Abstract
Abstract. Heterogeneous reactions of mineral dust aerosol with trace gases in the atmosphere could directly and indirectly affect tropospheric oxidation capacity, in addition to aerosol composition and physicochemical properties. In this article we provide a comprehensive and critical review of laboratory studies of heterogeneous uptake of OH, NO3, O3, and their directly related species as well (including HO2, H2O2, HCHO, HONO, and N2O5) by mineral dust particles. The atmospheric importance of heterogeneous uptake as sinks for these species is assessed (i) by comparing their lifetimes with respect to heterogeneous reactions with mineral dust to lifetimes with respect to other major loss processes and (ii) by discussing relevant field and modeling studies. We have also outlined major open questions and challenges in laboratory studies of heterogeneous uptake by mineral dust and discussed research strategies to address them in order to better understand the effects of heterogeneous reactions with mineral dust on tropospheric oxidation capacity.
Highlights
1.1 Mineral dust in the atmosphereMineral dust, emitted from arid and semiarid regions with an annual flux of ∼ 2000 Tg per year, is one of the most abundant types of aerosol particles in the troposphere (Zhang et al, 2003b; Textor et al, 2006; Huneeus et al, 2011; Ginoux et al, 2012; Huang et al, 2016)
The following approaches are used to achieve this goal: (1) lifetimes of reactive trace gases with respect to heterogeneous uptake by mineral dust, calculated using preferred uptake coefficients and typical mineral dust mass concentrations, are compared to their lifetimes in the troposphere in order to discuss the significance of heterogeneous reactions as atmospheric sinks for these trace gases; (2) the atmospheric importance of these heterogeneous reactions is further discussed by referring to representative box, regional, and global modeling studies reported previously; (3) we describe two of the largest challenges in the laboratory studies of heterogeneous reactions of mineral dust particles (Sect. 2.2) and explain why reported uptake coefficients show large variability and how we should interpret and use these kinetic data
It has been widely recognized that heterogeneous reactions with mineral dust particles can significantly affect tropospheric oxidation capacity directly and indirectly
Summary
Mineral dust, emitted from arid and semiarid regions with an annual flux of ∼ 2000 Tg per year, is one of the most abundant types of aerosol particles in the troposphere (Zhang et al, 2003b; Textor et al, 2006; Huneeus et al, 2011; Ginoux et al, 2012; Huang et al, 2016). Mineral dust particles can undergo heterogeneous and/or multiphase reactions during their transport (Dentener et al, 1996; Usher et al, 2003a; Crowley et al, 2010a) These reactions will modify the composition of dust particles (Matsuki et al, 2005; Ro et al, 2005; Sullivan et al, 2007; Shi et al, 2008; Li and Shao, 2009; He et al, 2014) and subsequently change their physicochemical properties, including hygroscopicity, CCN, and ice nucleation activities (Krueger et al, 2003b; Sullivan et al, 2009b; Chernoff and Bertram, 2010; Ma et al, 2012; Tobo et al, 2012; Sihvonen et al, 2014; Wex et al, 2014; Kulkarni et al, 2015), as well as the solubility of Fe and P, etc. Some minerals, such as CaCO3 and TiO2, are widely used as raw materials in construction, and their heterogeneous interactions with reactive trace gases can be important for local outdoor and indoor air quality (Langridge et al, 2009; Raff et al, 2009; Ammar et al, 2010; Baergen and Donaldson, 2016; George et al, 2016) and deterioration of construction surfaces (Lipfert, 1989; Webb et al, 1992; Striegel et al, 2003; Walker et al, 2012)
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