Atmospheric Chemistry and Physics (Nov 2019)

Gaseous, PM<sub>2.5</sub> mass, and speciated emission factors from laboratory chamber peat combustion

  • J. G. Watson,
  • J. G. Watson,
  • J. Cao,
  • J. Cao,
  • L.-W. A. Chen,
  • Q. Wang,
  • J. Tian,
  • J. Tian,
  • X. Wang,
  • S. Gronstal,
  • S. S. H. Ho,
  • A. C. Watts,
  • J. C. Chow,
  • J. C. Chow

DOI
https://doi.org/10.5194/acp-19-14173-2019
Journal volume & issue
Vol. 19
pp. 14173 – 14193

Abstract

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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.