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Biomass Combustion Produces Ice-Active Minerals in Biomass-Burning Aerosol and Bottom Ash

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Biomass Combustion Produces Ice-Active Minerals in Biomass-Burning Aerosol and Bottom Ash Biomass combustion produces ice-active minerals in biomass-burning aerosol and bottom ash Leif G. Jahna,1,2, Michael J. Polena,1,3, Lydia G. Jahla, Thomas A. Brubakera, Joshua Somersa, and Ryan C. Sullivana,4 aCenter for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213 Edited by Mark Thiemens, University of California San Diego, La Jolla, CA, and approved July 24, 2020 (received for review December 16, 2019) Ice nucleation and the resulting cloud glaciation are significant Minerals are the most common type of atmospheric INPs and atmospheric processes that affect the evolution of clouds and their are typically ice-active below −15 °C, with wide variation in IN properties including radiative forcing and precipitation, yet the activity (INA) observed for different mineral phases (7). These sources and properties of atmospheric ice nucleants are poorly ice-active minerals are found in atmospheric desert dust, soil, constrained. Heterogeneous ice nucleation caused by ice-nucleating and volcanic ash particles and have important effects on regional particles (INPs) enables cloud glaciation at temperatures above the and global scales (7–10). Biomass burning represents an impor- homogeneous freezing regime that starts near −35 °C. Biomass burn- tant component of the global aerosol burden (11–15) and can be ing is a significant global source of atmospheric particles and a highly a major episodic and regional source of particulate matter (11, variable and poorly understood source of INPs. The nature of these 13, 14, 16, 17). Biomass-burning aerosol (BBA) has been ob- INPs and how they relate to the fuel composition and its combustion served to undergo long-range transport (13, 15, 18) and to affect are critical gaps in our understanding of the effects of biomass burn- cloud properties by acting as cloud condensation nuclei (18–20) ing on the environment and climate. Here we show that the com- and INPs (18, 21, 22) over large regional extents. Changes in bustion process transforms inorganic elements naturally present in land use and climate at global and regional scales are predicted the biomass (not soil or dust) to form potentially ice-active minerals to increase the frequency, intensity, and scale of wildfires and in both the bottom ash and emitted aerosol particles. These particles prescribed burns over the coming years (23–27), making BBA an possess ice-nucleation activities high enough to be relevant to even more important perturbation to Earth’s atmosphere and mixed-phase clouds and are active over a wide temperature range, climate systems in the near future. Regions not historically prone nucleating ice at up to −13 °C. Certain inorganic elements can thus to major wildfires, such as the southeastern United States, have serve as indicators to predict the production of ice nucleants from the recently experienced extensive drought-driven biomass burning fuel. Combustion-derived minerals are an important but under- events (28). The Australian bushfires of 2019 to 2020 represent studied source of INPs in natural biomass-burning aerosol emissions the largest wildfire event in modern history (29), where tall in addition to lofted primary soil and dust particles. These discoveries grasses, shrubs, and other brush species as well as leaf litter and insights should advance the realistic incorporation of biomass- constituted some of the major biomass fuels consumed. Our lack burning INPs into atmospheric cloud and climate models. These min- eral components produced in biomass-burning aerosol should also Significance be studied in relation to other atmospheric chemistry processes, such as facilitating multiphase chemical reactions and nutrient availability. Ice-nucleating particles significantly alter cloud properties and aerosol–cloud–climate interactions | atmospheric chemistry | lifetime, causing large but poorly constrained climate impacts. heterogeneous ice nucleation | climate change | wildfires Biomass-burning aerosol emitted by wildfires is a major and growing source of atmospheric pollution. Prior work suggested that ice-nucleating particles can sometimes be emitted by bio- ce nucleation (IN) and cloud glaciation have extensive effects mass combustion, but the production and characteristics of these Ion cloud microphysics and the evolution, structure, lifetime, – particles are poorly understood. Here we show that mineral precipitation, and radiative properties of clouds (1 3). Ice- phases are a significant ice-active component of both biomass- nucleating particles (INPs) compose a tiny fraction of atmo- burning aerosol and ash particles. These mineral phases are spheric particle