scholarly journals Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES

2014 ◽  
Vol 14 (2) ◽  
pp. 2043-2085 ◽  
Author(s):  
A. Setyan ◽  
C. Song ◽  
M. Merkel ◽  
W. B. Knighton ◽  
T. B. Onasch ◽  
...  
Keyword(s):  
Sierra Nevada ◽  
Bulk Composition ◽  
Particle Growth ◽  
Climate Impacts ◽  
Oxidation Products ◽  
Rural Site ◽  
Urban Site ◽  
Biogenic Emissions ◽  
Urban Plumes ◽  
New Particles

Abstract. Regional new particle formation and growth events (NPE) were observed on most days over the Sacramento and western Sierra Foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPE usually occurred in the morning with the appearance of an ultrafine mode centered at ~15 nm (in mobility diameter, Dm, measured by a scanning mobility particle sizer operating in the range 10–858 nm) followed by the growth of this mode to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h−1) than at T1 (6.2 ± 2.5 nm h−1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPE was very similar to that of anthropogenically-influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NOx, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOC and the biogenically-influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPE over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implication for quantifying the climate impacts of NPE on global scale.

scholarly journals Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES

2014 ◽  
Vol 14 (13) ◽  
pp. 6477-6494 ◽  
Author(s):  
A. Setyan ◽  
C. Song ◽  
M. Merkel ◽  
W. B. Knighton ◽  
T. B. Onasch ◽  
...  
Keyword(s):  
Sierra Nevada ◽  
Bulk Composition ◽  
Particle Growth ◽  
Climate Impacts ◽  
Oxidation Products ◽  
Rural Site ◽  
Urban Site ◽  
Biogenic Emissions ◽  
Urban Plumes ◽  
New Particles

Abstract. Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, Dm, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h−1) than at T1 (6.2 ± 2.5 nm h−1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NOx, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.

scholarly journals Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES

2012 ◽  
Vol 12 (17) ◽  
pp. 8131-8156 ◽  
Author(s):  
A. Setyan ◽  
Q. Zhang ◽  
M. Merkel ◽  
W. B. Knighton ◽  
Y. Sun ◽  
...  
Keyword(s):  
High Resolution ◽  
Sierra Nevada ◽  
Oxidation Products ◽  
Biogenic Emissions ◽  
Anthropogenic Emissions ◽  
Mass Loading ◽  
Large Variability ◽  
Air Masses ◽  
Aerosol Mass ◽  
Urban Plumes

Abstract. An Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed during the Carbonaceous Aerosols and Radiative Effects Study (CARES) that took place in northern California in June 2010. We present results obtained at Cool (denoted as the T1 site of the project) in the foothills of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. During this study, the average mass loading of submicrometer particles (PM1) was 3.0 μg m−3, dominated by organics (80%) and sulfate (9.9%). The organic aerosol (OA) had a nominal formula of C1H1.38N0.004OM0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two distinct oxygenated OA factors were identified via Positive matrix factorization (PMF) of the high-resolution mass spectra of organics. The more oxidized MO-OOA (O/C = 0.54) was interpreted as a surrogate for secondary OA (SOA) influenced by biogenic emissions whereas the less oxidized LO-OOA (O/C = 0.42) was found to represent SOA formed in photochemically processed urban emissions. LO-OOA correlated strongly with ozone and MO-OOA correlated well with two 1st generation isoprene oxidation products (methacrolein and methyl vinyl ketone), indicating that both SOAs were relatively fresh. A hydrocarbon like OA (HOA) factor was also identified, representing primary emissions mainly due to local traffic. On average, SOA (= MO-OOA + LO-OOA) accounted for 91% of the total OA mass and 72% of the PM1 mass observed at Cool. Twenty three periods of urban plumes from T0 (Sacramento) to T1 (Cool) were identified using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). The average PM1 mass loading was considerably higher in urban plumes than in air masses dominated by biogenic SOA. The change in OA mass relative to CO (ΔOA/ΔCO) varied in the range of 5-196 μg m−3 ppm−1, reflecting large variability in SOA production. The highest ΔOA/ΔCO was reached when air masses were dominated by anthropogenic emissions in the presence of a high concentration of biogenic volatile organic compounds (BVOCs). This ratio, which was 97 μg m−3 ppm−1 on average, was much higher than when urban plumes arrived in a low BVOC environment (~36 μg m−3 ppm−1) or during other periods dominated by biogenic SOA (35 μg m−3 ppm−1). These results demonstrate that SOA formation is enhanced when anthropogenic emissions interact with biogenic precursors.

