Characterization of Organic Aerosol at a Rural Site in the North China Plain Region: Sources, Volatility and Organonitrates

Zhu, Qiao; Cao, Liming; Tang, Meng‐Xue; Huang, Xiaofeng; Saikawa, Eri; He, Lingyan

doi:10.1007/s00376-020-0127-2

Cited by 19 publications

(42 citation statements)

References 80 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The negligible correlation of NO 3,org with POA in summer in Beijing (R 2 = 0.05) is in contradiction with the results in Xianghe (a rural site in NCP), which shows that pON formation might be highly associated with primary emissions (Qiao et al, 2021). Such differences were caused by the different primary emission in different environments.…”

Section: Intercomparisonsmentioning

confidence: 57%

“…Yu et al (2019) found a good correlation between pON and fresh SOA at night at an urban site in southern China based on the NO x method and the PMF method. In contrast, Qiao et al (2021) reported that pON were more correlated with the emission from biomass burning but poorly correlated with less-oxidized oxygenated OA (LO-OOA) at a rural site (Xianghe) in summer. Despite these results, our understanding of the levels, sources and processes of pON in the North China Plain (NCP) remains poor.…”

Section: Introductionmentioning

confidence: 92%

“…Such differences were caused by the different primary emission in different environments. For example, BBOA is the dominant POA in Xianghe (Qiao et al, 2021) but not in Beijing during summertime. The higher correlation of NO 3,org with POA was found in winter in NCP (R 2 = 0.49-0.52), suggesting that primary emissions can be an important source of pON in winter in NCP, which may be related to NO 3 oxidation of AVOCs emitted from anthropogenic activities (Li et al, 2019;Lee et al, 2019).…”

Section: Intercomparisonsmentioning

confidence: 99%

See 2 more Smart Citations

Estimation of particulate organic nitrates from thermodenuder–aerosol mass spectrometer measurements in the North China Plain

Takeuchi

Chen

et al. 2021

Atmos. Meas. Tech.

View full text Add to dashboard Cite

Abstract. Particulate organic nitrates (pON) are an important component of secondary organic aerosol in biogenic-emission-dominant environments and play a critical role in NOx cycles. However, estimation of pON has been a challenge in polluted environments, e.g., North China Plain, with high concentrations of inorganic nitrate and NOx. Here we developed a method for estimation of pON from the measurements of high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally correlated well with those estimated from positive matrix factorization of combined organic and inorganic mass spectra and from the ratio of NO+ to NO2+ (NOx+ ratio), yet they had improvements in reducing negative values due to the influences of high concentration of inorganic nitrate and constant NOx+ ratio of organic nitrates (RON). By applying this approach to the measurements at an urban (Beijing) and a rural site (Gucheng) in summer and winter in the North China Plain, we estimated that the average mass concentrations of NO3,org (1.8 µg m−3 vs. 1.0 µg m−3) and pON to OA (27.5 % vs. 14.8 %) were higher in summer than in winter in Beijing, indicating more pON formation in biogenically and anthropogenically mixed environments. In addition, the average NO3,org loading in Gucheng was 1.9 µg m−3, and the pON at the rural site also showed higher contribution to OA than that in Beijing during wintertime due to higher primary emissions and gaseous precursors in Gucheng. In addition, RON was determined and showed considerable differences between day–night and clean–polluted periods, highlighting the complexity of pON compounds from different chemical pathways (e.g., OH and NO3 oxidation) and sources.

show abstract

Section: Intercomparisonsmentioning

confidence: 57%

Section: Introductionmentioning

confidence: 92%

Section: Intercomparisonsmentioning

confidence: 99%

See 1 more Smart Citation

Estimation of particulate organic nitrates from thermodenuder–aerosol mass spectrometer measurements in the North China Plain

Takeuchi

Chen

et al. 2021

Atmos. Meas. Tech.

View full text Add to dashboard Cite

show abstract

“…Compared with laboratory experiments, the oxidation pathways and oxidants are far more complex in ambient air, and the oxygenated products can be composed of hundreds or even thousands of species with a wide range of volatilities. Previous field observations on volatility distributions of OA have mainly been focused on Europe and the US under low NO x levels (Xu et al, 2016;Louvaris et al, 2017a;Saha et al, 2017;Kostenidou et al, 2018). Lee et al (2011a) found that NO x can have a large impact on the volatility of SOA in a chamber experiment, suggesting that the OA volatilities in high-NO x and high particulate-matter (PM) environments, e.g., the North China Plain (NCP), need to be further investigated.…”

Section: Introductionmentioning

confidence: 99%

Organic aerosol volatility and viscosity in the North China Plain: contrast between summer and winter

Chen

Qiu

et al. 2021

Atmos. Chem. Phys.

