scholarly journals Precursors and formation of secondary organic aerosols from wildfires in the Euro-Mediterranean region

2018 ◽  
Author(s):  
Marwa Majdi ◽  
Karine Sartelet ◽  
Grazia Maria Lanzafame ◽  
Florian Couvidat ◽  
Youngseob Kim ◽  
...  

Abstract. This work aims at quantifying the relative contribution of secondary organic aerosol (SOA) precursors emitted by wildfires to organic aerosol (OA) formation, during summer 2007 over the Euro-Mediterranean region, where intense wild-fires occurred. A new SOA formation mechanism, H2Oaro, including recently identified aromatic volatile organic compounds (VOCs) emitted from wildfires is developed based on smog chamber experiment measurements, under low and high-NOx regimes. The aromatic VOCs included in the mechanism are toluene, xylene, benzene, phenol, cresol, catechol, furan, naphthalene, methylnaphthalene, syringol, guaiacol and structurally assigned and unassigned compounds with at least 6 carbon atoms per molecule (USC>6). This mechanism H2Oaro is an extension of the H2O (Hydrophilic/Hydrophobic organic) aerosol mechanism: the oxidation of the precursor forms surrogate species with specific thermodynamic properties (volatility, oxidation degree, affinity to water). The SOA concentrations over the Euro-Mediterranean region in summer 2007 are simulated using the chemistry transport model (CTM) Polair3D of the air-quality plateform Polyphemus, where the mechanism H2Oaro was implemented. To estimate the relative contribution of the aromatic VOCs, intermediate, semi and low volatile organic compounds (I/S/L-VOCs) to wildfires OA concentrations, different estimations of the gaseous I/S/L-VOC emissions (from primary organic aerosol (POA) using a factor of 1.5 or from non-methanic organic gas (NMOG) using a factor of 0.36) and their ageing (one-step oxidation vs multi-generational oxidation), are also tested in the CTM.Most of the particle organic aerosol (OA) concentrations are formed from I/S/L-VOCs. In average during the summer 2007 and over the Euro-Mediterranean domain, they are about 10 times higher than the OA concentrations formed from VOCs. However, locally, the OA concentrations formed from VOCs can represent up to 30 % of the OA concentrations from biomass burning. Amongst the VOCs, the main contributors to SOA formation are phenol, benzene and catechol (47 %), USC>6 compounds (23 %), and toluene and xylene (12 %). Sensitivity studies of the influence of the VOCs and the I/S/L-VOCs emissions and chemical ageing mechanisms on PM2.5 concentrations show that surface PM2.5 concentrations are more sensitive to the parameterization used for gaseous I/S/L-VOCs emissions than for ageing. Estimating the gaseous I/S/L-VOCs emissions from POA or from NMOG has a high impact on local surface PM2.5 concentrations (reaching −30 % in Balkans, −8 to −16 % in the fire plume and +8 to +16 % in Greece). Considering the VOC emissions results in a moderate increase of PM2.5 concentrations mainly in Balkans (up to 24 %) and in the fire plume (+10 %).

2019 ◽  
Vol 19 (8) ◽  
pp. 5543-5569 ◽  
Author(s):  
Marwa Majdi ◽  
Karine Sartelet ◽  
Grazia Maria Lanzafame ◽  
Florian Couvidat ◽  
Youngseob Kim ◽  
...  

