scholarly journals Chamber investigation of the formation and transformation of secondary organic aerosol in mixtures of biogenic and anthropogenic volatile organic compounds

2022 ◽  
Author(s):  
Aristeidis Voliotis ◽  
Mao Du ◽  
Yu Wang ◽  
Yunqi Shao ◽  
M. Rami Alfarra ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Phase Behaviour ◽  
Ternary Mixtures ◽  
Base Case ◽  
Formation Potential ◽  
Seed Particles ◽  
Volatile Organic ◽  
The Difference ◽  
Initial Reactivity

Abstract. A comprehensive investigation of the photochemical secondary organic aerosol (SOA) formation and transformation in mixtures of anthropogenic (o-cresol) and biogenic (α-pinene and isoprene) volatile organic compound (VOC) precursors in the presence of NOx and inorganic seed particles was conducted. Initial iso-reactivity was used to enable direct comparison across systems, adjusting the initial reactivity of the systems towards the assumed dominant oxidant (OH). Comparing experiments conducted in single precursor systems at various initial reactivity levels (referenced to a nominal base case VOC reactivity) and their binary and ternary mixtures, we show that the molecular interactions from the mixing of the precursors can be investigated and discuss limitations in their interpretation. The observed average SOA yields in descending order were found for the α-pinene (32 ± 7 %), α-pinene/o-cresol (28 ± 9 %), α-pinene at ½ initial reactivity (21 ± 5 %), α-pinene/isoprene (16 ± 1 %), α-pinene at ⅓ initial reactivity (15 ± 4 %), o-cresol (13 ± 3 %), α-pinene/o-cresol/isoprene (11 ± 4%), o-cresol at ½ initial reactivity (11 ± 3 %), o-cresol/isoprene (6 ± 2 %) and isoprene systems (0 ± 0 %). We find a clear suppression of the SOA yield from α-pinene when it is mixed with isoprene, whilst the addition of isoprene to o-cresol may enhance the mixture’s SOA formation potential, however, the difference was too small to be unequivocal. The α-pinene/o-cresol system yield appeared to be increased compared to that calculated based on the additivity, whilst in the α-pinene/o-cresol/isoprene system the measured and predicted yield were comparable. However, in mixtures where more than one precursor contributes to the SOA mass it is unclear whether changes in the SOA formation potential are attributable to physical or chemical interactions, since the reference basis for the comparison is complex. Online and offline chemical composition and SOA particle volatility, water uptake and “phase” behaviour measurements that were used to interpret the SOA formation and behaviour are introduced and detailed elsewhere.

scholarly journals Comparison of secondary organic aerosol formation from toluene on initially wet and dry ammonium sulfate particles at moderate relative humidity

2018 ◽  
Vol 18 (8) ◽  
pp. 5677-5689 ◽  
Author(s):  
Tengyu Liu ◽  
Dan Dan Huang ◽  
Zijun Li ◽  
Qianyun Liu ◽  
ManNin Chan ◽  
...  
Keyword(s):  
Relative Humidity ◽  
Ammonium Sulfate ◽  
Functional Groups ◽  
Flow Reactor ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Aerosol Formation ◽  
Seed Particles ◽  
The Difference ◽  
Wet Particles

Abstract. The formation of secondary organic aerosol (SOA) has been widely studied in the presence of dry seed particles at low relative humidity (RH). At higher RH, initially dry seed particles can exist as wet particles due to water uptake by the seeds as well as the SOA. Here, we investigated the formation of SOA from the photooxidation of toluene using an oxidation flow reactor in the absence of NOx under a range of OH exposures on initially wet or dry ammonium sulfate (AS) seed particles at an RH of 68 %. The ratio of the SOA yield on wet AS seeds to that on dry AS seeds, the relative SOA yield, decreased from 1.31 ± 0.02 at an OH exposure of 4.66 × 1010 molecules cm−3 s to 1.01 ± 0.01 at an OH exposure of 5.28 × 1011 molecules cm−3 s. This decrease may be due to the early deliquescence of initially dry AS seeds after being coated by highly oxidized toluene-derived SOA. SOA formation lowered the deliquescence RH of AS and resulted in the uptake of water by both AS and SOA. Hence the initially dry AS seeds contained aerosol liquid water (ALW) soon after SOA formed, and the SOA yield and ALW approached those of the initially wet AS seeds as OH exposure and ALW increased, especially at high OH exposure. However, a higher oxidation state of the SOA on initially wet AS seeds than that on dry AS seeds was observed at all levels of OH exposure. The difference in mass fractions of m ∕ z 29, 43 and 44 of SOA mass spectra, obtained using an aerosol mass spectrometer (AMS), indicated that SOA formed on initially wet seeds may be enriched in earlier-generation products containing carbonyl functional groups at low OH exposures and later-generation products containing acidic functional groups at high exposures. Our results suggest that inorganic dry seeds become at least partially deliquesced particles during SOA formation and hence that ALW is inevitably involved in the SOA formation at moderate RH. More laboratory experiments conducted with a wide variety of SOA precursors and inorganic seeds under different NOx and RH conditions are warranted.