scholarly journals Photochemical modeling of glyoxal at a rural site: observations and analysis from BEARPEX 2007

2011 ◽  
Vol 11 (17) ◽  
pp. 8883-8897 ◽  
Author(s):  
A. J. Huisman ◽  
J. R. Hottle ◽  
M. M. Galloway ◽  
J. P. DiGangi ◽  
K. L. Coens ◽  
...  
Keyword(s):  
High Temperature ◽  
Sierra Nevada ◽  
Ponderosa Pine ◽  
Oxidation Products ◽  
Chemical Mechanism ◽  
Rural Site ◽  
High Time Resolution ◽  
Mixing Ratios ◽  
Dry Conditions ◽  
Oxidation Chemistry

Abstract. We present roughly one month of high time-resolution, direct, in situ measurements of gas-phase glyoxal acquired during the BEARPEX 2007 field campaign. The research site, located on a ponderosa pine plantation in the Sierra Nevada mountains, is strongly influenced by biogenic volatile organic compounds (BVOCs); thus this data adds to the few existing measurements of glyoxal in BVOC-dominated areas. The short lifetime of glyoxal of ~1 h, the fact that glyoxal mixing ratios are much higher during high temperature periods, and the results of a photochemical model demonstrate that glyoxal is strongly influenced by BVOC precursors during high temperature periods. A zero-dimensional box model using near-explicit chemistry from the Leeds Master Chemical Mechanism v3.1 was used to investigate the processes controlling glyoxal chemistry during BEARPEX 2007. The model showed that MBO is the most important glyoxal precursor (~67 %), followed by isoprene (~26 %) and methylchavicol (~6 %), a precursor previously not commonly considered for glyoxal production. The model calculated a noon lifetime for glyoxal of ~0.9 h, making glyoxal well suited as a local tracer of VOC oxidation in a forested rural environment; however, the modeled glyoxal mixing ratios over-predicted measured glyoxal by a factor 2 to 5. Loss of glyoxal to aerosol was not found to be significant, likely as a result of the very dry conditions, and could not explain the over-prediction. Although several parameters, such as an approximation for advection, were found to improve the model measurement discrepancy, reduction in OH was by far the most effective. Reducing model OH concentrations to half the measured values decreased the glyoxal over-prediction from a factor of 2.4 to 1.1, as well as the overprediction of HO2 from a factor of 1.64 to 1.14. Our analysis has shown that glyoxal is particularly sensitive to OH concentration compared to other BVOC oxidation products. This relationship arises from (i) the predominantly secondary- or higher-generation production of glyoxal from (mainly OH-driven, rather than O3-driven) BVOC oxidation at this site and (ii) the relative importance of photolysis in glyoxal loss as compared to reaction with OH. We propose that glyoxal is a useful tracer for OH-driven BVOC oxidation chemistry.

scholarly journals Salt Intake in Nigeria: a nationwide population survey

2020 ◽  
Vol 41 (Supplement_2) ◽  
Author(s):  
A.N Odili ◽  
B.S Chori ◽  
B Danladi ◽  
P.C Nwakile ◽  
J.O Ogedengbe ◽  
...  
Keyword(s):  
Salt Intake ◽  
Sodium Intake ◽  
Population Analysis ◽  
Cost Effective ◽  
Rural Site ◽  
Urban Site ◽  
Funding Source ◽  
Salt Reduction ◽  
High Salt Intake ◽  
The Impact

Abstract Background Population wide salt reduction programmes are cost effective strategies for control of cardiovascular diseases (CVDs). Obtaining a nationwide salt consumption data in a multi-cultural setting as Nigeria's is key for proper implementation and monitoring of such strategy. Methods We measured sodium in 24-hour urine of free-living adult Nigerians selected from an urban and a rural site each from the 6 geopolitical zones of Nigeria to evaluate patterns of salt intake and its associations with blood pressures (BP). Results Across the 12 sites, sodium intake ranged from 97.9 in the rural South-South to 210 mmol/day in the urban site of the same zone. Overall, the median (IQR) daily sodium intake was 143.5 (97.8) mmol; with higher (p=0.0028) levels among the urban 149.7 (113.8) compared to the rural 133.1 (105.2) dwellers. Overall, 20% of the subjects consumed less than the recommended 2g (86mmol) of sodium daily. After adjustment for age, sex and BMI; sodium intake and BP (systolic and diastolic) were positively associated in 8 out of the 12 sites; significantly so in 2 (p<0.05) for systolic. Within population analysis; which included 973 individuals, increasing sodium intake tended (not significantly) to increase SBP but decrease DBP. However, among subjects whose sodium intake was in excess of 257mmol/day, a 100 mmol/day increase in sodium intake was significantly (p=0.04) associated with a 3.3 mmHg increase in SBP. Conclusion Salt intake among Nigerians is higher than the recommended. The impact of sodium intake on BP appears to be evident only among individuals with high salt intake. Funding Acknowledgement Type of funding source: Foundation. Main funding source(s): Wellcome Trust