numbers. Typically, 1 to 10 per 1 million ambient derived from plant inorganic material that decomposes and re- particles are found to be ice-active at −30 °C under immersion — forms as ice-active minerals during combustion; they form more freezing conditions where the INP is immersed in a super- commonly from tall grass versus wood fuels. Aerosolized min- cooled cloud droplet (4). Despite their scarcity, INPs exert sig- eral and ash are now understood as a major source of the ice- nificant effects on cloud evolution, largely driven by the nucleating particles in biomass-burning smoke. scavenging of water from unfrozen droplets by ice crystals in mixed-phase clouds. Glaciation of supercooled liquid clouds dra- Author contributions: M.J.P. and R.C.S. designed research; L.G. Jahn, M.J.P., L.G. Jahl, and matically reduces their visible optical depth, and thus albedo (2, J.S. performed research; M.J.P., L.G. Jahl, and T.A.B. contributed new reagents/analytic 3), while often initiating precipitation (1–3). Furthermore, climate tools; L.G. Jahn, M.J.P., L.G. Jahl, T.A.B., and R.C.S. analyzed data; and L.G. Jahn, M.J.P., models with different representations of glaciation have system- L.G. Jahl, and R.C.S. wrote the paper. atically different cloud frozen fractions as well as climate sensi- The authors declare no competing interest. tivities (5). Not only is the accurate representation of INPs This article is a PNAS Direct Submission. essential to represent the current climate state, but a proper un- Published under the PNAS license. derstanding of potential changes to INPs due to human activity is 1L.G. Jahn and M.J.P. contributed equally to this work. essential to advance climate change modeling. However, accurate 2Present address: Department of Chemical Engineering, University of Texas at Austin, determination of INP sources, budgets, distributions, and the in- Austin, TX 78712. dividual particle characteristics that affect IN are a significant 3Present address: Department of Chemistry, McDaniel College, Westminster, MD 21157. challenge due to the overall scarcity of INPs. The nanoscale na- 4To whom correspondence may be addressed. Email: [email protected]. ture of heterogeneous IN and the associated ice-active surface This article contains supporting information online at https://www.pnas.org/lookup/suppl/ sites that control this phase transition make this process chal- doi:10.1073/pnas.1922128117/-/DCSupplemental. lenging to directly observe (6). First published August 24, 2020. 21928–21937 | PNAS | September 8, 2020 | vol. 117 | no. 36 www.pnas.org/cgi/doi/10.1073/pnas.1922128117 Downloaded by guest on September 29, 2021 of understanding regarding the sources, properties, and even the directly examined in the emitted aerosol particles. Combustion ash chemical identity of INPs present in biomass smoke plumes has can be a source of INPs, as first observed through the combustion precluded their proper representation in chemical transport and disintegration of a sugar cane leaf skeleton that released INPs and cloud microphysical models (18). inorganic refractory particles (56). Recent studies have examined Biomass burning is a complex process, producing aerosol the INA of wood ash and observed moderate INA, with activity (BBA) and ash particles composed of variable amounts of or- slightly weaker than common INPs such as desert dusts (57, 58). ganic carbon, elemental carbon (soot), and inorganic phases These studies have also suggested inorganic mineral materials, (most commonly potassium salts). Elevated levels of INPs that rather than carbonaceous materials, as the source of ash INA. freeze as warm as −16 °C are inconsistently observed in plumes However, the ash generated in these studies may not be repre- from wildfires and prescribed burns, but the INP sources and sentative of what would form during natural combustion events, as particle types remain undetermined with no clear correlation to ash samples were generated in domestic heating ovens that com- fuel type or combustion conditions (21, 22, 30, 31). Petters et al. bust fuel in a controlled and efficient manner. (21) found that INP concentrations at −30 °C in BBA correlated Here we investigate the ice nucleants produced in biomass- with aerosol potassium fraction, aerosol inorganic fraction, and burning bottom ash and aerosol generated from the open-pan modified combustion efficiency and negatively with organic flaming combustion of grass and wood fuels relevant to the carbon fraction. While soluble inorganic salts are not expected to western and southeastern United States (59, 60). Globally, both be ice-active, each observed positive correlating factor is an in- grassland and forest fires contribute significantly to biomass- dicator of higher-temperature flaming-phase combustion emis- burning emissions (12, 61). Grassland and forest biomes were sions. However, these
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