scholarly journals A new pseudodeterministic multivariate receptor model for individual source apportionment using highly time-resolved ambient concentration measurements

Author(s):  
Seung Shik Park
2019 ◽  
Author(s):  
Yunjiang Zhang ◽  
Olivier Favez ◽  
Jean-Eudes Petit ◽  
Francesco Canonaco ◽  
Francois Truong ◽  
...  

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly-time resolved year-round characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of Aerosol Chemical Speciation Monitor (ACSM) and multi-wavelength aethalometer from November 2011 to March 2018 at a background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase of LO-OOA concentrations and contributions (50–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely high concentrations and OA contributions (32–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter, and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about 200 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil fuel and biomass burning black carbon components), and no trend for LO-OOA over the 6+-year investigated period.


2013 ◽  
Vol 13 (10) ◽  
pp. 26657-26698
Author(s):  
Y. Hu ◽  
S. Balachandran ◽  
J. E. Pachon ◽  
J. Baek ◽  
C. Ivey ◽  
...  

Abstract. A hybrid fine particulate matter (PM2.5) source apportionment approach based on a receptor-model (RM) species balance and species specific source impacts from a chemical transport model (CTM) equipped with a sensitivity analysis tool is developed to provide physically- and chemically-consistent relationships between source emissions and receptor impacts. This hybrid approach enhances RM results by providing initial estimates of source impacts from a much larger number of sources than are typically used in RMs, and provides source-receptor relationships for secondary species. Further, the method addresses issues of source collinearities, and accounts for emissions uncertainties. Hybrid method results also provide information on the resulting source impact uncertainties. We apply this hybrid approach to conduct PM2.5 source apportionment at Chemical Speciation Network (CSN) sites across the US. Ambient PM2.5 concentrations at these receptor sites were apportioned to 33 separate sources. Hybrid method results led to large changes of impacts from CTM estimates for sources such as dust, woodstove, and other biomass burning sources, but limited changes to others. The refinements reduced the differences between CTM-simulated and observed concentrations of individual PM2.5 species by over 98% when using a weighted least squared error minimization. The rankings of source impacts changed from the initial estimates, revealing that CTM-only results should be evaluated with observations. Assessment with RM results at six US locations showed that the hybrid results differ somewhat from commonly resolved sources. The hybrid method also resolved sources that typical RM methods do not capture without extra measurement information on unique tracers. The method can be readily applied to large domains and long (such as multi-annual) time periods to provide source impact estimates for management- and health-related studies.


2019 ◽  
Vol 19 (23) ◽  
pp. 14755-14776 ◽  
Author(s):  
Yunjiang Zhang ◽  
Olivier Favez ◽  
Jean-Eudes Petit ◽  
Francesco Canonaco ◽  
Francois Truong ◽  
...  

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly time-resolved long-term characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of an aerosol chemical speciation monitor (ACSM) and a multiwavelength Aethalometer from November 2011 to March 2018 at a peri-urban background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18 %–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase in LO-OOA concentrations and contributions (50 %–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely, high concentrations and OA contributions (32 %–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about −175 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil-fuel and biomass-burning black carbon components) and no statistically significant trend for LO-OOA over the 6-year investigated period.


2002 ◽  
Author(s):  
Jared E. Campbell ◽  
Richard W. Coppom

Experiments were conducted to better understand the flow physics associated with axial flow mixers in pipes. Specifically, the dependence of the downstream mixing evolution on the velocity ratio of the secondary to primary stream was explored. Experiments were conducted in a 25.4 mm diameter water pipe flow loop (25,700 ≤ RD ≤ 28,500), in which a fluorescein dye was coaxially injected. The injection tube diameter was 1.5 mm. Three velocity ratios, VR = 0.5, 1.0 and 2.0 were explored, where VR = Vjet/Vmain. The present results indicate that the effects of velocity ratio on the mean concentration are primarily evident in the near-field flow downstream of the injector, while concentration variance measurements indicate a primary influence at intermediate axial locations. Analysis of higher order moments and flow visualizations suggest that these influences are associated with the injected flow conditions. Two-dimensional LIF analysis of the coherent jet breakup region showed an instability in this transition related to injector flow Reynolds number. The present concentration measurements do not indicate the exponential variance decay commonly used for modelling mixing in pipes. Far field data exhibit low wavenumber motions as predicted by the recent theory of Guilkey et al. (1997).


2020 ◽  
Vol 20 (2) ◽  
pp. 735-752 ◽  
Author(s):  
Sahil Bhandari ◽  
Shahzad Gani ◽  
Kanan Patel ◽  
Dongyu S. Wang ◽  
Prashant Soni ◽  
...  

Abstract. Delhi, India, is the second most populated city in the world and routinely experiences some of the highest particulate matter concentrations of any megacity on the planet, posing acute challenges to public health (World Health Organization, 2018). However, the current understanding of the sources and dynamics of PM pollution in Delhi is limited. Measurements at the Delhi Aerosol Supersite (DAS) provide long-term chemical characterization of ambient submicron aerosol in Delhi, with near-continuous online measurements of aerosol composition. Here we report on source apportionment based on positive matrix factorization (PMF), conducted on 15 months of highly time-resolved speciated submicron non-refractory PM1 (NR-PM1) between January 2017 and March 2018. We report on seasonal variability across four seasons of 2017 and interannual variability using data from the two winters and springs of 2017 and 2018. We show that a modified tracer-based organic component analysis provides an opportunity for a real-time source apportionment approach for organics in Delhi. Phase equilibrium modeling of aerosols using the extended aerosol inorganics model (E-AIM) predicts equilibrium gas-phase concentrations and allows evaluation of the importance of the ventilation coefficient (VC) and temperature in controlling primary and secondary organic aerosol. We also find that primary aerosol dominates severe air pollution episodes, and secondary aerosol dominates seasonal averages.


2019 ◽  
Author(s):  
Pragati Rai ◽  
Markus Furger ◽  
Jay Slowik ◽  
Francesco Canonaco ◽  
Roman Fröhlich ◽  
...  

Abstract. Trace element measurements in PM10 were performed with 1 h time resolution at a rural freeway site during summer 2015 in Switzerland using the Xact multi-metals monitor. On average the Xact 625 elements (without accounting for oxygen and other associated elements) make up about 20 % of the total PM10 mass (14.6 µg m−3). Subsequently, a source apportionment by positive matrix factorization (PMF) implemented via the Source Finder software (SoFi Pro) was applied. Eight different sources were identified (notable elements in brackets) for PM10: fireworks-I (K, S, Ba, Cl), fireworks-II (K), sea salt (Cl), secondary sulfate (S), background dust (Si, Ti), road dust (Ca), traffic-related (Fe) and industrial (Zn, Pb). The major components were secondary sulfate and traffic-related followed by background dust and road dust factors, explaining 21 %, 20 %, 18 % and 16 % of the analysed PM10 elemental mass, respectively, with the factor mass not corrected for oxygen content. Further, there are minor contributions (on the order of a few percent) of sea salt and industrial sources. The regionally influenced secondary sulfate factor experiences negligible resuspension, and concentrations are similar throughout the day. The significant loads of the traffic-related and road dust factors with strong diurnal variations highlight the continuing importance of vehicle-related air pollutants at this site. Enhanced control of PMF using SoFi Pro allowed for a successful apportionment of transient sources such as the two firework factors and sea salt, which remained mixed when analysed by unconstrained PMF.


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