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Relative Importance of Gas Uptake on Aerosol and Ground Surfaces Characterized by Equivalent Uptake Coefficients

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Relative Importance of Gas Uptake on Aerosol and Ground Surfaces Characterized by Equivalent Uptake Coefficients Atmos. Chem. Phys., 19, 10981–11011, 2019 https://doi.org/10.5194/acp-19-10981-2019 © Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License. Relative importance of gas uptake on aerosol and ground surfaces characterized by equivalent uptake coefficients Meng Li1,a, Hang Su1, Guo Li1, Nan Ma2, Ulrich Pöschl1, and Yafang Cheng1 1Max Planck Institute for Chemistry, Mainz, 55118, Germany 2Center for Air Pollution and Climate Change Research (APCC), Institute for Environmental and Climate Research (ECI), Jinan University, Guangzhou, 511443, China anow at: Chemical Science Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration (NOAA), Boulder, Colorado 80305, USA Correspondence: Hang Su ([email protected]) and Yafang Cheng ([email protected]) Received: 19 March 2019 – Discussion started: 2 April 2019 Revised: 9 July 2019 – Accepted: 19 July 2019 – Published: 29 August 2019 Abstract. Quantifying the relative importance of gas up- Given the fact that most models have considered the up- take on the ground and aerosol surfaces helps to determine takes of these species on the ground surface, we suggest also which processes should be included in atmospheric chem- considering the following processes in atmospheric models: istry models. Gas uptake by aerosols is often characterized N2O5 uptake by all types of aerosols, HNO3 and SO2 uptake by an effective uptake coefficient (γeff), whereas gas uptake by mineral dust and sea salt aerosols, H2O2 uptake by min- on the ground is usually described by a deposition velocity eral dust, NO2 uptakes by sea salt aerosols and O3 uptake by (Vd). For efficient comparison, we introduce an equivalent liquid organic aerosols. uptake coefficient (γeqv) at which the uptake flux of aerosols would equal that on the ground surface. If γeff is similar to or larger than γeqv, aerosol uptake is important and should be included in atmospheric models. In this study, we com- 1 Introduction pare uptake fluxes in the planetary boundary layer (PBL) for different reactive trace gases (O3, NO2, SO2,N2O5, HNO3 Multiphase processes play an essential role in atmospheric and H2O2), aerosol types (mineral dust, soot, organic aerosol chemistry and atmosphere–biosphere exchange (Ravis- and sea salt aerosol), environments (urban areas, agricultural hankara, 1997; Ammann et al., 1998, 2013; Gard et al., 1998; land, the Amazon forest and water bodies), seasons and mix- Usher et al., 2003; Bauer et al., 2004; Fowler et al., 2009; ing heights. Kolb et al., 2010; Su et al., 2011, 2013; Herrmann, 2003; For all investigated gases, γeqv ranges from magnitudes Herrmann et al., 2015; Pöhlker et al., 2012; Oswald et al., of 10−6–10−4 in polluted urban environments to 10−4–10−1 2013; Andreae et al., 2015; George et al., 2015; McNeill, under pristine forest conditions. In urban areas, aerosol up- 2015; Pöschl and Shiraiwa, 2015; Quinn et al., 2015; We- take is relevant for all species (γeff ≥ γeqv) and should be con- ber et al., 2015; Cheng et al., 2016; Fröhlich-Nowoisky et sidered in models. On the contrary, contributions of aerosol al., 2016; Lappalainen et al., 2016; Tang et al., 2016; Meusel uptakes in the Amazon forest are minor compared with the et al., 2018). They not only affect the atmospheric trace gas dry deposition. The phase state of aerosols could be one of concentrations but also modify the properties of condensed the crucial factors influencing the uptake rates. Current mod- phases, commonly known as the aging process (Song and els tend to underestimate the O3 uptake on liquid organic Carmichael, 1999; Cheng et al., 2006, 2012; Rudich et al., aerosols which can be important, especially over regions with 2007; Andreae 2009; Jimenez et al., 2009; Gunthe et al., γeff ≥ γeqv.H2O2 uptakes on a variety of aerosols are yet to 2011; Ditas et al., 2018). In the planetary boundary layer be measured under laboratory conditions and evaluated. (PBL), aerosols and the ground provide two kinds of sur- faces for multiphase reactions. In previous gas uptake stud- Published by Copernicus Publications on behalf of the European Geosciences Union. 