New insights into the formation of ammonium nitrate from a physical and chemical level perspective

doi:10.1007/s11783-023-1737-6

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (11) : 137 https://doi.org/10.1007/s11783-023-1737-6

RESEARCH ARTICLE

New insights into the formation of ammonium nitrate from a physical and chemical level perspective

Yuting Wei^1,², Xiao Tian^1,², Junbo Huang^1,², Zaihua Wang³(

), Bo Huang⁴, Jinxing Liu^5,⁶, Jie Gao^1,², Danni Liang^1,², Haofei Yu⁷, Yinchang Feng^1,², Guoliang Shi^1,²(

)

¹. State Environmental Protection Key Laboratory of Urban Ambient Air Particulate Matter Pollution Prevention and Control, Tianjin Key Laboratory of Urban Transport Emission Research, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China
². CMA-NKU Cooperative Laboratory for Atmospheric Environment-Health Research (CLAER), College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China
³. Institute of Resources Utilization and Rare Earth Development, Guangdong Academy of Sciences, Guangzhou 510650, China
⁴. Guangzhou Hexin Instrument Co. Ltd., Guangzhou 510530, China
⁵. State Key Laboratory of Precision Measuring Technology and Instruments, Tianjin Key Laboratory of Air pollutants Monitoring Technology, School of Precision Instrument and Opto-electronics Engineering, Tianjin University, Tianjin 300072, China
⁶. Gigantic Technology (Tianjin) Co. Ltd., Tianjin 300384, China
⁷. Department of Civil, Environmental and Construction Engineering, University of Central Florida, Orlando, FL32816, USA

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Abstract

● Factor analysis of ammonium nitrate formation based on thermodynamic theory.

● Aerosol liquid water content has important role on the ammonium nitrate formation.

● Contribution of coal combustion and vehicle exhaust is significant in haze periods.

High levels of fine particulate matter (PM_2.5) is linked to poor air quality and premature deaths, so haze pollution deserves the attention of the world. As abundant inorganic components in PM_2.5, ammonium nitrate (NH₄NO₃) formation includes two processes, the diffusion process (molecule of ammonia and nitric acid move from gas phase to liquid phase) and the ionization process (subsequent dissociation to form ions). In this study, we discuss the impact of meteorological factors, emission sources, and gaseous precursors on NH₄NO₃ formation based on thermodynamic theory, and identify the dominant factors during clean periods and haze periods. Results show that aerosol liquid water content has a more significant effect on ammonium nitrate formation regardless of the severity of pollution. The dust source is dominant emission source in clean periods; while a combination of coal combustion and vehicle exhaust sources is more important in haze periods. And the control of ammonia emission is more effective in reducing the formation of ammonium nitrate. The findings of this work inform the design of effective strategies to control particulate matter pollution.

Keywords Ammonium nitrate formation Thermodynamic theory Aerosol liquid water content Source apportionment

Corresponding Author(s): Zaihua Wang,Guoliang Shi

Issue Date: 15 November 2023

Cite this article:

Yuting Wei,Xiao Tian,Junbo Huang, et al. New insights into the formation of ammonium nitrate from a physical and chemical level perspective[J]. Front. Environ. Sci. Eng., 2023, 17(11): 137.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1737-6
https://academic.hep.com.cn/fese/EN/Y2023/V17/I11/137

Fig.1 Concentrations of SO₄^2–, NO₃^–, NH₄⁺ (a) and their proportion in PM_2.5 (b) under different pollution levels. (c) Correlations between equivalent concentrations of SO₄^2– and NH₄⁺. (d) Correlations between equivalent concentrations of NO₃^– + 2SO₄^2– and NH₄⁺.

Fig.2 S-curve constructed by fitting ε(NO₃^–) and ε(NH₄⁺) as a function of pH using the Boltzmann equation (R² = 0.65 and R² = 0.97, respectively). (a) Orange points are actual atmospheric samples with higher sulfate contributions (> 7 μg/m³) and orange curve is fitted by the Boltzmann equation. (b) Purple points are actual atmospheric samples with ε*(NO₃^–) > 0.8 in summer and purple curve is also fitted by the Boltzmann equation.

Fig.3 (a, c) The relationship between I_TL(NO₃^–) and [H⁺] in ε(NO₃^–). The red dotted line indicates that [H⁺] and I_TL(NO₃^–) are equal, so their effects on the distribution of nitrate are similar at the same time. In the upper left of the dotted line, the influence of I_TL(NO₃^–) is more significant because the order of magnitude of I_TL(NO₃^–) is larger than [H⁺]. On the contrary, in the lower right of the dotted line, the influence of [H⁺] is more significant. (b, d) The relationship between I_TL(NH₄⁺) and 1/[H⁺] in ε(NH₄⁺). Similar to (a, c), the red dotted line indicates that 1/[H⁺] and I_TL(NH₄⁺) are equal, so their effects on the distribution of ammonia are similar. Color represents concentrations of PM_2.5 during (a, b) clean periods and (c, d) haze periods. Data points within circles are samples with relatively high PM_2.5 concentrations (higher than 50 μg/m³ in clean periods and 170 μg/m³ in haze periods).

Fig.4 The relationship between I_TL(NO₃^–) and [H⁺] in ε(NO₃^–). Color represents temperature (a for clean periods, c for haze periods) and liquid water content (b for clean periods, d for haze periods). The meaning of red dotted line is similar to Fig.3.

Fig.5 The relationship between I_TL(NO₃^–) and [H⁺] in ε(NO₃^–). Color represent contributions of dust (a, e), coal combustion (b, f), vehicle (c, g), and biomass burning & SOC (d, h) during clean periods (a through d), and haze periods (e through h). The meaning of red dotted line is similar to Fig. 3.

Fig.6 ε(NO₃^–) and ε(NH₄⁺) in haze days. The scattered points are samples in the actual environment. The red solid line is the fitted equation of the S-curve and the reverse S-curve. The orange shaded portion indicates that ammonium nitrate is insensitive to the emission of precursors (HNO₃ and NH₃), while the blue shaded portion indicates the contrary.

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