Simultaneous measurement of particulate and gaseous pollutants in an urban city in North China Plain during the heating period: Implication of source contribution

• Pollutants were measured at an urban site in NCP during the winter heating period.
• Coal combustion and vehicular emissions are the main sources.
• Two haze episodes were affected by coal-fired and vehicular emissions, respectively.
• On non-hazy days, pollutants were mainly from the mixing of two types of emissions.
• Even in the heating period in NCP, vehicular emissions are the dominant source.

A comprehensive measurement program was undertaken in winter 2009 in a large urban city (Ji'nan) in North China Plain (NCP). The average concentrations of NO, NO2, NOx, NOy, SO2, O3, CO, PM2.5 and BC during the program were 63.9 ± 65.1 ppb, 45.2 ± 16.9 ppb, 106.6 ± 77.8 ppb, 120.7 ± 77.4 ppb, 54.3 ± 25.8 ppb, 6.3 ± 6.0 ppb, 2138.3 ± 1512.8 ppb, 171.3 ± 83.9 μg/m3 and 9.8 ± 6.9 μg/m3, respectively. Two severe haze episodes were observed. All species, except O3, had elevated concentrations on the episodes compared with those on non-hazy days due to accumulation of pollutants. Diurnal variations of species concentrations and correlation analysis suggested that emissions from vehicles and coal combustion (from power plants, industry and domestic heating) are the main sources. Air mass on Episode 1 was predominately influenced by coal combustion, while pollution was characterized by the vehicular emissions on Episode 2. In contrast, on non-hazy days, pollutants were mainly from the mixing of local coal-fired and vehicular exhaust emissions. These distinct characteristics were further supported by higher ratios of CO to NOy and SO2 to NOy on Episode 1 (25.46 ppb/ppb and 0.51 ppb/ppb) compared to Episode 2 (15.55 ppb/ppb and 0.36 ppb/ppb) and non-hazy days (18.15 ppb/ppb and 0.45 ppb/ppb). Multiple linear regression analysis was applied to the concentrations of NOy, SO2 and CO in the observation and empirical equations were obtained for the NOy concentration. Based on the equations, the relative contributions from mobile (i.e. vehicular exhaust) and point sources (i.e. coal combustion) to NOy were estimated to be 68.2% and 38.6%, respectively, demonstrating that even in the demanding period of domestic heating in NCP, vehicular emissions in a large urban city contribute more to NOy than coal combustion emissions. This also implies that vehicular emissions, featured with high NOx, become a dominant source of pollution, highlighting the recent finding of long-term increase of NO2 in the NCP region by satellite observation (Richter et al., 2005).