highly time-resolved manner, the current study was able to demonstrate the dynamic and complex nature of PM transformation during high-PM episodes.

2016 ◽  
Vol 16 (22) ◽  
pp. 14131-14145 ◽  
Author(s):  
Yi Ming Qin ◽  
Yong Jie Li ◽  
Hao Wang ◽  
Berto Paul Yok Long Lee ◽  
Dan Dan Huang ◽  
...  

Abstract. Episodes with high concentrations of particulate matter (PM) across the seasons were investigated during four 1-month campaigns at a suburban site in Hong Kong. High-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurements revealed that both regional transport and secondary formation contributed to high PM levels during the episodes at this site. Based on distinct meteorological conditions, episodes were categorized into three types: liquid water content (LWC), solar irradiance (IR), and long-range transport (LRT). Despite the difference in meteorological conditions, all episodes were characterized by a high fraction of sulfate (45–56 %) and organics (23–34 %). However, aerosols in LWC episodes were less aged, consisting of the lowest fraction of secondary organic aerosol (SOA) and the highest fraction of small particles. Large particles mixed internally while freshly formed small particles mixed externally in LWC episodes. Aerosols in LRT episodes, by contrast, were the most aged and consisted of the highest proportion of low-volatility oxygenated organic aerosol (LVOOA) and the lowest proportion of small particles. Both small and large particles mixed externally in LRT episodes. The highest proportion of semi-volatile oxygenated organic aerosol (SVOOA) and a medium proportion of small particles were observed in IR episodes. Both small and large particles were likely externally mixed during IR episodes. Furthermore, aerosols experienced the most dramatic size increase and diurnal variation, with a time lag between SVOOA and LVOOA and a gradual increase in carbon oxidation state (OSc ≈ 2 × O : C − H : C). Five out of 10 episodes were of the IR type, further reflecting the importance of this type of episode. The evolution of aerosol components in one particular episode of the IR type, which exhibited a clear land–sea breeze pattern, was examined in detail. Sulfate and SOA due to photochemical aging were very efficiently produced during the course of 6 h. The “less-oxidized” SOA (SVOOA) was initially formed at a higher rate than the “more-oxidized” SOA (LVOOA). The SVOOA transformed to LVOOA at the later stage of photochemical aging. This transformation was further supported by mass spectral analysis, which showed an increase in the most oxidized ion (CO2+) and decreases in moderately oxidized ones (C2H3O+, C3H3O+ and C3H5O+). By measuring the physical and chemical properties of PM in a highly time-resolved manner, the current study was able to demonstrate the dynamic and complex nature of PM transformation during high-PM episodes.


2015 ◽  
Vol 15 (23) ◽  
pp. 35057-35115 ◽  
Author(s):  
D. E. Young ◽  
H. Kim ◽  
C. Parworth ◽  
S. Zhou ◽  
X. Zhang ◽  
...  

Abstract. The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. During January and February 2013, a ground supersite was installed at the Fresno-Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Ionicon Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 μg m−3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi-volatile oxygenated OA (SV-OOA; 16 % of total OA; O / C = 0.63) and low volatility oxygenated OA (LV-OOA; 24 % of total OA; O / C = 0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a previous wintertime campaign (winter 2010), most notably that PM1 concentrations were nearly three times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 to 12:00 PST. This is an indication that nighttime chemistry might also be higher in 2013. As solar radiation was stronger in 2013 the higher nitrate and OOA concentrations in 2013 could also be partly due to greater photochemical production of secondary aerosol species. The greater solar radiation and larger range in temperature in 2013 also likely led to both SV-OOA and LV-OOA being observed in 2013 whereas only a single OOA factor was identified in 2010.


