Trends of inorganic sulfur and nitrogen species at an urban site in western Canada (2004–2018)

A 15-year (2004–2018) record of measurement data of gaseous and particulate sulfur and nitrogen pollutants in air collected at an urban site in Burnaby in western Canada was analyzed for generating their decadal trends using three different methods, including linear regression, Mann-Kendall test and Theil-Sen trend estimator (MK-TS), and ensemble empirical mode decomposition (EEMD). Annual mean concentration of SO2 and SO42− decreased by about 59% and 42%, respectively, during the 15-year period. The slower decreases of SO42− than SO2 were mainly caused by the increased O3 concentration and temperature in spring and summer, which promoted conversion of SO2 to SO42− through gas-phase reaction, and by the increased aerosol pH value and availability of H2O2 in winter, which enhanced aqueous-phase SO42− formation. Accordingly, the sulfur oxidation ratio (SOR) increased by 23% or more in spring, summer, and winter during the 15-year period. Annual mean concentrations of NO2 and NO3− declined by 36% and 38%, respectively, during this period. On seasonal basis, NO3− decreased faster than NO2 in autumn and slower in winter. The non-linear responses of NO3− to NO2 concentration decreases were more evident in winter than the other seasons, partly due to the increased particulate NO3− fraction caused by decreased temperature, increased aerosol pH value, and enhanced NO3− formation caused by increased O3 concentrations. Annual mean concentration of NH3 showed small increases due to stable NH3 emission and reduced conversion of NH3 to NH4+. NH4+ concentration decreased by 51% during the 15-year period. These results suggest that reduced oxidants levels are likely responsible for weakened formation of secondary inorganic aerosols, besides emission reductions for SO2 and NO2.