View full text Add to dashboard Cite

Abstract. Volatility and viscosity have substantial impacts on gas–particle partitioning, formation and evolution of aerosol and hence the predictions of aerosol-related air quality and climate effects. Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) in summer and winter were investigated by using a thermodenuder coupled with a high-resolution aerosol mass spectrometer. The effective saturation concentration (C*) of organic aerosol (OA) in summer was smaller than that in winter (0.55 µg m−3 vs. 0.71–0.75 µg m−3), indicating that OA in winter in the NCP is more volatile due to enhanced primary emissions from coal combustion and biomass burning. The volatility distributions varied and were largely different among different OA factors. In particular, we found that hydrocarbon-like OA (HOA) contained more nonvolatile compounds compared to coal-combustion-related OA. The more oxidized oxygenated OA (MO-OOA) showed overall lower volatility than less oxidized OOA (LO-OOA) in both summer and winter, yet the volatility of MO-OOA was found to be relative humidity (RH) dependent showing more volatile properties at higher RH. Our results demonstrated the different composition and chemical formation pathways of MO-OOA under different RH levels. The glass transition temperature (Tg) and viscosity of OA in summer and winter are estimated using the recently developed parameterization formula. Our results showed that the Tg of OA in summer in Beijing (291.5 K) was higher than that in winter (289.7–290.0 K), while it varied greatly among different OA factors. The viscosity suggested that OA existed mainly as solid in winter in Beijing (RH = 29 ± 17 %), but as semisolids in Beijing in summer (RH = 48 ± 25 %) and Gucheng in winter (RH = 68 ± 24 %). These results have the important implication that kinetically limited gas–particle partitioning may need to be considered when simulating secondary OA formation in the NCP.

show abstract

“…3. Additionally, a number of analyses of field studies have used the NO x + 110 ratios (or its 46/30 UMR equivalent) to support qualitative or semi-quantitative statements about the presence (or low contribution) of pRONO 2 (Setyan et al, 2012;Brown et al, 2013;Xu et al, 2016;Schneider et al, 2017;Bottenus et al, 2018) or to quantify pRONO 2 (Fry et al, 2013(Fry et al, , 2018Ayres et al, 2015;Kostenidou et al, 2015;Xu et al, 2015aXu et al, , 2021Fisher et al, 2016;Kiendler-Scharr et al, 2016;Lee et al, 2016Lee et al, , 2019Nault et al, 2016;Zhou et al, 2016;Zhu et al, 2016Zhu et al, , 2021Florou et al, 2017;115 Palm et al, 2017;Brito et al, 2018;de Sá et al, 2018de Sá et al, , 2019Reyes-Villegas et al, 2018;Schulz et al, 2018;Avery et al, 2019;Dai et al, 2019;Huang et al, 2019aHuang et al, , 2019bYu et al, 2019;Chen et al, 2020. Yu et al (2019) also used the particle size dependence of the 46/30 ratio to investigate particle size and temporal (diurnal and seasonal) trends in pRONO 2 .…”

mentioning

confidence: 99%

A Systematic Re-evaluation of Methods for Quantification of Bulk Particle-phase Organic Nitrates Using Real-time Aerosol Mass Spectrometry

Day

Campuzano‐Jost

Nault

et al. 2021

Preprint

View full text Add to dashboard Cite

Abstract. Organic nitrate (RONO2) formation in the atmosphere represents a sink of NOx (NOx = NO + NO2) and termination of the NOx/HOx (HOx = HO2 + OH) ozone formation and radical propagation cycles, can act as a NOx reservoir transporting reactive nitrogen, and contributes to secondary organic aerosol formation. While some fraction of RONO2 is thought to reside in the particle phase, particle-phase organic nitrates (pRONO2) are infrequently measured and thus poorly understood. There is an increasing prevalence of aerosol mass spectrometer (AMS) instruments, which have shown promise for determining quantitative total organic nitrate functional group contribution to aerosols. A simple approach that relies on the relative intensities of NO+ and NO2+ ions in the AMS spectrum, the calibrated NOx+ ratio for NH4NO3, and the inferred ratio for pRONO2 has been proposed as a way to apportion the total nitrate signal to NH4NO3 and pRONO2. This method is increasingly being applied to field and laboratory data. However, the methods applied have been largely inconsistent and poorly characterized, and therefore, a detailed evaluation is timely. Here, we compile an extensive survey of NOx+ ratios measured for various pRONO2 compounds and mixtures from multiple AMS instruments, groups, and laboratory and field measurements. We show that, in the absence of pRONO2 standards, the pRONO2 NOx+ ratio can be estimated using a ratio referenced to the calibrated NH4NO3 ratio, a so-called Ratio-of-Ratios method (RoR = 2.75 ± 0.41). We systematically explore the basis for quantifying pRONO2 (and NH4NO3) with the RoR method using ground and aircraft field measurements conducted over a large range of conditions. The method is compared to another AMS method (positive matrix factorization, PMF) and other pRONO2 and related (e.g., total gas + particle RONO2) measurements, generally showing good agreement/correlation. A broad survey of ground and aircraft AMS measurements shows a pervasive trend of higher fractional contribution of pRONO2 to total nitrate with lower total nitrate concentrations, which generally corresponds to shifts from urban-influenced to rural/remote regions. Compared to ground campaigns, observations from all aircraft campaigns showed substantially lower pRONO2 contributions at mid ranges of total nitrate (0.01–0.1 up to 2–5 μg m−3), suggesting that the balance of effects controlling NH4NO3 and pRONO2 formation and lifetimes — such as higher humidity, lower temperatures, greater dilution, different sources, higher particle acidity, and pRONO2 hydrolysis (possibly accelerated by particle acidity) — favors lower pRONO2 contributions for those environments and altitudes sampled.

show abstract

Characterization of Organic Aerosol at a Rural Site in the North China Plain Region: Sources, Volatility and Organonitrates

Cited by 19 publications

References 80 publications

Estimation of particulate organic nitrates from thermodenuder–aerosol mass spectrometer measurements in the North China Plain

Estimation of particulate organic nitrates from thermodenuder–aerosol mass spectrometer measurements in the North China Plain

Organic aerosol volatility and viscosity in the North China Plain: contrast between summer and winter

A Systematic Re-evaluation of Methods for Quantification of Bulk Particle-phase Organic Nitrates Using Real-time Aerosol Mass Spectrometry

Contact Info

Product

Resources

About