Atmospheric Chemistry and Physics (Nov 2019)
Gaseous, PM<sub>2.5</sub> mass, and speciated emission factors from laboratory chamber peat combustion
Abstract
Peat fuels representing four biomes of boreal (western Russia and Siberia), temperate (northern Alaska, USA), subtropical (northern and southern Florida, USA), and tropical (Borneo, Malaysia) regions were burned in a laboratory chamber to determine gas and particle emission factors (EFs). Tests with 25 % fuel moisture were conducted with predominant smoldering combustion conditions (average modified combustion efficiency (MCE) =0.82±0.08). Average fuel-based EFCO2 (carbon dioxide) are highest (1400 ± 38 g kg−1) and lowest (1073 ± 63 g kg−1) for the Alaskan and Russian peats, respectively. EFCO (carbon monoxide) and EFCH4 (methane) are ∼12 %–15 % and ∼0.3 %–0.9 % of EFCO2, in the range of 157–171 and 3–10 g kg−1, respectively. EFs for nitrogen species are at the same magnitude as EFCH4, with an average of 5.6 ± 4.8 and 4.7 ± 3.1 g kg−1 for EFNH3 (ammonia) and EFHCN (hydrogen cyanide); 1.9±1.1 g kg−1 for EFNOx (nitrogen oxides); and 2.4±1.4 and 2.0 ± 0.7 g kg−1 for EFNOy (total reactive nitrogen) and EFN2O (nitrous oxide). An oxidation flow reactor (OFR) was used to simulate atmospheric aging times of ∼2 and ∼7 d to compare fresh (upstream) and aged (downstream) emissions. Filter-based EFPM2.5 varied by > 4-fold (14–61 g kg−1) without appreciable changes between fresh and aged emissions. The majority of EFPM2.5 consists of EFOC (organic carbon), with EFOC ∕ EFPM2.5 ratios in the range of 52 %–98 % for fresh emissions and ∼14 %–23 % degradation after aging. Reductions of EFOC (∼7–9 g kg−1) after aging are most apparent for boreal peats, with the largest degradation in low-temperature OC1 that evolves at < 140 ∘C, indicating the loss of high-vapor-pressure semivolatile organic compounds upon aging. The highest EFLevoglucosan is found for Russian peat (∼16 g kg−1), with ∼35 %–50 % degradation after aging. EFs for water-soluble OC (EFWSOC) account for ∼20 %–62 % of fresh EFOC. The majority (> 95 %) of the total emitted carbon is in the gas phase, with 54 %–75 % CO2, followed by 8 %–30 % CO. Nitrogen in the measured species explains 24 %–52 % of the consumed fuel nitrogen, with an average of 35 ± 11 %, consistent with past studies that report ∼1/3 to 2∕3 of the fuel nitrogen measured in biomass smoke. The majority (> 99 %) of the total emitted nitrogen is in the gas phase, with an average of 16.7 % as NH3 and 9.5 % as HCN. N2O and NOy constituted 5.7 % and 2.9 % of consumed fuel nitrogen. EFs from this study can be used to refine current emission inventories.