PM_2.5 pollution in a megacity of southwest China: source apportionment and implication

Abstract. Daily PM_2.5 (aerosol particles with an aerodynamic diameter of less than 2.5 μm) samples were collected at an urban site in Chengdu, an inland megacity in southwest China, during four 1-month periods in 2011, with each period in a different season. Samples were subject to chemical analysis for various chemical components ranging from major water-soluble ions, organic carbon (OC), element carbon (EC), trace elements to biomass burning tracers, anhydrosugar levoglucosan (LG), and mannosan (MN). Two models, the ISORROPIA II thermodynamic equilibrium model and the positive matrix factorization (PMF) model, were applied to explore the likely chemical forms of ionic constituents and to apportion sources for PM_2.5. Distinctive seasonal patterns of PM_2.5 and associated main chemical components were identified and could be explained by varying emission sources and meteorological conditions. PM_2.5 showed a typical seasonality of waxing in winter and waning in summer, with an annual mean of 119 μg m⁻³. Mineral soil concentrations increased in spring, whereas biomass burning species elevated in autumn and winter.

Six major source factors were identified to have contributed to PM_2.5 using the PMF model. These were secondary inorganic aerosols, coal combustion, biomass burning, iron and steel manufacturing, Mo-related industries, and soil dust, and they contributed 37 ± 18, 20 ± 12, 11 ± 10, 11 ± 9, 11 ± 9, and 10 ± 12%, respectively, to PM_2.5 masses on annual average, while exhibiting large seasonal variability. On annual average, the unknown emission sources that were not identified by the PMF model contributed 1 ± 11% to the measured PM_2.5 mass. Various chemical tracers were used for validating PMF performance. Antimony (Sb) was suggested to be a suitable tracer of coal combustion in Chengdu. Results of LG and MN helped constrain the biomass burning sources, with wood burning dominating in winter and agricultural waste burning dominating in autumn. Excessive Fe (Ex-Fe), defined as the excessive portion in measured Fe that cannot be sustained by mineral dust, is corroborated to be a straightforward useful tracer of iron and steel manufacturing pollution. In Chengdu, Mo / Ni mass ratios were persistently higher than unity, and considerably distinct from those usually observed in ambient airs. V / Ni ratios averaged only 0.7. Results revealed that heavy oil fuel combustion should not be a vital anthropogenic source, and additional anthropogenic sources for Mo are yet to be identified. Overall, the emission sources identified in Chengdu could be dominated by local sources located in the vicinity of Sichuan, a result different from those found in Beijing and Shanghai, wherein cross-boundary transport is significant in contributing pronounced PM_2.5. These results provided implications for PM_2.5 control strategies.