scholarly journals A cross-sectional study measuring contact patterns using diaries in an urban and a rural community in South Africa, 2018

2021 ◽  
Vol 21 (1) ◽  
Author(s):  
Jackie Kleynhans ◽  
Stefano Tempia ◽  
Meredith L. McMorrow ◽  
Anne von Gottberg ◽  
Neil A. Martinson ◽  
...  
Keyword(s):  
South Africa ◽  
Age Groups ◽  
Cross Sectional Study ◽  
Rural Site ◽  
Urban Site ◽  
Contact Rate ◽  
Sectional Study ◽  
Cross Sectional ◽  
Contact Rates ◽  
Contact Patterns

Abstract Background Describing contact patterns is crucial to understanding infectious disease transmission dynamics and guiding targeted transmission mitigation interventions. Data on contact patterns in Africa, especially South Africa, are limited. We measured and compared contact patterns in a rural and urban community, South Africa. We assessed participant and contact characteristics associated with differences in contact rates. Methods We conducted a cross-sectional study nested in a prospective household cohort study. We interviewed participants to collect information on persons in contact with for one day. We described self-reported contact rates as median number people contacted per day, assessed differences in contact rates based on participant characteristics using quantile regression, and used a Poisson model to assess differences in contact rates based on contact characteristics within age groups. We also calculated cumulative person hours in contact within age groups at different locations. Results We conducted 535 interviews (269 rural, 266 urban), with 17,252 contacts reported. The overall contact rate was 14 (interquartile range (IQR) 9–33) contacts per day. Those ≤18 years had higher contact rates at the rural site (coefficient 17, 95% confidence interval (95%CI) 10–23) compared to the urban site, for those aged 14–18 years (13, 95%CI 3–23) compared to < 7 years. No differences were observed for adults. There was a strong age-based mixing, with age groups interacting more with similar age groups, but also interaction of participants of all ages with adults. Children aged 14–18 years had the highest cumulative person hours in contact (116.3 rural and 76.4 urban). Conclusions Age played an important role in the number and duration of contact events, with children at the rural site having almost double the contact rate compared to the urban site. These contact rates can be utilized in mathematical models to assess transmission dynamics of infectious diseases in similar communities.

scholarly journals Spatial and seasonal variability of PM<sub>2.5</sub> acidity at two Chinese megacities: insights into the formation of secondary inorganic aerosols

2012 ◽  
Vol 12 (3) ◽  
pp. 1377-1395 ◽  
Author(s):  
K. He ◽  
Q. Zhao ◽  
Y. Ma ◽  
F. Duan ◽  
F. Yang ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Temporal Variations ◽  
Early Summer ◽  
Heterogeneous Reactions ◽  
Rural Site ◽  
Urban Site ◽  
Simultaneous Increase ◽  
Northwestern Pacific ◽  
Inorganic Aerosols ◽  
Aerosol Acidity