Abstract. This work aims at quantifying the relative contribution of secondary organic aerosol (SOA) precursors emitted by wildfires to organic aerosol (OA) formation during summer of 2007 over the Euro-Mediterranean region, where intense wildfires occurred. A new SOA formation mechanism, H2Oaro, including recently identified aromatic volatile organic compounds (VOCs) emitted from wildfires, is developed based on smog chamber experiment measurements under low- and high-NOx regimes. The aromatic VOCs included in the mechanism are toluene, xylene, benzene, phenol, cresol, catechol, furan, naphthalene, methylnaphthalene, syringol, guaiacol, and structurally assigned and unassigned compounds with at least six carbon atoms per molecule (USC>6). This mechanism H2Oaro is an extension of the H2O (hydrophilic–hydrophobic organic) aerosol mechanism: the oxidation of the precursor forms surrogate species with specific thermodynamic properties (volatility, oxidation degree and affinity to water). The SOA concentrations over the Euro-Mediterranean region in summer of 2007 are simulated using the chemistry transport model (CTM) Polair3D of the air-quality platform Polyphemus, where the mechanism H2Oaro was implemented. To estimate the relative contribution of the aromatic VOCs, intermediate volatility, semi-volatile and low-volatility organic compounds (I/S/L-VOCs), to wildfires OA concentrations, different estimations of the gaseous I/S/L-VOC emissions (from primary organic aerosol – POA – using a factor of 1.5 or from non-methanic organic gas – NMOG – using a factor of 0.36) and their ageing (one-step oxidation vs. multi-generational oxidation) are also tested in the CTM. Most of the particle OA concentrations are formed from I/S/L-VOCs. On average during the summer of 2007 and over the Euro-Mediterranean domain, they are about 10 times higher than the OA concentrations formed from VOCs. However, locally, the OA concentrations formed from VOCs can represent up to 30 % of the OA concentrations from biomass burning. Amongst the VOCs, the main contributors to SOA formation are phenol, benzene and catechol (CAT; 47 %); USC>6 compounds (23 %); and toluene and xylene (12 %). Sensitivity studies of the influence of the VOCs and the I/S/L-VOC emissions and chemical ageing mechanisms on PM2.5 concentrations show that surface PM2.5 concentrations are more sensitive to the parameterization used for gaseous I/S/L-VOC emissions than for ageing. Estimating the gaseous I/S/L-VOC emissions from POA or from NMOG has a high impact on local surface PM2.5 concentrations (reaching −30 % in the Balkans, −8 % to −16 % in the fire plume and +8 % to +16 % in Greece). Considering the VOC as SOA precursors results in a moderate increase in PM2.5 concentrations mainly in the Balkans (up to 24 %) and in the fire plume (+10 %).


Author(s):  
Hind A. A. Al-Abadleh

Extensive research has been done on the processes that lead to the formation of secondary organic aerosol (SOA) including atmospheric oxidation of volatile organic compounds (VOCs) from biogenic and anthropogenic...


2021 ◽  
Vol 11 (1) ◽  
Author(s):  
M. Y. Song ◽  
H. Chun

AbstractVolatile organic compounds (VOCs) are secondary pollutant precursors having adverse impacts on the environment and human health. Although VOC emissions, their sources, and impacts have been investigated, the focus has been on large-scale industrial sources or indoor environments; studies on relatively small-scale enterprises (e.g., auto-repair workshops) are lacking. Here, we performed field VOC measurements for an auto-repair painting facility in Korea and analyzed the characteristics of VOCs emitted from the main painting workshop (top coat). The total VOC concentration was 5069–8058 ppb, and 24–35 species were detected. The VOCs were mainly identified as butyl acetate, toluene, ethylbenzene, and xylene compounds. VOC characteristics differed depending on the paint type. Butyl acetate had the highest concentration in both water- and oil-based paints; however, its concentration and proportion were higher in the former (3256 ppb, 65.5%) than in the latter (2449 ppb, 31.1%). Comparing VOC concentration before and after passing through adsorption systems, concentrations of most VOCs were lower at the outlets than the inlets of the adsorption systems, but were found to be high at the outlets in some workshops. These results provide a theoretical basis for developing effective VOC control systems and managing VOC emissions from auto-repair painting workshops.


2021 ◽  
Vol 13 (12) ◽  
pp. 6570
Author(s):  
Asma Akter Parlin ◽  
Monami Kondo ◽  
Noriaki Watanabe ◽  
Kengo Nakamura ◽  
Mizuki Yamada ◽  
...  

