Formation of secondary inorganic aerosol in a frigid urban atmosphere

doi:10.1007/s11783-021-1452-0

Front. Environ. Sci. Eng.

2022, Vol. 16

Issue (2) : 18 https://doi.org/10.1007/s11783-021-1452-0

RESEARCH ARTICLE

Formation of secondary inorganic aerosol in a frigid urban atmosphere

Yuan Cheng¹, Qinqin Yu¹, Jiumeng Liu¹(

), Youwen Sun²(

), Linlin Liang³, Zhenyu Du⁴, Guannan Geng⁵, Wanli Ma¹, Hong Qi¹, Qiang Zhang⁶, Kebin He⁵

¹. State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
². Key Laboratory of Environmental Optics and Technology, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China
³. State Key Laboratory of Severe Weather & CMA Key Laboratory of Atmospheric Chemistry, Chinese Academy of Meteorological Sciences, Beijing 100081, China
⁴. National Research Center for Environmental Analysis and Measurement, Environmental Development Center of the Ministry of Ecology and Environment, Beijing 100029, China
⁵. State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
⁶. Department of Earth System Science, Tsinghua University, Beijing 100084, China

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Abstract

•Harbin showed relatively high threshold RH (80%) for apparent increase of SOR.

•The observed SOR were at the lower end of the ratios from Beijing’s winter.

•Temperature-dependent increase of NOR was sharper than that of SOR.

• NOR increased with stronger biomass burning impact but SOR was largely unchanged.

Formation of secondary inorganic aerosol (SIA) was investigated during a six-month long heating season in Harbin, China. Enhanced sulfate formation was observed at high relative humidity (RH), with the same threshold RH (80%) for both colder and warmer measurement periods. Compared to wintertime results from Beijing, the threshold RH was considerably higher in Harbin, whereas the RH-dependent enhancement of sulfur oxidation ratio (SOR) was less significant. In addition, the high RH events were rarely encountered, and for other periods, the SOR were typically as low as ~0.1. Therefore, the sulfate formation was considered inefficient in this study. After excluding the several cases with high RH, both SOR and the nitrogen oxidation ratio (NOR) exhibited increasing trends as the temperature increased, with the increase of NOR being sharper. The nitrate to sulfate ratio tended to increase with increasing temperature as well. Based on a semi-quantitative approach, this trend was attributed primarily to the temperature-dependent variations of precursors including SO₂ and NO₂. The influence of biomass burning emissions on SIA formation was also evident. With stronger impact of biomass burning, an enhancement in NOR was observed whereas SOR was largely unchanged. The different patterns were identified as the dominant driver of the larger nitrate to sulfate ratios measured at higher concentrations of fine particulate matter.

Keywords Haze Sulfate Nitrate Heterogeneous chemistry Biomass burning Northeast China

Corresponding Author(s): Jiumeng Liu,Youwen Sun

Issue Date: 24 May 2021

Cite this article:

Yuan Cheng,Qinqin Yu,Jiumeng Liu, et al. Formation of secondary inorganic aerosol in a frigid urban atmosphere[J]. Front. Environ. Sci. Eng., 2022, 16(2): 18.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-021-1452-0
https://academic.hep.com.cn/fese/EN/Y2022/V16/I2/18

Fig.1 RH-dependent variations of SOR and NOR in (a) fall, (b) winter and (c) spring. Also shown are the RH-dependent variations of the sulfate to EC ratio and the nitrate to EC ratio during the respective periods (d–f). The same threshold RH for enhanced sulfate formation, i.e., 80%, was observed in different seasons. Due to the relatively high threshold RH, only a small number of samples (N = 8) showed RH-dependent increase of SOR during the six-month long period, as highlighted by the solid circles in (a)–(c). These samples are also highlighted using solid circles in (d)–(f). All these samples contained liquid water in aerosol-phase, as predicted by the E-AIM thermodynamic model which was run in the reverse mode by assuming an “H⁺–NH₄⁺–SO₄²⁻–NO₃⁻–H₂O” inorganic aerosol system. The predicted aerosol water contents (AWC) were ~7–23 and ~75–225 μg/m³ for the samples from warmer (i.e., fall and spring; N = 5) and colder (i.e., winter; N = 3) measurement periods, respectively. After RH exceeded 80%, concurrent increases of SOR, NOR, the sulfate to EC ratio and the nitrate to EC ratio were evident in winter (as highlighted by the dashed ovals), but this phenomenon was not apparent during fall and spring.

Fig.2 Two-dimensional histograms showing variations of (a) sulfate concentration and (b) the relative number of samples with the changes of RH and NO₂. Bin width and height are 10% (for RH) and 10 μg/m³ (for NO₂), respectively. The bins are colored by sulfate concentration in (a) and by the relative number of samples in (b). In (b), the bin with an RH range of 55%–65% and a NO₂ range of 40–50 μg/m³ was found to have the largest number of samples (N_max), then for each bin, the absolute number of samples was normalized by N_max to determine the relative number of samples.

Fig.3 Temperature-dependent variations of (a) SOR, (b) NOR, (c) SO₂, (d) NO₂, (e) the sulfate to (PM_2.5)* ratio, (f) the nitrate to (PM_2.5)* ratio, (g) the nitrate to sulfate ratio and (h) the NO₂ to SO₂ ratio. Samples showing enhanced SOR at high RH (N = 8) are not involved. Lower and upper box bounds indicate the 25^th and 75^th percentiles, the whiskers below and above the box indicate the 5^th and 95^th percentiles, and the diamond within the box marks the median (the same hereinafter).

Fig.4 Comparison of (a) SOR, (b) NOR, (c) levoglucosan, (d) K⁺, (e) the nitrate to sulfate ratio and (f) the NO₂ to SO₂ ratio across different (PM_2.5)* ranges. Samples showing enhanced SOR at high RH (N = 8) are not involved. The solid circles above and below the box indicate the maximum and minimum, respectively.

Fig.5 Dependences of (a) SOR, (b) NOR, (c) the nitrate to sulfate ratio and (d) the NO₂ to SO₂ ratio on levoglucosan. Samples showing enhanced SOR at high RH (N = 8) are not involved. Results from different daily average temperature ranges (i.e., below or above 0°C) are shown separately.

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