10982 M. Li et al.: Relative importance of gas uptake on aerosol and ground surfaces ies, different formulations have been used to describe and and photochemical data for the multiphase reactions were parameterize the gas uptake processes (Wesely, 1989, 2007; conducted afterwards (Crowley et al., 2010, 2013; Ammann Ravishankara, 1997; Jacob, 2000; Wesely and Hicks, 2000; et al., 2013; Burkholder et al., 2015). Pöschl et al. (2007), and Zhang et al., 2003; Ammann and Pöschl, 2007; Pöschl et al., the follow-up studies (e.g., Shiraiwa et al., 2010, 2011) de- 2007). veloped a comprehensive kinetic model framework, enabling A variety of ground surfaces, including vegetation, water, consistent and unambiguous descriptions of mass transfer rock, roads and so on, can take up gaseous species via dry and chemical reactions in aerosol systems. deposition, and, thus, have significant impacts on the bud- However, the question still remains as to which surface get of these reactive gases and on the physicochemical prop- types are more important for gas uptake in the PBL. The an- erties of the ground surface itself (Lelieveld and Dentener, swer is not straightforward due to the following reasons: 2000; Ashmore, 2005). Dry deposition is one of the major removal pathways for most gaseous species and has been ex- 1. First, although the surface of the Earth seems to be tensively parameterized in atmospheric models (Wesely and much larger than that of tiny aerosols, its contribution Hicks, 2000; Zhang et al., 2002, 2003). A resistance model, is diluted by the large volume of the PBL, resulting in which consists of the aerodynamic resistance, quasi-laminar a surface to volume ratio close to that of aerosol; for resistance and surface resistance, has been widely applied to example, for a PBL height of 1000 m, the correspond- 2 −3 calculate the dry deposition flux in global and regional atmo- ing surface to volume ratio is 1000 µm cm , which is comparable to aerosol surface area concentrations of spheric models (see Fig. 1, Wesely and Hicks, 2000; Wesely, − −1 200–2000 µm2 cm 3 for urban areas (Woo et al., 2001; 2007). The dry deposition velocity, Vd (in units of cm s ) calculated as the reciprocal of the total resistance, is the key Stanier et al., 2004; Wu et al., 2008, 2017; Ma and Bir- 2 −3 parameter to describe the uptake fluxes on the ground. mili, 2015) and 200–1000 µm cm for rural environ- Since the late 1990s, the importance of reactive uptake ments (Ma et al., 2014; Ma and Birmili, 2015; Wu et al., of gases by aerosols has been commonly accepted (Ravis- 2017; Held et al., 2008). hankara, 1997; Gard et al., 1998; Jacob, 2000). Gas uptake 2. Second, different formulations also hinder the compar- by aerosols not only influences the fate of reactive gases, but ison. As illustrated above, different schemes, formula- also changes the physiochemical properties of atmospheric tions and terminologies are applied to calculate the up- aerosols (Kolb et al., 2010). Taking the multiphase chem- take fluxes on ground and aerosols. The dry deposition istry into account has proven to be a key factor to explain the velocity (V ) is the fundamental parameter to describe observations and improve the model performances (Zhang d the deposition process on the ground, whereas the ef- and Carmichael, 1999; Song and Carmichael, 2001; Liao fective uptake coefficient (γ ) is used to describe the and Seinfeld, 2005; Wang et al., 2006; McNaughton et al., eff uptake fluxes on aerosols. 2009; X. Wang, et al., 2012; B. Zheng et al., 2015; Tang et al., 2017; Chen et al., 2018; Mu et al., 2018). Compared In this study, we conducted a comparative assessment of with dry deposition, the parameterization of gas uptake on the gas uptake on both ground and aerosol surfaces. Our goal aerosols is more challenging (Jacob, 2000; Pöschl and Shi- is to identify the prevailing multiphase process in the PBL, raiwa, 2015). The mass transfer between gases and aerosols especially those processes that have not yet been sufficiently can be described by the resistance model in analogy with an considered in atmospheric models. Section 2 describes the electrical circuit that decoupled the physiochemical limita- methods of calculation and comparison. We present and dis- tions in the gas phase, gas–surface interface and the bulk cuss the main results in Sect. 3, which is followed by a sum- phase under (quasi-) steady-state conditions (Schwartz and mary of our major findings in Sect. 4. Freiberg, 1981; Schwartz, 1986; Kolb et al., 1995). A sim- plified scheme, which relies on the formulation of an effec- tive uptake coefficient (γeff) has been widely used in cur- 2 Methods rent atmospheric models (Jacob, 2000; Liao and Seinfeld, 2005; K. Wang et al., 2012). Growing numbers of labora- In this work, we compared the relative importance of gas up- tory studies have reported γeff for various trace gases and take by the ground and by aerosols based on their uptake aerosol particles that are potentially important for atmo- fluxes. In this comparison, resistance models were applied spheric chemistry, such as O3, NO2, SO2,N2O5, HNO3 on to calculate uptake fluxes on both ground and aerosol sur- mineral dust (Ullerstam et al., 2002; Mogili et al., 2006; faces (see Fig. 1) as detailed below. The uptake fluxes of Vlasenko et al., 2006; Wagner et al., 2008; Ndour et al., six reactive gases (O3, NO2, SO2,N2O5, HNO3 and H2O2) 2009), soot (Rogaski et al., 1997; Longfellow et al., 2000; were calculated and compared for four typical land use cate- Al-Abadleh and Grassian, 2000; Saathoff et al., 2001) and gories (urban areas, agricultural land, the Amazon forest and sea salt aerosols (Mochida et al., 2000; Gebel and Finlayson- water) and five aerosol types (mineral dust, soot, solid or- Pitts, 2000; Hoffman et al., 2003; Thornton and Abbatt, ganic aerosol, liquid organic aerosol and sea salt aerosol).
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