The quantitative understanding of the transport behavior of volatile organic compounds (VOCs) in near-surface soils is highly important in light of the potential impacts of soil VOC emissions on the air quality and climate. Previous studies have suggested that temperature changes affect the transport behavior; however, the effects are not well understood. Indeed, much larger changes in the VOC flux under in situ dynamic temperatures than those expected from the temperature dependence of the diffusion coefficients of VOCs in the air have been suggested but rarely investigated experimentally. Here, we present the results of a set of experiments on the upward vertical vapor-phase diffusive transport of benzene and trichloroethylene (TCE) in sandy soils with water contents ranging from an air-dried value to 10 wt% during sinusoidal temperature variation between 20 and 30 °C. In all experiments, the flux from the soil surface was correlated with the temperature, as expected. However, the changes in flux under wet conditions were unexpectedly large and increased with increasing water content; they were also larger for TCE, the volatility of which depended more strongly on the temperature. Additionally, the larger flux changes were accompanied by a recently discovered water-induced inverse correlation between temperature and flux into the overlying soil. These results demonstrated that the flux changes of VOCs under dynamic temperatures could be increased by volatilization-dissolution interactions of VOCs with water. Future extensive studies on this newly discovered phenomenon would contribute to a better understanding of the impacts of soil VOC emissions on the air quality and climate.


2018 ◽  
Author(s):  
Mounir Chrit ◽  
Karine Sartelet ◽  
Jean Sciare ◽  
Marwa Majdi ◽  
José Nicolas ◽  
...  

Abstract. Organic aerosols are measured at a remote site (Ersa) on Corsica Cape in the northwestern Mediterranean basin during the Chemistry-Aerosol Mediterranean Experiment (CharMEx) winter campaign of 2014, when high organic concentrations from anthropogenic origin are observed. This work aims at representing the observed organic aerosol concentrations and properties (oxidation state) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Because intermediate/semi-volatile organic compounds (I/S-VOC) are the main precursors of SOA at Ersa during the winter 2014, different parameterizations to represent the emission and ageing of I/S-VOC were implemented in the chemistry-transport model of the air-quality platform Polyphemus (different volatility distribution emissions, single-step oxidation vs multi-step oxidation within a Volatility Basis Set framework, inclusion of non-traditional volatile organic compounds NTVOC). Simulations using the different parameterizations are compared to each other and to the measurements (concentration and oxidation state). The high observed organic concentrations are well reproduced whatever the parameterizations. They are slightly under-estimated with most parameterizations, but they are slightly over-estimated when the ageing of NTVOC is taken into account. The volatility distribution at emissions influences more strongly the concentrations than the choice of the parameterization that may be used for ageing (single-step oxidation vs multi-step oxidation), stressing the importance of an accurate characterization of emissions. Assuming the volatility distribution of sectors other than residential heating to be the same as residential heating may lead to a strong under-estimation of organic concentrations. The observed organic oxidation and oxygenation states are strongly under-estimated in all simulations, even when a recently developed parameterization for modeling the ageing of I/S-VOC from residential heating is used. This suggests that uncertainties in the ageing of I/S-VOC emissions remain to be elucidated, with a potential role of organic nitrate from anthropogenic precursors and highly oxygenated organic molecules.


2019 ◽  
Vol 19 (11) ◽  
pp. 7429-7443 ◽  
Author(s):  
Tian Feng ◽  
Shuyu Zhao ◽  
Naifang Bei ◽  
Jiarui Wu ◽  
Suixin Liu ◽  
...  

Abstract. The implementation of the Air Pollution Prevention and Control Action Plan in China since 2013 has profoundly altered the ambient pollutants in the Beijing–Tianjin–Hebei (BTH) region. Here we show observations of substantially increased O3 concentrations (about 30 %) and a remarkable increase in the ratio of organic carbon (OC) to elemental carbon (EC) in BTH during the autumn from 2013 to 2015, revealing an enhancement in atmospheric oxidizing capacity (AOC) and secondary organic aerosol (SOA) formation. To explore the impacts of increasing AOC on the SOA formation, a severe air pollution episode from 3 to 8 October 2015 with high O3 and PM2.5 concentrations is simulated using the WRF-Chem model. The model performs reasonably well in simulating the spatial distributions of PM2.5 and O3 concentrations over BTH and the temporal variations in PM2.5, O3, NO2, OC, and EC concentrations in Beijing compared to measurements. Sensitivity studies show that the change in AOC substantially influences the SOA formation in BTH. A sensitivity case characterized by a 31 % O3 decrease (or 36 % OH decrease) reduces the SOA level by about 30 % and the SOA fraction in total organic aerosol by 17 % (from 0.52 to 0.43, dimensionless). Spatially, the SOA decrease caused by reduced AOC is ubiquitous in BTH, but the spatial relationship between SOA concentrations and the AOC is dependent on the SOA precursor distribution. Studies on SOA formation pathways further show that when the AOC is reduced, the SOA from oxidation and partitioning of semivolatile primary organic aerosol (POA) and co-emitted intermediate volatile organic compounds (IVOCs) decreases remarkably, followed by those from anthropogenic and biogenic volatile organic compounds (VOCs). Meanwhile, the SOA decrease in the irreversible uptake of glyoxal and methylglyoxal on the aerosol surfaces is negligible.


