Measurement report: Variations in surface SO₂ and NO_x mixing ratios from 2004 to 2016 at a background site in the North China Plain

Strict air pollution control strategies have been implemented in recent decades in the North China Plain (NCP), previously one of the most polluted regions in the world, and have resulted in considerable changes in emissions of air pollutants. However, little is so far known about the long-term trends of the regional background level of NOx and SO2, along with the increase and decrease processes of regional emissions. In this study, the seasonal and diurnal variations of NOx and SO2 as well as their long-term trends at a regional background station in the NCP were characterized from 2004 to 2016. On average, SO2 and NOx mixing ratios were 5.7 ± 8.4 ppb and 14.2 ± 12.4 ppb, respectively. The seasonal variations in SO2 and NOx mixing ratios showed a similar pattern with a peak in winter and a valley in summer. However, the diurnal variations in SO2 and NOx mixing ratios greatly differed for all seasons, indicating different sources for SO2 and NOx. Overall, the annual mean SO2 exhibited a significant decreasing trend of ‒6.1 % yr−1 (R = −0.84, P < 0.01) from 2004 to 2016, which is very close to −6.3 % yr−1 of the annual SO2 emission in Beijing, and a greater decreasing trend of −7.4 % yr−1 (R = −0.95, P < 0.01) from 2008 to 2016. The annual mean of NOx showed a fluctuating rise of +3.4 % yr−1 (R = 0.38, P = 0.40) from 2005 to 2010, reaching the peak value (16.9 ppb) in 2010, and then exhibited an extremely significant fluctuating downward trend of −4.5 % yr−1 (R = 0.95, P < 0.01) from 2010 to 2016. After 2010, the annual mean NOx mixing ratios correlated significantly (R = 0.94, P < 0.01) with the annual NOx emission in North China. The decreasing rate (−4.8 % yr−1, R = −0.92, P < 0.01) of the annual mean NOx mixing ratios from 2011 to 2016 at SDZ are lower than the one (−8.8 % yr−1, R = −0.94, P < 0.01) for the annual NOx emission in the NCP and (−9.0 % yr−1, R = −0.96, P < 0.01) in Beijing. It indicated that surface NOx mixing ratios at SDZ had weaker influence than SO2 by the emission reduction in Beijing and its surrounding areas in the NCP. The increase in the amount of motor vehicles led to an increase in traffic emissions for NOx. This study supported conclusions from previous studies that the measures taken for controlling NOx and SO2 in the NCP in the past decades were generally successful. However, NOx emission control should be strengthened in the future.