scholarly journals A mass-balance-based emission inventory of non-methane volatile organic compounds (NMVOCs) for solvent use in China

2021 ◽  
Vol 21 (17) ◽  
pp. 13655-13666
Author(s):  
Ziwei Mo ◽  
Ru Cui ◽  
Bin Yuan ◽  
Huihua Cai ◽  
Brian C. McDonald ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Emission Inventory ◽  
Secondary Organic Aerosol ◽  
Personal Care Products ◽  
Organic Aerosol ◽  
Personal Care ◽  
Formation Potential ◽  
Volatile Organic ◽  
Solvent Use

Abstract. Non-methane volatile organic compounds (NMVOCs) are important precursors of ozone (O3) and secondary organic aerosol (SOA), which play key roles in tropospheric chemistry. A huge amount of NMVOC emissions from solvent use are complicated by a wide spectrum of sources and species. This work presents a long-term NMVOC emission inventory of solvent use during 2000–2017 in China. Based on a mass (material) balance method, NMVOC emissions were estimated for six categories, including coatings, adhesives, inks, pesticides, cleaners, and personal care products. The results show that NMVOC emissions from solvent use in China increased rapidly from 2000 to 2014 then kept stable after 2014. The total emission increased from 1.6 Tg (1.2–2.2 Tg at 95 % confidence interval) in 2000 to 10.6 Tg (7.7–14.9 Tg) in 2017. The substantial growth is driven by the large demand for solvent products in both industrial and residential activities. However, increasing treatment facilities in the solvent-related factories in China restrained the continued growth of solvent NMVOC emissions in recent years. Rapidly developing and heavily industrialized provinces such as Jiangsu, Shandong, and Guangdong contributed significantly to the solvent use emissions. Oxygenated VOCs, alkanes, and aromatics were the main components, accounting for 42 %, 28 %, and 21 % of total NMVOC emissions in 2017, respectively. Our results and previous inventories are generally comparable within the estimation uncertainties (−27 %–52 %). However, there exist significant differences in the estimates of sub-categories. Personal care products were a significant and quickly rising source of NMVOCs, which were probably underestimated in previous inventories. Emissions from solvent use were growing faster compared with transportation and combustion emissions, which were relatively better controlled in China. Environmentally friendly products can reduce the NMVOC emissions from solvent use. Supposing all solvent-based products were substituted with water-based products, it would result in 37 %, 41 %, and 38 % reduction of emissions, ozone formation potential (OFP), and secondary organic aerosol formation potential (SOAP), respectively. These results indicate there is still large potential for NMVOC reduction by reducing the utilization of solvent-based products and implementation of end-of-pipe controls across industrial sectors.

scholarly journals Comparison of secondary organic aerosol formation from toluene on initially wet and dry ammonium sulfate particles

2017 ◽  
Author(s):  
Tengyu Liu ◽  
Dan Dan Huang ◽  
Zijun Li ◽  
Qianyun Liu ◽  
ManNin Chan ◽  
...  
Keyword(s):  
Ammonium Sulfate ◽  
Functional Groups ◽  
Flow Reactor ◽  
Secondary Organic Aerosol ◽  
Large Fraction ◽  
Organic Aerosol ◽  
Aerosol Formation ◽  
Seed Particles ◽  
The Difference ◽  
Wet Particles

Abstract. The formation of secondary organic aerosol (SOA) has been widely studied in the presence of dry seed particles at low relative humidity (RH). At higher RH, seed particles can exist as dry or wet particles. Here, we investigated the formation of SOA from the photooxidation of toluene using an oxidation flow reactor under a range of OH exposures on initially wet or dry ammonium sulfate (AS) seed particles at an RH of 68 %. At an OH exposure of 4.66 × 1010 molecules cm -3 s, the ratio of the SOA yield on wet AS seeds to that on dry AS seeds was 1.31 ± 0.02. However, this ratio decreased to 1.01 ± 0.01 at an OH exposure of 5.28 × 1011 molecules cm -3 s. The decrease in the ratios of SOA yields as the increase of OH exposure may be due to the early deliquescence of initially dry AS seeds after coated by highly oxidized toluene-derived SOA. SOA formation lowered the deliquescence RH of AS and resulted in the uptake of water by both AS and SOA. Hence the initially dry AS seeds contained aerosol liquid water (ALW) soon after a large fraction of SOA formed and the SOA yield and ALW approached those of the initially wet AS seeds as OH exposure and ALW increased. However, a higher oxidation state of the SOA on initially wet AS seeds than that on dry AS seeds was observed at all levels of OH exposure. The difference in mass fractions of m/z 29, 43 and 44 of SOA mass spectra indicated that SOA formed on initially wet seeds may be enriched in earlier-generation products containing carbonyl functional groups at low OH exposures and later-generation products containing acidic functional groups at high exposures. Our results suggest that AS dry seeds soon turn to at least partially deliquesced particles during SOA formation and more studies on the interplay of SOA formation and ALW are warranted.