Abstract. Aerosol acidity is one of the most important parameters influencing atmospheric chemistry and physics. Based on continuous field observations from January 2005 to May 2006 and thermodynamic modeling, we investigated the spatial and seasonal variations in PM2.5 acidity in two megacities in China, Beijing and Chongqing. Spatially, PM2.5 was generally more acidic in Chongqing than in Beijing, but a reverse spatial pattern was found within the two cities, with more acidic PM2.5 at the urban site in Beijing whereas the rural site in Chongqing. Ionic compositions of PM2.5 revealed that it was the higher concentrations of NO3− at the urban site in Beijing and the lower concentrations of Ca2+ within the rural site in Chongqing that made their PM2.5 more acidic. Temporally, PM2.5 was more acidic in summer and fall than in winter, while in the spring of 2006, the acidity of PM2.5 was higher in Beijing but lower in Chongqing than that in 2005. These were attributed to the more efficient formation of nitrate relative to sulfate as a result of the influence of Asian desert dust in 2006 in Beijing and the greater wet deposition of ammonium compared to sulfate and nitrate in 2005 in Chongqing. Furthermore, simultaneous increase of PM2.5 acidity was observed from spring to early summer of 2005 in both cities. This synoptic-scale evolution of PM2.5 acidity was accompanied by the changes in air masses origins, which were influenced by the movements of a subtropical high over the northwestern Pacific in early summer. Finally, the correlations between [NO3−]/[SO42−] and [NH4+]/[SO42−] suggests that under conditions of high aerosol acidity, heterogeneous reactions became one of the major pathways for the formation of nitrate at both cities. These findings provided new insights in our understanding of the spatial and temporal variations in aerosol acidity in Beijing and Chongqing, as well as those reported in other cities in China.

scholarly journals Impact of rural versus urban setting on kidney markers: a cross-sectional study in South-Kivu, DRCongo

2021 ◽  
Vol 22 (1) ◽  
Author(s):  
Mannix Imani Masimango ◽  
Michel P. Hermans ◽  
Espoir Bwenge Malembaka ◽  
Pierre Wallemacq ◽  
Ernest Kiswaya Sumaili ◽  
...  
Keyword(s):  
Positive Predictive Value ◽  
Negative Predictive Value ◽  
Predictive Value ◽  
Democratic Republic Of Congo ◽  
Urban Setting ◽  
Sub Saharan Africa ◽  
Rural Site ◽  
Urban Site ◽  
Cross Sectional ◽  
South Kivu

Abstract Background Most studies of chronic kidney disease (CKD) in Sub-Saharan Africa (SSA) have been conducted in urban settings. They relied on GFR estimated from serum creatinine alone and on the inexpensive, convenient urinary dipstick to assess proteinuria. The dipstick for proteinuria has not been directly compared with the gold standard albumin-to-creatinine ratio (ACR) in a large-sized study in SSA. We hereby assessed the influence of rural versus urban location on the level, interpretation, and diagnostic performance of proteinuria dipstick versus ACR. Methods In a cross-sectional population-based study of CKD in both urban (n = 587) and rural (n = 730) settings in South-Kivu, Democratic Republic of Congo (DRC), we assessed the prevalence, performance (sensitivity, specificity, positive predictive value and negative predictive value) and determinants of a positive dipstick proteinuria as compared with albuminuria (ACR). Albuminuria was subdivided into: A1 (< 30 mg/g creatinine), A2 (30 to 299 mg/g creatinine) and A3 (≥ 300 mg/g creatinine). Results The overall prevalence of positive dipstick proteinuria (≥ 1+) was 9.6 % (95 % CI, 7.9–11.3) and was higher in rural than in urban residents (13.1 % vs. 4.8 %, p < 0.001), whereas the prevalence of albuminuria (A2 or A3) was similar in both sites (6 % rural vs. 7.6 % urban, p = 0.31). In both sites, dipstick proteinuria ≥ 1 + had a poor sensitivity (< 50 %) and positive predictive value (< 11 %) for the detection of A2 or A3. The negative predictive value was 95 %. Diabetes [aOR 6.12 (1.52–24.53)] was a significant predictor of A3 whereas alkaline [aOR 7.45 (3.28–16.93)] and diluted urine [aOR 2.19 (1.35–3.57)] were the main predictors of positive dipstick proteinuria. Conclusions ACR and dipstick proteinuria have similar positivity rates in the urban site whereas, in the rural site, dipstick was 2-fold more often positive than ACR. The poor sensitivity and positive predictive value of the dipstick as compared with ACR makes it unattractive as a screening tool in community studies of CKD in SSA.

scholarly journals Triple oxygen isotopes indicate urbanization affects sources of nitrate in wet and dry atmospheric deposition

2018 ◽  
Author(s):  
David M. Nelson ◽  
Urumu Tsunogai ◽  
Ding Dong ◽  
Takuya Ohyama ◽  
Daisuke D. Komatsu ◽  
...  
Keyword(s):  
Dry Deposition ◽  
Wet Deposition ◽  
Urban Environments ◽  
Rural Site ◽  
Urban Site ◽  
Peroxy Radicals ◽  
Long Distance ◽  
Wet And Dry Deposition ◽  
Atmospheric Nitrate ◽  
Nitrate Deposition

