Aerosol surface area concentration: a governing factor in new particle formation in Beijing

Cai, Runlong; Yang, Dongsen; Fu, Yuan; Wang, Xing; Li, Xiaoxiao; Ma, Yan; Hao, Jiming; Zheng, Jun; Jiang, Jingkun

doi:10.5194/acp-17-12327-2017

Cited by 103 publications

(127 citation statements)

References 55 publications

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“…The wet aerosol surface areas of the sampling sites in China were simulated with the CMAQ model, whereas these surface areas of other sites were simulated using the GEOS-Chem global CTM. Cai et al (2017) reported that the R 2 between the active aerosol surface area and PM 2.5 mass concentration reached a value of 0.85. Hence, the correction method is adequate for the analysis of correlating the unknown HONO source with aerosol surface area.…”

Section: Methodsmentioning

confidence: 99%

Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source

Wang

et al. 2018

Environ. Res. Lett.

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Large missing daytime HONO sources have been reported by many previous studies around the world. Possible HONO sources include ground heterogeneous conversion, aerosol heterogeneous formation, soil emission, and photochemical production. In this study, a consistent 1D framework based on regional and 3D chemical transport models (CTMs) was used to analyze the unknown daytime HONO sources in 14 cases worldwide. We assume that the source of HONO from aerosols is through NO 2 hydrolysis (not including its oxidation products) and that non-local mixing effect is negligible. Assuming all the missing unknown HONO source is from the ground, it would imply a NO 2 -to-HONO ground heterogeneous conversion exceeding 100% in daytime, which is unphysical. In contrast, a strong R 2 reaching up to 0.92 is found between the unknown HONO sources and the products of aerosol wet surface area and short-wave radiation. Because the largest unknown daytime HONO sources are found in China due to high concentrations of aerosols and NO 2 , we derive an optimized NO 2 uptake coefficient on the basis of these measurements. The 3D CTM simulations suggest that in some regions of central, eastern, and southwestern (e.g. SiChuan province) China, the aerosol HONO source has the greatest effects on ozone (>10 ppbv) and OH (>200%) in winter. In January, the simulated particulate sulfate level over these three regions increases by 6-10 μg m −3 after including the aerosol-HONO source, which helps reduce the previous model underestimation of sulfate production in winter. Additional measurement studies that target the daytime HONO sources will be essential to a better understanding of the mechanisms and resulting effects on atmospheric oxidants.

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Section: Methodsmentioning

confidence: 99%

Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source

Wang

et al. 2018

Environ. Res. Lett.

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“…On the other hand, water vapor may also directly influence NPF by regulating the formation of gas-phase precursors or by participating in cluster formation. For example, chamber and model experiments on the binary sulfuric acid-water system have demonstrated positive relationships between particle formation rate and RH , while in the ternary (H 2 SO 4 /MSA-H 2 O-amine/NH 3 ) system, H 2 O was reported to have either positive (Chen et al, 2015) or negative (Napari et al, 2002) effects on NPF. Some studies have hypothesized that high water content might suppress the formation of NPF-related organics from the oxidation of biogenic precursors (Hyvönen et al, 2005;Boy and Kulmala, 2002).…”

Section: Introductionmentioning

confidence: 99%

Relative humidity effect on the formation of highly oxidized molecules and new particles during monoterpene oxidation

Li¹,

Hao²,

Abbatt³

et al. 2019

Atmos. Chem. Phys.

