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Emissions of Trace Organic Gases from Western US Wildfires Based on WE manuscript submitted to JGR Atmospheres 1 Emissions of trace organic gases from western U.S. wildfires based on WE--CAN 2 aircraft measurements 3 4 Wade Permar1, Qian Wang1, 7, Vanessa Selimovic1, Catherine Wielgasz1, Robert J. 5 Yokelson1, Rebecca S. Hornbrook2, Alan J. Hills2, Eric C. Apel2, I-Ting Ku3 , Yong Zhou3, 6 Barkley C. Sive4, Amy P. Sullivan3, Jeffrey L. Collett Jr3, Teresa L. Campos2, Brett B. 7 Palm5, Qiaoyun Peng5, Joel A. Thornton5, Lauren A. Garofalo6, Delphine K. Farmer6, 8 Sonia M. Kreidenweis6, Ezra J. T. Levin3, 8, Paul J. DeMott3, Frank Flocke2, Emily V. 9 Fischer3, Lu Hu1 10 1Department of Chemistry and Biochemistry, University of Montana, Missoula, MT, USA. 11 2Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric 12 Research, Boulder, CO, USA. 13 3Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA. 14 4Air Resources Division, National Park Service, Denver, CO, USA. 15 5Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA. 16 6Department of Chemistry, Colorado State University, Fort Collins, CO, USA. 17 7Now at Guizhou Provincial Key Laboratory of Geographic State Monitoring of Watershed, 18 Guizhou Education University, Guiyang 550018, China. 19 8Now at Handix Scientific, Boulder, CO, USA. 20 21 Correspondence author: Lu Hu ([email protected]) 22 23 Key Points: 24 • Volatile organic compound emission factors and emission ratios for western U.S. 25 wildfires are reported. 26 • 76% of the total measured volatile organic compound emitted mass has statistically 27 significant dependence on modified combustion efficiency. 28 • Mass fraction contributions of individual species to the total measured emissions have 29 little fire-to-fire variability. 30 31 32 manuscript submitted to JGR Atmospheres 33 Abstract 34 We present emissions measurements of volatile organic compounds (VOCs) for western U.S. 35 wildland fires made on the NSF/NCAR C-130 research aircraft during the Western Wildfire 36 Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) field campaign 37 in summer 2018. VOCs were measured with complementary instruments onboard the C-130, 38 including a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) and two 39 gas chromatography (GC)-based methods. Agreement within combined instrument uncertainties 40 (< 60 %) was observed for most co-measured VOCs. GC-based measurements speciated the 41 isomeric contributions to selected PTR-ToF-MS ion masses and generally showed little fire-to- 42 fire variation. We report emission ratios (ERs) and emission factors (EFs) for 161 VOCs 43 measured in 31 near-fire smoke plume transects of 24 specific individual fires sampled in the 44 afternoon when burning conditions are typically most active. Modified combustion efficiency 45 (MCE) ranged from 0.85–0.94. The measured campaign-average total VOC EF was 26.1 ± 6.9 g 46 kg-1, approximately 67% of which is accounted for by oxygenated VOCs. The 10 most 47 abundantly emitted species contributed more than half of the total measured VOC mass. We 48 found that MCE alone explained nearly 70 % of the observed variance for total measured VOC 49 emissions (r2 = 0.67) and > 50 % for 57 individual VOC EFs representing more than half the 50 organic carbon mass. Finally, we found little fire-to-fire variability for the mass fraction 51 contributions of individual species to the total measured VOC emissions, suggesting that a single 52 speciation profile can describe VOC emissions for the wildfires in coniferous ecosystems 53 sampled during WE-CAN. 54 55 1 Introduction 56 Wildland fires are a significant source of non-methane volatile organic compounds (VOCs) to 57 the atmosphere (Akagi et al., 2011; Crutzen & Andreae, 1991; Hatch et al., 2017; Koss et al., 58 2018; Liu et al., 2017), impacting downwind air quality, public health, and the formation of 59 secondary pollutants such as ozone (O3), and secondary organic aerosol (SOA). However, their 60 global and regional emissions are highly uncertain, in part reflecting the scarcity of field 61 measurements to constrain VOC emissions from biomass burning. As the size and intensity of 62 wildfires have increased due to historic forest management practices and climate change 63 (Bowman et al., 2017; Jolly, 2015; Westerling, 2006, 2016), air quality in the western United 64 States (U.S.) is degrading relative to the rest of the country (McClure & Jaffe, 2018; O’Dell et 65 al., 2019). These issues motivated comprehensive smoke characterization measurements from 66 the National Science Foundation / National Center for Atmospheric Research (NSF/NCAR) C- 67 130 research aircraft for western U.S. wildfires during the 2018 Western Wildfire Experiment for 68 Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) field campaign. manuscript submitted to JGR Atmospheres 69 Biomass burning emission factors (EFs, g compound emitted per kg biomass burned) are a 70 critical input to air quality models which rely mainly on “bottom-up” emissions inventories 71 derived from regional or vegetation specific EFs, burned area, and fuel consumption per unit area 72 (Larkin et al., 2014; Urbanski, 2014; van der Werf et al., 2017; Wiedinmyer et al., 2011). Total 73 emissions are subject to large uncertainties given the difficulty of estimating burned area and fuel 74 consumption along with large fire-to-fire VOC emissions variability and a general under- 75 sampling of many wildfire-prone regions, including the western U.S. The large natural fire-to- 76 fire variability of some commonly measured VOC emissions can be partially explained by a 77 simple proxy of “flaming” and “smoldering” combustion processes, known as the modified 78 combustion efficiency (MCE), which is readily calculated from observations of carbon monoxide 79 (CO) and carbon dioxide (CO2) (Akagi et al., 2013; Andreae & Merlet, 2001; Ferek et al., 1998; 80 Guérette et al., 2018; Liu et al., 2017; Urbanski, 2014; Yokelson et al., 1999). 81 82 To better constrain VOC and other air pollutant emissions from western U.S. fires, several recent 83 large laboratory burn experimental studies have been conducted for representative fuels (Gilman 84 et al., 2015; Hatch et al., 2017; Koss et al., 2018; Selimovic et al., 2018; Stockwell et al., 2014, 85 2015; Yokelson et al., 2013). Laboratory experiments attempt to simulate real-world burning 86 conditions using fuels selected to reflect their natural composition, sometimes resulting in good 87 agreement between field and laboratory measured EFs and emission ratios (ERs) of well- 88 characterized species (Akagi et al., 2013; Christian et al., 2003; Selimovic et al., 2018; Yokelson 89 et al., 2008, 2013). However, laboratory burning experiments are imperfect proxies for the 90 complexity of the dynamic burning processes, meteorological conditions, and varying fuels 91 present in wildland fires. Meanwhile, field emission measurements, either using ground- or 92 airborne-based platforms, are typically limited by how near a wildfire they can sample due to 93 safety and logistical constraints. As chemical processes take place in the smoke plume within 94 tens of minutes between emission and sampling by research aircraft (Hobbs et al., 2003; Peng et 95 al., 2020), field emission measurements likely reflect some removal of highly reactive species 96 along with formation of secondary products. Airborne measurements may also miss emissions 97 from residual smoldering combustion (Bertschi et al., 2003), which tend to not be lofted into the 98 main convective column of the plume, while ground based measurements reflect the opposite 99 problem as they are often unable to sample portions of the smoke most impacted by flaming manuscript submitted to JGR Atmospheres 100 emissions (Akagi et al., 2013; Ottmar, 2014; Prichard et al., 2020; Yokelson et al., 2013). 101 Additionally, laboratory studies can allow for a large suite of analytical instrumentation to 102 sample smoke within meters of a fire, from ignition to extinction. Field measurements are often 103 limited by instrument payload and these samples include emissions from a variety of burning 104 conditions. Consequently, to most accurately characterize wildfire emissions, insights gained 105 from laboratory studies are useful in the interpretation of field measurements (Selimovic et al., 106 2019). 107 108 Hundreds, if not thousands, of VOCs are known to be present in biomass burning smoke (Bruns 109 et al., 2017; Hatch et al., 2017; Koss et al., 2018; Müller et al., 2016; Stockwell et al., 2015). 110 Characterization of these VOCs remains a challenge though as no single technique is best suited 111 to measure such a large variety of compounds, particularly at the temporal resolution needed for 112 aircraft sampling. Chemical ionization mass spectrometry (CIMS), such as proton-transfer- 113 reaction time-of-flight mass spectrometry (PTR-ToF-MS), is capable of measuring hundreds of 114 VOCs at < 1 s, but lacks speciation information without prior knowledge of the sampling 115 medium. Gas chromatography (GC)-based systems are highly complementary to CIMS 116 instruments, providing speciated VOC measurements with low ppt detection limits at lower 117 temporal resolution. During the recent Fire Influence on Regional to Global Environments 118 Missoula Fire Lab experiment (FIREX-MFL), 119 https://www.esrl.noaa.gov/csl/projects/firex/firelab), Koss et al. (2018) identified the VOC 120 contributors to more than 150 ions detected
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