Abstract. Atmospheric nitrate deposition resulting from anthropogenic activities negatively affects human and environmental health. Identifying deposited nitrate that is produced locally vs. that originating from long-distance transport would help inform efforts to mitigate such impacts. However, distinguishing the relative transport distances of atmospheric nitrate in urban areas remains a major challenge since it may be produced locally and/or come from upwind regions. To address this uncertainty we assessed spatiotemporal variation in monthly weighted-average Δ17O and δ15N values of wet and dry nitrate deposition during one year at urban and rural sites along the western coast of the northern Japanese island of Hokkaido, downwind of the East Asian continent. Δ17O values of nitrate in wet deposition at the urban site mirrored those of wet and dry deposition at the rural site, ranging between ~ +22 and +30 ‰ with higher values during winter and lower values in summer, which suggests greater relative importance of oxidation of NO2 by O3 during winter and OH during summer. In contrast, Δ17O values of nitrate in dry deposition at the urban site were lower (+19–+25 ‰) and displayed less distinct seasonal variation. Furthermore, the difference between δ15N values of nitrate in wet and dry nitrate deposition was, on average, 3 ‰ greater at the urban than rural site, and Δ17O and δ15N values were correlated for both forms of deposition at both sites with the exception of dry deposition at the urban site. These results suggest that, relative to nitrate in wet deposition in urban environments and wet and dry deposition in rural environments, nitrate in dry deposition in urban environments forms from relatively greater oxidation of NO by peroxy radicals and/or oxidation of NO2 by OH. Given greater concentrations of peroxy radicals and OH in cities, these results imply that dry nitrate deposition results from local NOx emissions more so than wet deposition, which is transported longer distances. These results illustrate the value of stable isotope data for distinguishing the transport distances and reaction pathways of atmospheric nitrate pollution.

scholarly journals Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

2016 ◽  
Vol 16 (2) ◽  
pp. 1139-1160 ◽  
Author(s):  
L. Xu ◽  
L. R. Williams ◽  
D. E. Young ◽  
J. D. Allan ◽  
H. Coe ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Solid Fuel ◽  
Field Studies ◽  
Rural Site ◽  
Urban Site ◽  
High Temporal Resolution ◽  
Volatile Organics ◽  
Aerosol Mass ◽  
Rural And Urban ◽  
Wide Range

Abstract. The composition of PM1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.

scholarly journals Measurements of higher alkanes using NO<sup>+</sup> chemical ionization in PTR-ToF-MS: important contributions of higher alkanes to secondary organic aerosols in China

2020 ◽  
Vol 20 (22) ◽  
pp. 14123-14138
Author(s):  
Chaomin Wang ◽  
Bin Yuan ◽  
Caihong Wu ◽  
Sihang Wang ◽  
Jipeng Qi ◽  
...  
Keyword(s):  
Chemical Ionization ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Proton Transfer Reaction ◽  
Rural Site ◽  
Urban Site ◽  
Accurate Estimation ◽  
High Time Resolution ◽  
The North ◽  
Tof Ms

Abstract. Higher alkanes are a major class of intermediate-volatility organic compounds (IVOCs), which have been proposed to be important precursors of secondary organic aerosols (SOA) in the atmosphere. Accurate estimation of SOA from higher alkanes and their oxidation processes in the atmosphere is limited, partially due to the difficulty of their measurement. High-time-resolution (10 s) measurements of higher alkanes were performed using NO+ chemical ionization in proton transfer reaction time-of-flight mass spectrometry (NO+ PTR-ToF-MS) at an urban site in Guangzhou in the Pearl River Delta (PRD) and at a rural site in the North China Plain (NCP). High concentrations were observed in both environments, with significant diurnal variations. At both sites, SOA production from higher alkanes is estimated from their photochemical losses and SOA yields. Higher alkanes account for significant fractions of SOA formation at the two sites, with average contributions of 7.0 % ± 8.0 % in Guangzhou and 9.4 % ± 9.1 % in NCP, which are comparable to or even higher than both single-ring aromatics and naphthalenes. The significant contributions of higher alkanes to SOA formation suggests that they should be explicitly included in current models for SOA formation. Our work also highlights the importance of NO+ PTR-ToF-MS in measuring higher alkanes and quantifying their contributions to SOA formation.

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