Modeling of gaseous methylamines in the global atmosphere: Impacts of oxidation and aerosol uptake

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Abstract

Gaseous amines have attracted increasing attention due to their potential role in enhancing particle nucleation and growth and affecting secondary organic aerosol formation. Here we study with a chemistry transport model the global distributions of the most common and abundant amines in the air: monomethylamine (MMA), dimethylamine (DMA), and trimethylamine (TMA). We show that gas phase oxidation and aerosol uptakes are dominant sinks for these methylamines. The oxidation alone (i.e., no aerosol uptake) leads to methylamine lifetimes of 5-10 h in most parts of low and middle latitude regions. The uptake by secondary species with uptake coefficient (γ) of 0.03 (corresponding to the uptake by sulfuric acid particles) reduces the lifetime by ∼30% over oceans and much more over the major continents, resulting in a methylamine lifetime of less than 1-2 h over central Europe, eastern Asia, and eastern US. With the estimated global emission flux, from the literature, our simulations indicate that [DMA] in the model surface layer over major continents is generally in the range of 0.1-2 ppt (parts per trillion) when γ = 0.03 and 0.2-10 ppt when γ = 0, and decreases quickly with altitude. [DMA] over oceans is below 0.05 ppt and over polar regions it is below 0.01 ppt. The simulated [MMA] is about a factor of ∼2.5 higher while [TMA] is a factor of ∼8 higher than [DMA]. The modeled concentrations of methylamines are substantially lower than the limited observed values available, with normalized mean bias ranging from -57 (γ = 0) to -88% (γ = 0.03) for MMA and TMA, and from -78 (γ = 0) to -93% (γ = 0.03) for DMA.

Figures

  • Table 1. Calculated global annual mean emissions, sinks, and burdens of ammonia, MMA, DMA, and TMA. Sinks and burdens under four different uptake coefficients (γ = 0.03, 0.01, 0.001, and 0) are given.
  • Figure 1. Horizontal distributions of annual mean DMA emissions assumed in the present study.
  • Table 2. Available measurements of MMA, DMA, and TMA concentrations (in pptv) and site information.
  • Figure 2. Simulated horizontal distributions of annual mean DMA oxidation and uptake lifetime and concentration ([DMA]) in the model surface layer (0–150 m above surface) under two aerosol uptake coefficients: (a, b) γ = 0 (i.e., oxidation only) and (c, d) γ = 0.03 (uptake by sulfuric acid particles).
  • Figure 3. Same as Fig. 2 but for zonally averaged values. Vertical axis is the ratio of pressure (P ) at the model layer to the pressure at the surface (Psurf).
  • Figure 4. Horizontal distributions of [MMA] in the surface layer (a, c) and its zonally averaged values (b, d) under two different uptake coefficients (γ = 0.03, and 0).
  • Figure 5. Same as Fig. 4 except for [TMA].
  • Figure 6. A comparison of simulated and measured [MMA], [DMA], and [TMA] at the sites listed in Table 2 and marked in Fig. 1 by letters. Model results correspond to the months of the observations, and vertical bars define the simulated ranges of monthly mean values.

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APA

Yu, F., & Luo, G. (2014). Modeling of gaseous methylamines in the global atmosphere: Impacts of oxidation and aerosol uptake. Atmospheric Chemistry and Physics, 14(22), 12455–12464. https://doi.org/10.5194/acp-14-12455-2014

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