1985 ◽  
Vol 36 (6) ◽  
pp. 819 ◽  
Author(s):  
PM Kennedy

Two Hereford steers, fitted with cannulas in the oesophagus and rumen, were given four forage diets in either the chopped or ground and pelleted form. Collections from the oesophageal fistula were made of boluses regurgitated during rumination of the chopped diets. Diets were given at 95% of voluntary feed consumption at intervals of 2 h. Rumination of the chopped diets required 28-36000 chews/day compared to values of 3-10 000 chews/day for the pelleted forms. The weight of material regurgitated during rumination averaged 786 g, of which 493 g was swallowed before chewing commenced. Fractionation of particulate DM by wet sieving showed that the material retained in the mouth for chewing contained 41% more large particulate matter than did regurgitated material. Approximately 70% of large particles in the mouth were comminuted to small particles during one cycle of rumination. Comminution per chew was positively related to the amount of large particulate matter retained in the mouth for chewing and negatively to the number of chews/cycle. Rumination accounted for approximately 85% of comminution of large particles which entered the rumen. Measurements of digestion of dietary materials from nylon bags and rates of outflow of small particles and water from the rumen were used in conjunction with intake and chewing measurements to predict the rumen content of large particles.


2019 ◽  
Author(s):  
Christopher Y. Lim ◽  
David H. Hagan ◽  
Matthew M. Coggon ◽  
Abigail R. Koss ◽  
Kanako Sekimoto ◽  
...  

Abstract. Biomass burning is an important source of aerosol and trace gases to the atmosphere, but how these emissions change chemically during their lifetimes is not fully understood. As part of the Fire Influence on Regional and Global Environments Experiment (FIREX 2016), we investigated the effect of photochemical aging on biomass burning organic aerosol (BBOA), with a focus on fuels from the western United States. Emissions were sampled into a small (150 L) environmental chamber and photochemically aged via the addition of ozone and irradiation by 254 nm light. While some fraction of species undergoes photolysis, the vast majority of aging occurs via reaction with OH radicals, with total OH exposures corresponding to the equivalent of up to 10 days of atmospheric oxidation. For all fuels burned, large and rapid changes are seen in the ensemble chemical composition of BBOA, as measured by an aerosol mass spectrometer (AMS). Secondary organic aerosol (SOA) formation is seen for all aging experiments and continues to grow with increasing OH exposure, but the magnitude of the SOA formation is highly variable between experiments. This variability can be explained well by a combination of experiment-to-experiment differences in OH exposure and the total concentration of non-methane organic gases (NMOGs) in the chamber before oxidation, measured by PTR-ToF-MS (r2 values from 0.64 to 0.83). From this relationship, we calculate the fraction of carbon from biomass burning NMOGs that is converted to SOA as a function of equivalent atmospheric aging time, with carbon yields ranging from 24 ± 4 % after 6 hours to 56 ± 9 % after 4 days.


Atmosphere ◽  
2021 ◽  
Vol 12 (2) ◽  
pp. 190
Author(s):  
William Hicks ◽  
Sean Beevers ◽  
Anja H. Tremper ◽  
Gregor Stewart ◽  
Max Priestman ◽  
...  

This research quantifies current sources of non-exhaust particulate matter traffic emissions in London using simultaneous, highly time-resolved, atmospheric particulate matter mass and chemical composition measurements. The measurement campaign ran at Marylebone Road (roadside) and Honor Oak Park (background) urban monitoring sites over a 12-month period between 1 September 2019 and 31 August 2020. The measurement data were used to determine the traffic increment (roadside–background) and covered a range of meteorological conditions, seasons, and driving styles, as well as the influence of the COVID-19 “lockdown” on non-exhaust concentrations. Non-exhaust particulate matter (PM)10 concentrations were calculated using chemical tracer scaling factors for brake wear (barium), tyre wear (zinc), and resuspension (silicon) and as average vehicle fleet non-exhaust emission factors, using a CO2 “dilution approach”. The effect of lockdown, which saw a 32% reduction in traffic volume and a 15% increase in average speed on Marylebone Road, resulted in lower PM10 and PM2.5 traffic increments and brake wear concentrations but similar tyre and resuspension concentrations, confirming that factors that determine non-exhaust emissions are complex. Brake wear was found to be the highest average non-exhaust emission source. In addition, results indicate that non-exhaust emission factors were dependent upon speed and road surface wetness conditions. Further statistical analysis incorporating a wider variability in vehicle mix, speeds, and meteorological conditions, as well as advanced source apportionment of the PM measurement data, were undertaken to enhance our understanding of these important vehicle sources.