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Abstract. It has been widely observed around the world that the frequency and intensity of new particle formation (NPF) events are reduced during periods of high relative humidity (RH). The current study focuses on how RH affects the formation of highly oxidized molecules (HOMs), which are key components of NPF and initial growth caused by oxidized organics. The ozonolysis of α-pinene, limonene, and Δ3-carene, with and without OH scavengers, were carried out under low NOx conditions under a range of RH (from ∼3 % to ∼92 %) in a temperature-controlled flow tube to generate secondary organic aerosol (SOA). A Scanning Mobility Particle Sizer (SMPS) was used to measure the size distribution of generated particles, and a novel transverse ionization chemical ionization inlet with a high-resolution time-of-fight mass spectrometer detected HOMs. A major finding from this work is that neither the detected HOMs nor their abundance changed significantly with RH, which indicates that the detected HOMs must be formed from water-independent pathways. In fact, the distinguished OH- and O3-derived peroxy radicals (RO2), HOM monomers, and HOM dimers could mostly be explained by the autoxidation of RO2 followed by bimolecular reactions with other RO2 or hydroperoxy radicals (HO2), rather than from a water-influenced pathway like through the formation of a stabilized Criegee intermediate (sCI). However, as RH increased from ∼3 % to ∼92 %, the total SOA number concentrations decreased by a factor of 2–3 while SOA mass concentrations remained relatively constant. These observations show that, while high RH appears to inhibit NPF as evident by the decreasing number concentration, this reduction is not caused by a decrease in RO2-derived HOM formation. Possible explanations for these phenomena were discussed.

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“…in Switzerland, Mt. Werner in the US, and the Himalayas in Nepal (Hallar et al, 2011;Chiharu et al, 2008;Weingartner et al, 1999;Venzac et al, 2008). At present, there have not been many observations at mountaintop sites in China.…”

Section: Introductionmentioning

confidence: 99%

Investigation of new particle formation at the summit of Mt. Tai, China

Lv¹,

Sui²,

Chen³

et al. 2018

Atmos. Chem. Phys.

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Abstract. To date, few comprehensive field observations of new particle formation (NPF) have been carried out at mountaintop sites in China. In this study, simultaneous measurements of particle size distribution, trace gases, meteorological parameters, and mass concentration and chemical composition of PM 2.5 were performed at the summit of Mt. Tai (1534 m a.s.l.) from 25 July to 24 August 2014 (Phase I), 21 September to 9 December 2014 (Phase II), and 16 June to 7 August 2015 (Phase III) to investigate characteristics and favorable conditions of NPF in a relatively clean mountaintop environment. The NPF events were identified based on particle size distribution measured by the neutral cluster and air ion spectrometer (NAIS), and 66 such events were observed during a period of 164 days -corresponding to an occurrence frequency of 40 %. The formation rates of 3 nm particles (J 3 ) and growth rates were in the ranges of 0.82-25.04 cm −3 s −1 and 0.58-7.76 nm h −1 , respectively. On average, the condensation sink (CS), O 3 concentration, air temperature, and relative humidity were lower, whereas the SO 2 concentration was higher on NPF days than that on non-NPF days. The CS on Mt. Tai was at a low level and lower CS was critical for NPF. NPF events were common when wind came from the east-southeast and west-southwest, which was probably associated with relatively lower CS in the east-southeast and higher SO 2 concentration in the west-southwest. O 3 was not a governing factor for NPF in this study, and a high level of NO x concentration might be responsible for the decreased O 3 concentration on NPF days. Three categories of backward trajectories were classified, among which the continental air mass was the majority. The continental air mass passing through more polluted areas (denoted as Type I) favored NPF because of enhanced SO 2 concentration and potential ammonia with it. An in-depth analysis of SO 2 indicated that sulfuric acid was a dominant precursor on Mt. Tai; meanwhile, biogenic organics released from ambient forests in warm seasons and anthropogenic volatile organic compounds emitted from domestic heating in cold seasons also promoted NPF.

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Aerosol surface area concentration: a governing factor in new particle formation in Beijing

Cited by 103 publications

References 55 publications

Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source

Evidence of heterogeneous HONO formation from aerosols and the regional photochemical impact of this HONO source

Relative humidity effect on the formation of highly oxidized molecules and new particles during monoterpene oxidation

Investigation of new particle formation at the summit of Mt. Tai, China

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