2014 ◽  
Vol 14 (12) ◽  
pp. 5871-5891 ◽  
Author(s):  
M. Wang ◽  
M. Shao ◽  
W. Chen ◽  
B. Yuan ◽  
S. Lu ◽  
...  

Abstract. Understanding the sources of volatile organic compounds (VOCs) is essential for ground-level ozone and secondary organic aerosol (SOA) abatement measures. We made VOC measurements at 27 sites and online observations at an urban site in Beijing from July 2009 to January 2012. Based on these measurement data, we determined the spatial and temporal distribution of VOCs, estimated their annual emission strengths based on their emission ratios relative to carbon monoxide (CO), and quantified the relative contributions of various sources using the chemical mass balance (CMB) model. These results from ambient measurements were compared with existing emission inventories to evaluate the spatial distribution, species-specific emissions, and source structure of VOCs in Beijing. The measured VOC distributions revealed a hotspot in the southern suburban area of Beijing, whereas current emission inventories suggested that VOC emissions were concentrated in downtown areas. Compared with results derived from ambient measurements, the annual inventoried emissions of oxygenated VOC (OVOC) species and C2–C4 alkanes may be underestimated, while the emissions of styrene and 1,3-butadiene may be overestimated by current inventories. Source apportionment using the CMB model identified vehicular exhaust as the most important VOC source, with the relative contribution of 49%, in good agreement with the 40–51% estimated by emission inventories. The relative contribution of paint and solvent utilization obtained from the CMB model was 14%, significantly lower than the value of 32% reported by one existing inventory. Meanwhile, the relative contribution of liquefied petroleum gas (LPG) usage calculated using the CMB model was 6%, whereas LPG usage contribution was not reported by current emission inventories. These results suggested that VOC emission strengths in southern suburban area of Beijing, annual emissions of C2–C4 alkanes, OVOCs and some alkenes, and the contributions of solvent and paint utilization and LPG usage in current inventories all require significant revisions.


2016 ◽  
Author(s):  
N. L. Ng ◽  
S. S. Brown ◽  
A. T. Archibald ◽  
E. Atlas ◽  
R. C. Cohen ◽  
...  

Abstract. Oxidation of biogenic volatile organic compounds (BVOC) by the nitrate radical (NO3) represents one of the important interactions between anthropogenic emissions related to combustion and natural emissions from the biosphere. This interaction has been recognized for more than three decades, during which time a large body of research has emerged from laboratory, field and modeling studies. NO3-BVOC reactions influence air quality, climate and visibility through regional and global budgets for reactive nitrogen (particularly organic nitrates), ozone and organic aerosol. Despite its long history of research and the significance of this topic in atmospheric chemistry, a number of important uncertainties remain. These include an incomplete understanding of the rates, mechanisms and organic aerosol yields for NO3-BVOC reactions, lack of constraints on the role of heterogeneous oxidative processes associated with the NO3 radical, the difficulty of characterizing the spatial distributions of BVOC and NO3 within the poorly mixed nocturnal atmosphere and the challenge of constructing appropriate boundary layer schemes and non-photochemical mechanisms for use in state-of-the-art chemical transport and chemistry-climate models. This review is the result of a workshop of the same title held at the Georgia Institute of Technology in June 2015. The first section summarizes the current literature on NO3-BVOC chemistry, with a particular focus on recent advances in instrumentation and models, and in organic nitrate and secondary organic aerosol (SOA) formation chemistry. Building on this current understanding, the second half of the review outlines impacts of NO3-BVOC chemistry on air quality and climate, and suggests critical research needs to better constrain this interaction to improve the predictive capabilities of atmospheric models.


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