scholarly journals Impact of NO<sub><i>x</i></sub> and OH on secondary organic aerosol formation from <i>β</i>-pinene photooxidation

2016 ◽  
Vol 16 (17) ◽  
pp. 11237-11248 ◽  
Author(s):  
Mehrnaz Sarrafzadeh ◽  
Jürgen Wildt ◽  
Iida Pullinen ◽  
Monika Springer ◽  
Einhard Kleist ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Particle Surface ◽  
Organic Aerosol ◽  
Aerosol Formation ◽  
Substantial Fraction ◽  
Pronounced Increase ◽  
Mass Growth ◽  
Seed Particles ◽  
Volatile Organic ◽  
Induced Changes

Abstract. In this study, the NOx dependence of secondary organic aerosol (SOA) formation from photooxidation of the biogenic volatile organic compound (BVOC) β-pinene was comprehensively investigated in the Jülich Plant Atmosphere Chamber. Consistent with the results of previous NOx studies we found increases of SOA yields with increasing [NOx] at low-NOx conditions ([NOx]0  <  30 ppb, [BVOC]0 ∕ [NOx]0  >  10 ppbC ppb−1). Furthermore, increasing [NOx] at high-NOx conditions ([NOx]0  >  30 ppb, [BVOC]0 ∕ [NOx]0  ∼  10 to  ∼  2.6 ppbC ppb−1) suppressed the SOA yield. The increase of SOA yield at low-NOx conditions was attributed to an increase of OH concentration, most probably by OH recycling in NO + HO2  →  NO2 + OH reaction. Separate measurements without NOx addition but with different OH primary production rates confirmed the OH dependence of SOA yields. After removing the effect of OH concentration on SOA mass growth by keeping the OH concentration constant, SOA yields only decreased with increasing [NOx]. Measuring the NOx dependence of SOA yields at lower [NO] ∕ [NO2] ratio showed less pronounced increase in both OH concentration and SOA yield. This result was consistent with our assumption of OH recycling by NO and to SOA yields being dependent on OH concentrations. Our results furthermore indicated that NOx dependencies vary for different NOx compositions. A substantial fraction of the NOx-induced decrease of SOA yields at high-NOx conditions was caused by NOx-induced suppression of new particle formation (NPF), which subsequently limits the particle surface where low volatiles condense. This was shown by probing the NOx dependence of SOA formation in the presence of seed particles. After eliminating the effect of NOx-induced suppression of NPF and NOx-induced changes of OH concentrations, the remaining effect of NOx on the SOA yield from β-pinene photooxidation was moderate. Compared to β-pinene, the SOA formation from α-pinene photooxidation was only suppressed by increasing NOx. However, basic mechanisms of the NOx impacts were the same as that of β-pinene.

scholarly journals Secondary organic aerosol phase behaviour in chamber photo-oxidation of mixed precursors

2021 ◽  
Author(s):  
Yu Wang ◽  
Aristeidis Voliotis ◽  
Yunqi Shao ◽  
Taomou Zong ◽  
Xiangxinyue Meng ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Inorganic Compounds ◽  
Organic Aerosol ◽  
Phase Behaviour ◽  
Particle Phase ◽  
Photo Oxidation ◽  
Physicochemical Processes ◽  
Volatile Organic ◽  
Aerosol Chamber ◽  
Seed Aerosol

Abstract. The phase behaviour of aerosol particles plays a profound role in atmospheric physicochemical processes, influencing their physical and optical properties and further impacting climate and air quality. However, understanding of aerosol phase behaviour is still incomplete, especially that of multicomponent particles which contain inorganic compounds and secondary organic aerosol (SOA) from mixed volatile organic compound (VOC) precursors. We report measurements conducted in the Manchester Aerosol Chamber (MAC) to investigate the aerosol rebounding tendency, measured as bounce fraction, as a surrogate of particle phase behaviour during SOA formation from photo-oxidation of biogenic (α-pinene, isoprene) and anthropogenic (o-cresol) VOCs and their binary mixtures on deliquescent ammonium sulphate seed. Aerosol phase behaviour is RH and chemical composition dependent. Liquid (bounce fraction, BF  80 % and non-liquid behaviour (BF > 0.8) at RH 

scholarly journals Aging of atmospheric aerosols and the role of iron in catalyzing brown carbon formation

2021 ◽  
Author(s):  
Hind A. A. Al-Abadleh
Keyword(s):  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Atmospheric Aerosols ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Atmospheric Oxidation ◽  
Carbon Formation ◽  
Brown Carbon ◽  
Volatile Organic

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...

Sign in / Sign up

Export Citation Format

Share Document