1989 ◽  
Vol 171 ◽  
Author(s):  
Dale W. Schaefer ◽  
James E. Mark ◽  
David Mccarthy ◽  
Li Jian ◽  
C. -C. Sun ◽  
...  

ABSTRACTThe structure of several classes of silica/siloxane molecular composites is investigated using small-angle x-ray and neutron scattering. These filled elastomers can be prepared through different synthethic protocols leading to a range of fillers including particulates with both rough and smooth surfaces, particulates with dispersed interfaces, and polymeric networks. We also find examples of bicontinuous filler phases that we attribute to phase separation via spinodal decomposition. In-situ kinetic studies of particulate fillers show that the precipitate does not develop by conventional nucleation-and-growth. We see no evidence of growth by ripening whereby large particles grow by consumption of small particles. Rather, there appears to be a limiting size set by the elastomer network itself. Phase separation develops by continuous nucleation of particles and subsequent growth to the limiting size. We also briefly report studies of polymer-toughened glasses. In this case, we find no obvious correlation between organic content and structure.


2015 ◽  
Vol 15 (1) ◽  
pp. 37-53 ◽  
Author(s):  
Y. J. Li ◽  
B. P. Lee ◽  
L. Su ◽  
J. C. H. Fung ◽  
C.K. Chan

Abstract. Atmospheric particulate matter (PM) remains poorly understood due to the lack of comprehensive measurements at high time resolution for tracking its dynamic features and the lack of long-term observation for tracking its seasonal variability. Here, we present highly time-resolved and seasonal compositions and characteristics of non-refractory components in PM with a diameter less than 1 μm (NR-PM1) at a suburban site in Hong Kong. The measurements were made with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) at the Hong Kong University of Science and Technology (HKUST) Air Quality Research Supersite for 4 months, with one in each season of the year. The average NR-PM1 concentration of ~ 15 μg m−3 is higher than those AMS measurements made in South Korea and Japan, but lower than those in North China, the Yangtze River Delta and the nearby Pearl River Delta. The seasonal dependence of the total NR-PM1 monthly averaged concentrations was small, but that of the fractions of the species in NR-PM1 was significant. Site characteristic plays an important role in the relative fractions of species in NR-PM1 and our results are generally consistent with measurements at other non-urban sites in this regard. Detailed analyses were conducted on the AMS data in the aspects of (1) species concentrations, (2) size distributions, (3) degree of oxygenation of organics, and (4) positive matrix factorization (PMF)-resolved organic factors in a seasonal context, as well as with air mass origin from back-trajectory analysis. Sulfate had the highest fraction in NR-PM1 (> 40%), and the surrogates of secondary organic species – semi-volatile oxygenated organic aerosol (SVOOA) and low-volatility oxygenated organic aerosol (LVOOA) – prevailed (~ 80%) in the organic portion of NR-PM1. Local contributions to the organic portion of NR-PM1 at this suburban site was strongly dependent on season. The hydrocarbon-like organic aerosol (HOA) factor related to local traffic emissions contributed > 10% to organic aerosols in spring and summer but only 6–7% in autumn and winter. The cooking organic aerosol (COA) factor contributed > 10% to organic aerosols in winter. With the aid of highly time-resolved data, diurnal patterns of the degree of oxygenation of organic aerosols were used to determine the sources and formation processes of the least understood organic portion of PM. The oxygen-to-carbon atomic ratio (O : C) and average carbon oxidation state OS C) showed little variation in autumn and winter, when the long-range transport of oxidized organics dominated, whereas they peaked in the afternoon in spring and summer, when locally produced secondary organic aerosol prevailed. Air mass origin, in contrast, had a strong influence on both NR-PM1 concentrations and the fractions of species in NR-PM1. The findings of the current study provide a better understanding of the role of air mass origin in the seasonal characteristics of the PM composition and the relative importance of local vs. transported organic aerosols in this region.


2002 ◽  
Vol 300 (1-3) ◽  
pp. 59-67 ◽  
Author(s):  
K.F Ho ◽  
S.C Lee ◽  
Jimmy C Yu ◽  
S.C Zou ◽  
Kochy Fung

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